2024
|
Lai, Wenhui; Lee, Jong Hak; Shi, Lu; Liu, Yuqing; Pu, Yanhui; Ong, Yong Kang; Limpo, Carlos; Xiong, Ting; Rao, Yifan; Sow, Chorng Haur; Ozyilmaz, Barbaros High mechanical strength Si anode synthesis with interlayer bonded expanded graphite structure for lithium-ion batteries JOURNAL OF ENERGY CHEMISTRY, 93 , pp. 253-263, 2024, DOI: 10.1016/j.jechem.2024.02.021. Abstract | BibTeX | Endnote @article{ISI:001203104900001,
title = {High mechanical strength Si anode synthesis with interlayer bonded expanded graphite structure for lithium-ion batteries},
author = {Wenhui Lai and Jong Hak Lee and Lu Shi and Yuqing Liu and Yanhui Pu and Yong Kang Ong and Carlos Limpo and Ting Xiong and Yifan Rao and Chorng Haur Sow and Barbaros Ozyilmaz},
doi = {10.1016/j.jechem.2024.02.021},
times_cited = {0},
issn = {2095-4956},
year = {2024},
date = {2024-06-01},
journal = {JOURNAL OF ENERGY CHEMISTRY},
volume = {93},
pages = {253-263},
publisher = {ELSEVIER},
address = {RADARWEG 29, 1043 NX AMSTERDAM, NETHERLANDS},
abstract = {Despite advancements in silicon -based anodes for high -capacity lithium -ion batteries, their widespread commercial adoption is still hindered by significant volume expansion during cycling, especially at high active mass loadings crucial for practical use. The root of these challenges lies in the mechanical instability of the material, which subsequently leads to the structural failure of the electrode. Here, we present a novel synthesis of a composite combining expanded graphite and silicon nanoparticles. This composite features a unique interlayer-bonded graphite structure, achieved through the application of a modified spark plasma sintering method. Notably, this innovative structure not only facilitates efficient ion and electron transport but also provides exceptional mechanical strength (Vickers hardness: up to 658 MPa, Young's modulus: 11.6 GPa). This strength effectively accommodates silicon expansion, resulting in an impressive areal capacity of 2.9 mA h cm -2 (736 mA h g-1) and a steady cycle life (93% after 100 cycles). Such outstanding performance is paired with features appropriate for large-scale industrial production of silicon batteries, such as active mass loading of at least 3.9 mg cm -2, a high -tap density electrode material of 1.68 g cm -3 (secondary clusters: 1.12 g cm -3), and a production yield of up to 1 kg per day. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.},
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Despite advancements in silicon -based anodes for high -capacity lithium -ion batteries, their widespread commercial adoption is still hindered by significant volume expansion during cycling, especially at high active mass loadings crucial for practical use. The root of these challenges lies in the mechanical instability of the material, which subsequently leads to the structural failure of the electrode. Here, we present a novel synthesis of a composite combining expanded graphite and silicon nanoparticles. This composite features a unique interlayer-bonded graphite structure, achieved through the application of a modified spark plasma sintering method. Notably, this innovative structure not only facilitates efficient ion and electron transport but also provides exceptional mechanical strength (Vickers hardness: up to 658 MPa, Young's modulus: 11.6 GPa). This strength effectively accommodates silicon expansion, resulting in an impressive areal capacity of 2.9 mA h cm -2 (736 mA h g-1) and a steady cycle life (93% after 100 cycles). Such outstanding performance is paired with features appropriate for large-scale industrial production of silicon batteries, such as active mass loading of at least 3.9 mg cm -2, a high -tap density electrode material of 1.68 g cm -3 (secondary clusters: 1.12 g cm -3), and a production yield of up to 1 kg per day. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AULai, WH
Lee, JH
Shi, L
Liu, YQ
Pu, YH
Ong, YK
Limpo, C
Xiong, T
Rao, YF
Sow, CH
Özyilmaz, B
- AFWenhui Lai
Jong Hak Lee
Lu Shi
Yuqing Liu
Yanhui Pu
Yong Kang Ong
Carlos Limpo
Ting Xiong
Yifan Rao
Chorng Haur Sow
Barbaros Ozyilmaz
- TIHigh mechanical strength Si anode synthesis with interlayer bonded expanded graphite structure for lithium-ion batteries
- SOJOURNAL OF ENERGY CHEMISTRY
- LAEnglish
- DTArticle
- DELithium -ion Battery; Silicon Anode; Spark Plasma Sintering; Interlayer Bonding; Mechanical Strength; Tap Density
- IDSILICON ANODES; COMPOSITE; DESIGN
- ABDespite advancements in silicon -based anodes for high -capacity lithium -ion batteries, their widespread commercial adoption is still hindered by significant volume expansion during cycling, especially at high active mass loadings crucial for practical use. The root of these challenges lies in the mechanical instability of the material, which subsequently leads to the structural failure of the electrode. Here, we present a novel synthesis of a composite combining expanded graphite and silicon nanoparticles. This composite features a unique interlayer-bonded graphite structure, achieved through the application of a modified spark plasma sintering method. Notably, this innovative structure not only facilitates efficient ion and electron transport but also provides exceptional mechanical strength (Vickers hardness: up to 658 MPa, Young's modulus: 11.6 GPa). This strength effectively accommodates silicon expansion, resulting in an impressive areal capacity of 2.9 mA h cm -2 (736 mA h g-1) and a steady cycle life (93% after 100 cycles). Such outstanding performance is paired with features appropriate for large-scale industrial production of silicon batteries, such as active mass loading of at least 3.9 mg cm -2, a high -tap density electrode material of 1.68 g cm -3 (secondary clusters: 1.12 g cm -3), and a production yield of up to 1 kg per day. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
- C1[Lai, Wenhui; Shi, Lu; Pu, Yanhui; Limpo, Carlos; Rao, Yifan; Ozyilmaz, Barbaros] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore.
[Lee, Jong Hak; Ong, Yong Kang; Sow, Chorng Haur; Ozyilmaz, Barbaros] Natl Univ Singapore, Ctr Adv Mat 2D, Singapore 117546, Singapore.
[Liu, Yuqing; Xiong, Ting; Sow, Chorng Haur; Ozyilmaz, Barbaros] Natl Univ Singapore, Dept Phys, Singapore 117551, Singapore.
[Ozyilmaz, Barbaros] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore - C3National University of Singapore; National University of Singapore; National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM)
- RPÖzyilmaz, B (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore; Özyilmaz, B (corresponding author), Natl Univ Singapore, Ctr Adv Mat 2D, Singapore 117546, Singapore; Özyilmaz, B (corresponding author), Natl Univ Singapore, Dept Phys, Singapore 117551, Singapore; Özyilmaz, B (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore
- FUNational Research Foundation, Prime Minister's Office, Singapore [NRF-CRP22-2019-008, CA2DM]; Ministry of Education of Singapore [EDUNC-33-18-279-V12]; EDB Singapore [S22-19013-STDP];
- FXThis work was supported by the National Research Foundation, Prime Minister's Office, Singapore, under its Competitive Research Programme (CRP award number NRF-CRP22-2019-008) and Medium-Sized Centre Programme (CA2DM) , by the Ministry of Education of Singapore, under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (I-FIM, Project No. EDUNC-33-18-279-V12) , and by the EDB Singapore, under its Space Technology Development Programme (S22-19013-STDP) .
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Wang, Hao; Sun, Bin; Ge, Shuzhi Sam; Su, Jie; Jin, Ming Liang On non-von Neumann flexible neuromorphic vision sensors NPJ FLEXIBLE ELECTRONICS, 8 (1), 2024, DOI: 10.1038/s41528-024-00313-3. Abstract | BibTeX | Endnote @article{ISI:001215635300003,
title = {On non-von Neumann flexible neuromorphic vision sensors},
author = {Hao Wang and Bin Sun and Shuzhi Sam Ge and Jie Su and Ming Liang Jin},
doi = {10.1038/s41528-024-00313-3},
times_cited = {0},
year = {2024},
date = {2024-05-07},
journal = {NPJ FLEXIBLE ELECTRONICS},
volume = {8},
number = {1},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {The structure and mechanism of the human visual system contain rich treasures, and surprising effects can be achieved by simulating the human visual system. In this article, starting from the human visual system, we compare and discuss the discrepancies between the human visual system and traditional machine vision systems. Given the wide variety and large volume of visual information, the use of non-von Neumann structured, flexible neuromorphic vision sensors can effectively compensate for the limitations of traditional machine vision systems based on the von Neumann architecture. Firstly, this article addresses the emulation of retinal functionality and provides an overview of the principles and circuit implementation methods of non-von Neumann computing architectures. Secondly, in terms of mimicking the retinal surface structure, this article introduces the fabrication approach for flexible sensor arrays. Finally, this article analyzes the challenges currently faced by non-von Neumann flexible neuromorphic vision sensors and offers a perspective on their future development.},
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The structure and mechanism of the human visual system contain rich treasures, and surprising effects can be achieved by simulating the human visual system. In this article, starting from the human visual system, we compare and discuss the discrepancies between the human visual system and traditional machine vision systems. Given the wide variety and large volume of visual information, the use of non-von Neumann structured, flexible neuromorphic vision sensors can effectively compensate for the limitations of traditional machine vision systems based on the von Neumann architecture. Firstly, this article addresses the emulation of retinal functionality and provides an overview of the principles and circuit implementation methods of non-von Neumann computing architectures. Secondly, in terms of mimicking the retinal surface structure, this article introduces the fabrication approach for flexible sensor arrays. Finally, this article analyzes the challenges currently faced by non-von Neumann flexible neuromorphic vision sensors and offers a perspective on their future development. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUWang, H
Sun, B
Ge, SS
Su, J
Jin, ML
- AFHao Wang
Bin Sun
Shuzhi Sam Ge
Jie Su
Ming Liang Jin
- TIOn non-von Neumann flexible neuromorphic vision sensors
- SONPJ FLEXIBLE ELECTRONICS
- LAEnglish
- DTArticle
- IDNEURAL-NETWORK; GANGLION-CELLS; ANALOG; PHOTODETECTOR; ULTRAFAST; MEMORY; PHOTOTRANSISTORS; PLASTICITY; MONOLAYER; FRAMEWORK
- ABThe structure and mechanism of the human visual system contain rich treasures, and surprising effects can be achieved by simulating the human visual system. In this article, starting from the human visual system, we compare and discuss the discrepancies between the human visual system and traditional machine vision systems. Given the wide variety and large volume of visual information, the use of non-von Neumann structured, flexible neuromorphic vision sensors can effectively compensate for the limitations of traditional machine vision systems based on the von Neumann architecture. Firstly, this article addresses the emulation of retinal functionality and provides an overview of the principles and circuit implementation methods of non-von Neumann computing architectures. Secondly, in terms of mimicking the retinal surface structure, this article introduces the fabrication approach for flexible sensor arrays. Finally, this article analyzes the challenges currently faced by non-von Neumann flexible neuromorphic vision sensors and offers a perspective on their future development.
- C1[Wang, Hao; Jin, Ming Liang] Qingdao Univ, Inst Future, Sch Automat, Shandong Key Lab Ind Control Technol, Qingdao 266071, Peoples R China.
[Sun, Bin; Su, Jie] Qingdao Univ, Coll Elect & Informat Engn, Qingdao 266071, Peoples R China.
[Ge, Shuzhi Sam] Natl Univ Singapore, Dept Elect & Comp Engn, Singapore 117583, Singapore.
[Ge, Shuzhi Sam] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117583, Singapore - C3Qingdao University; Qingdao University; National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM)
- RPJin, ML (corresponding author), Qingdao Univ, Inst Future, Sch Automat, Shandong Key Lab Ind Control Technol, Qingdao 266071, Peoples R China; Su, J (corresponding author), Qingdao Univ, Coll Elect & Informat Engn, Qingdao 266071, Peoples R China; Ge, SS (corresponding author), Natl Univ Singapore, Dept Elect & Comp Engn, Singapore 117583, Singapore; Ge, SS (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117583, Singapore
- FUNational Natural Science Foundation of China (National Science Foundation of China) [201909099]; Young Taishan Scholars Program of Shandong Province [EDUNC-33-18-279-V12]; Ministry of Education, Singapore [52003134, 12374088]; National Natural Science Foundation of China
- FXThe work was financially supported by the Young Taishan Scholars Program of Shandong Province (grant nos. 201909099) to M.L. Jin, Ministry of Education, Singapore, under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (I-FIM, project No. EDUNC-33-18-279-V12) to S.S. Ge, and National Natural Science Foundation of China (grant nos. 52003134 and 12374088) to M.L. Jin and J. Su.
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|
Wang, Zhe; Kalathingal, Vijith; Trushin, Maxim; Liu, Jiawei; Wang, Junyong; Guo, Yongxin; Ozyilmaz, Barbaros; Nijhuis, Christian A; Eda, Goki Upconversion electroluminescence in 2D semiconductors integrated with plasmonic tunnel junctions NATURE NANOTECHNOLOGY, 2024, DOI: 10.1038/s41565-024-01650-0. Abstract | BibTeX | Endnote @article{ISI:001205711600001,
title = {Upconversion electroluminescence in 2D semiconductors integrated with plasmonic tunnel junctions},
author = {Zhe Wang and Vijith Kalathingal and Maxim Trushin and Jiawei Liu and Junyong Wang and Yongxin Guo and Barbaros Ozyilmaz and Christian A Nijhuis and Goki Eda},
doi = {10.1038/s41565-024-01650-0},
times_cited = {0},
issn = {1748-3387},
year = {2024},
date = {2024-04-19},
journal = {NATURE NANOTECHNOLOGY},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Plasmonic tunnel junctions are a unique electroluminescent system in which light emission occurs via an interplay between tunnelling electrons and plasmonic fields instead of electron-hole recombination as in conventional light-emitting diodes. It was previously shown that placing luminescent molecules in the tunneling pathway of nanoscopic tunnel junctions results in peculiar upconversion electroluminescence where the energy of emitted photons exceeds that of excitation electrons. Here we report the observation of upconversion electroluminescence in macroscopic van der Waals plasmonic tunnel junctions comprising gold and few-layer graphene electrodes separated by a similar to 2-nm-thick hexagonal boron nitride tunnel barrier and a monolayer semiconductor. We find that the semiconductor ground exciton emission is triggered at excitation electron energies lower than the semiconductor optical gap. Interestingly, this upconversion is reached in devices operating at a low conductance (<10(-6) S) and low power density regime (<10(2) W cm(-2)), defying explanation through existing proposed mechanisms. By examining the scaling relationship between plasmonic and excitonic emission intensities, we elucidate the role of inelastic electron tunnelling dipoles that induce optically forbidden transitions in the few-layer graphene electrode and ultrafast hot carrier transfer across the van der Waals interface.},
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Plasmonic tunnel junctions are a unique electroluminescent system in which light emission occurs via an interplay between tunnelling electrons and plasmonic fields instead of electron-hole recombination as in conventional light-emitting diodes. It was previously shown that placing luminescent molecules in the tunneling pathway of nanoscopic tunnel junctions results in peculiar upconversion electroluminescence where the energy of emitted photons exceeds that of excitation electrons. Here we report the observation of upconversion electroluminescence in macroscopic van der Waals plasmonic tunnel junctions comprising gold and few-layer graphene electrodes separated by a similar to 2-nm-thick hexagonal boron nitride tunnel barrier and a monolayer semiconductor. We find that the semiconductor ground exciton emission is triggered at excitation electron energies lower than the semiconductor optical gap. Interestingly, this upconversion is reached in devices operating at a low conductance (<10(-6) S) and low power density regime (<10(2) W cm(-2)), defying explanation through existing proposed mechanisms. By examining the scaling relationship between plasmonic and excitonic emission intensities, we elucidate the role of inelastic electron tunnelling dipoles that induce optically forbidden transitions in the few-layer graphene electrode and ultrafast hot carrier transfer across the van der Waals interface. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUWang, Z
Kalathingal, V
Trushin, M
Liu, JW
Wang, JY
Guo, YX
Özyilmaz, B
Nijhuis, CA
Eda, G
- AFZhe Wang
Vijith Kalathingal
Maxim Trushin
Jiawei Liu
Junyong Wang
Yongxin Guo
Barbaros Ozyilmaz
Christian A Nijhuis
Goki Eda
- TIUpconversion electroluminescence in 2D semiconductors integrated with plasmonic tunnel junctions
- SONATURE NANOTECHNOLOGY
- LAEnglish
- DTArticle
- IDLIGHT-EMISSION; LUMINESCENT EXCITONS; ENERGY-TRANSFER; ORIENTATION
- ABPlasmonic tunnel junctions are a unique electroluminescent system in which light emission occurs via an interplay between tunnelling electrons and plasmonic fields instead of electron-hole recombination as in conventional light-emitting diodes. It was previously shown that placing luminescent molecules in the tunneling pathway of nanoscopic tunnel junctions results in peculiar upconversion electroluminescence where the energy of emitted photons exceeds that of excitation electrons. Here we report the observation of upconversion electroluminescence in macroscopic van der Waals plasmonic tunnel junctions comprising gold and few-layer graphene electrodes separated by a similar to 2-nm-thick hexagonal boron nitride tunnel barrier and a monolayer semiconductor. We find that the semiconductor ground exciton emission is triggered at excitation electron energies lower than the semiconductor optical gap. Interestingly, this upconversion is reached in devices operating at a low conductance (<10(-6) S) and low power density regime (<10(2) W cm(-2)), defying explanation through existing proposed mechanisms. By examining the scaling relationship between plasmonic and excitonic emission intensities, we elucidate the role of inelastic electron tunnelling dipoles that induce optically forbidden transitions in the few-layer graphene electrode and ultrafast hot carrier transfer across the van der Waals interface.
- C1[Wang, Zhe; Eda, Goki] Natl Univ Singapore, Dept Chem, Singapore, Singapore.
[Wang, Zhe; Kalathingal, Vijith; Guo, Yongxin] Natl Univ Singapore, Dept Elect & Comp Engn, Singapore, Singapore.
[Kalathingal, Vijith] Kannur Univ, Dept Phys, Swami Anandatheertha Campus Payyanur, Kannur, India.
[Trushin, Maxim; Liu, Jiawei; Ozyilmaz, Barbaros] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore.
[Trushin, Maxim; Liu, Jiawei; Ozyilmaz, Barbaros; Eda, Goki] Natl Univ Singapore, Ctr Adv 2D Mat & Graphene Res Ctr, Singapore, Singapore.
[Trushin, Maxim; Ozyilmaz, Barbaros] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore, Singapore.
[Liu, Jiawei; Ozyilmaz, Barbaros; Eda, Goki] Natl Univ Singapore, Dept Phys, Singapore, Singapore.
[Wang, Junyong] Suzhou Inst Nanotech & Nanobion, Chinese Acad Sci, CAS Key Lab Nanobio Interface, i Lab, Suzhou, Peoples R China.
[Wang, Junyong] Chinese Acad Sci, Suzhou Inst Nanotech & Nanobion, Key Lab Nanodevices & Applicat, i Lab, Suzhou, Peoples R China.
[Nijhuis, Christian A.] Univ Twente, Mol Ctr, Fac Sci & Technol, Hybrid Mat Optoelect Grp,Dept Mol & Mat,MESA Inst, Enschede, Netherlands.
[Nijhuis, Christian A.] Univ Twente, Fac Sci & Technol, Ctr Brain Inspired Nano Syst, Enschede, Netherlands - C3National University of Singapore; National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National University of Singapore; National University of Singapore; Chinese Academy of Sciences; Suzhou Institute of Nano-Tech & Nano-Bionics, CAS; Chinese Academy of Sciences; Suzhou Institute of Nano-Tech & Nano-Bionics, CAS; University of Twente; University of Twente
- RPEda, G (corresponding author), Natl Univ Singapore, Dept Chem, Singapore, Singapore; Eda, G (corresponding author), Natl Univ Singapore, Ctr Adv 2D Mat & Graphene Res Ctr, Singapore, Singapore; Eda, G (corresponding author), Natl Univ Singapore, Dept Phys, Singapore, Singapore; Nijhuis, CA (corresponding author), Univ Twente, Mol Ctr, Fac Sci & Technol, Hybrid Mat Optoelect Grp,Dept Mol & Mat,MESA Inst, Enschede, Netherlands; Nijhuis, CA (corresponding author), Univ Twente, Fac Sci & Technol, Ctr Brain Inspired Nano Syst, Enschede, Netherlands
- FUMinistry of Education (MOE), Singapore, under Academic Research Fund (AcRF) Tier 3 [MOE2018-T3-1-005]; National Research Foundation (NRF), under the Prime Minister's Office, Singapore, under the Medium Sized Centre Programme [NRF-CRP17-2017-08]; Competitive Research Programme (CRP) [EDUNC-33-18-279-V12]; Institute for Functional Intelligent Materials (I-FIM) [NRF-NRFI2018-8]; Singapore NRF Investigatorship [MOE-T2EP50220-0017]; MOE-AcRF-Tier 2 [2021YFA1200804]; National Key R&D Program of China
- FXWe acknowledge the support from the Ministry of Education (MOE), Singapore, under Academic Research Fund (AcRF) Tier 3 (grant no. MOE2018-T3-1-005), and the National Research Foundation (NRF), under the Prime Minister's Office, Singapore, under the Medium Sized Centre Programme and the Competitive Research Programme (CRP) (grant no. NRF-CRP17-2017-08). M.T. acknowledges Institute for Functional Intelligent Materials (I-FIM, grant no. EDUNC-33-18-279-V12). B.OE. acknowledges the Singapore NRF Investigatorship (grant no. NRF-NRFI2018-8) and MOE-AcRF-Tier 2 (grant no. MOE-T2EP50220-0017). J.W. acknowledges the National Key R & D Program of China (grant no. 2021YFA1200804).
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|
Pham, Minh Nhat; Su, Chun-Jen; Huang, Yu-Ching; Lin, Kun-Ta; Huang, Ting-Yu; Lai, Yu-Ying; Wang, Chen-An; Liaw, Yong-Kang; Lin, Ting-Han; Wan, Keng-Cheng; He, Cheng-Tai; Huang, Yu-Han; Yang, Yong-Ping; Wei, Hsuan-Yen; Jeng, U-Ser; Ruan, Jrjeng; Luo, Chan; Huang, Ye; Bazan, Guillermo C; Hsu, Ben B Y Forming Long-Range Order of Semiconducting Polymers through Liquid-Phase Directional Molecular Assemblies MACROMOLECULES, 57 (8), pp. 3544-3556, 2024, DOI: 10.1021/acs.macromol.3c02188. Abstract | BibTeX | Endnote @article{ISI:001203973200001,
title = {Forming Long-Range Order of Semiconducting Polymers through Liquid-Phase Directional Molecular Assemblies},
author = {Minh Nhat Pham and Chun-Jen Su and Yu-Ching Huang and Kun-Ta Lin and Ting-Yu Huang and Yu-Ying Lai and Chen-An Wang and Yong-Kang Liaw and Ting-Han Lin and Keng-Cheng Wan and Cheng-Tai He and Yu-Han Huang and Yong-Ping Yang and Hsuan-Yen Wei and U-Ser Jeng and Jrjeng Ruan and Chan Luo and Ye Huang and Guillermo C Bazan and Ben B Y Hsu},
doi = {10.1021/acs.macromol.3c02188},
times_cited = {0},
issn = {0024-9297},
year = {2024},
date = {2024-04-12},
journal = {MACROMOLECULES},
volume = {57},
number = {8},
pages = {3544-3556},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Intermolecular interactions are crucial in determining the morphology of solution-processed semiconducting polymer thin films. However, these random interactions often lead to disordered or short-range ordered structures. Achieving long-range order in these films has been a challenge due to limited control over microscopic interactions in current techniques. Here, we present a molecular-level methodology that leverages spatial matching of intermolecular dynamics among solutes, solvents, and substrates to induce a directional molecular assembly in weakly bonded polymers. Within the optimized dynamic scale of 2.5 & Aring; between polymer side chains and self-assembled monolayers (SAMs) on nanogrooved substrates, our approach transforms random aggregates into unidirectional fibers with a remarkable increase in the anisotropic stacking ratio from 1 to 11. The Flory-Huggins-based molecular stacking model accurately predicts the transitioning order on various SAMs, validated by morphological and spectroscopic observations. The enhanced structural ordering spans over 3 orders of magnitude in length, rising from the smallest 7.3 nm random crystallites to >14 mu m unidirectional fibers on submillimeter areas. Overall, this study provides insights into the control of complex intermolecular interactions and offers enhanced molecular-level controllability in solution-based processes.},
keywords = {},
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Intermolecular interactions are crucial in determining the morphology of solution-processed semiconducting polymer thin films. However, these random interactions often lead to disordered or short-range ordered structures. Achieving long-range order in these films has been a challenge due to limited control over microscopic interactions in current techniques. Here, we present a molecular-level methodology that leverages spatial matching of intermolecular dynamics among solutes, solvents, and substrates to induce a directional molecular assembly in weakly bonded polymers. Within the optimized dynamic scale of 2.5 & Aring; between polymer side chains and self-assembled monolayers (SAMs) on nanogrooved substrates, our approach transforms random aggregates into unidirectional fibers with a remarkable increase in the anisotropic stacking ratio from 1 to 11. The Flory-Huggins-based molecular stacking model accurately predicts the transitioning order on various SAMs, validated by morphological and spectroscopic observations. The enhanced structural ordering spans over 3 orders of magnitude in length, rising from the smallest 7.3 nm random crystallites to >14 mu m unidirectional fibers on submillimeter areas. Overall, this study provides insights into the control of complex intermolecular interactions and offers enhanced molecular-level controllability in solution-based processes. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUPham, MN
Su, CJ
Huang, YC
Lin, KT
Huang, TY
Lai, YY
Wang, CA
Liaw, YK
Lin, TH
Wan, KC
He, CT
Huang, YH
Yang, YP
Wei, HY
Jeng, US
Ruan, J
Luo, C
Huang, Y
Bazan, GC
Hsu, BBY
- AFMinh Nhat Pham
Chun-Jen Su
Yu-Ching Huang
Kun-Ta Lin
Ting-Yu Huang
Yu-Ying Lai
Chen-An Wang
Yong-Kang Liaw
Ting-Han Lin
Keng-Cheng Wan
Cheng-Tai He
Yu-Han Huang
Yong-Ping Yang
Hsuan-Yen Wei
U-Ser Jeng
Jrjeng Ruan
Chan Luo
Ye Huang
Guillermo C Bazan
Ben B Y Hsu
- TIForming Long-Range Order of Semiconducting Polymers through Liquid-Phase Directional Molecular Assemblies
- SOMACROMOLECULES
- LAEnglish
- DTArticle
- IDEFFICIENT CHARGE-TRANSPORT; THIN-FILMS; POLY(3-HEXYLTHIOPHENE); PERFORMANCE; MORPHOLOGY; MICROSTRUCTURE; SOLUBILITY; CRYSTALS; DENSITY; PACKING
- ABIntermolecular interactions are crucial in determining the morphology of solution-processed semiconducting polymer thin films. However, these random interactions often lead to disordered or short-range ordered structures. Achieving long-range order in these films has been a challenge due to limited control over microscopic interactions in current techniques. Here, we present a molecular-level methodology that leverages spatial matching of intermolecular dynamics among solutes, solvents, and substrates to induce a directional molecular assembly in weakly bonded polymers. Within the optimized dynamic scale of 2.5 & Aring; between polymer side chains and self-assembled monolayers (SAMs) on nanogrooved substrates, our approach transforms random aggregates into unidirectional fibers with a remarkable increase in the anisotropic stacking ratio from 1 to 11. The Flory-Huggins-based molecular stacking model accurately predicts the transitioning order on various SAMs, validated by morphological and spectroscopic observations. The enhanced structural ordering spans over 3 orders of magnitude in length, rising from the smallest 7.3 nm random crystallites to >14 mu m unidirectional fibers on submillimeter areas. Overall, this study provides insights into the control of complex intermolecular interactions and offers enhanced molecular-level controllability in solution-based processes.
- C1[Pham, Minh Nhat; Lin, Kun-Ta; Huang, Ting-Yu; Lai, Yu-Ying; Liaw, Yong-Kang; Lin, Ting-Han; Wan, Keng-Cheng; He, Cheng-Tai; Huang, Yu-Han; Yang, Yong-Ping; Wei, Hsuan-Yen; Ruan, Jrjeng; Hsu, Ben B. Y.] Natl Cheng Kung Univ, Dept Mat Sci & Engn, Tainan 70101, Taiwan.
[Su, Chun-Jen; Wang, Chen-An; Jeng, U-Ser] Natl Synchrotron Radiat Res Ctr, Hsinchu 30077, Taiwan.
[Huang, Yu-Ching] Ming Chi Univ Technol, Dept Mat Engn, New Taipei City 24301, Taiwan.
[Luo, Chan] Intel Corp, Hillsboro, OR 97124 USA.
[Huang, Ye] Dow Chem Co USA, Houston, TX 77077 USA.
[Bazan, Guillermo C.] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore - C3National Cheng Kung University; National Synchrotron Radiation Research Center; Ming Chi University of Technology; Intel Corporation; Dow Chemical Company; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM)
- RPHsu, BBY (corresponding author), Natl Cheng Kung Univ, Dept Mat Sci & Engn, Tainan 70101, Taiwan
- FUMinistry of Science and Technology, Taiwan [MOST 110-2112-M-006-025-MY2]; Ministry of Science and Technology, Taiwan [112-2628-E-131-001-MY4]; NSTC [XRD005100]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; Taiwan Photon Source (TPS) in National Synchrotron Radiation Research Center (NSRRC); Teledyne Princeton Instruments
- FXThe authors are grateful to the financial support of the Ministry of Science and Technology, Taiwan (MOST 110-2112-M-006-025-MY2 and NSTC 112-2628-E-131-001-MY4). We appreciate Dr. Chan Luo, Dr. Ye Huang, and Dr. Guillermo C. Bazan's kind help on the 2D-GIWAXS spectra when they were working in the UCSB. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. The authors gratefully acknowledge the use of code XRD005100 of the machine equipment belonging to the Core Facility Center of National Cheng Kung University. Use of the 13A BioSAXS beamline of the Taiwan Photon Source (TPS) in National Synchrotron Radiation Research Center (NSRRC) is acknowledged. Tzu-Cheng Hsu's and Hong-Hsuan Lin's works on the temperature-dependent UV-vis absorption, water contact angles, and polarized Raman scattering in the Supporting Information are acknowledged. We thank Dr. Feng-Yin Chang's, Dr. Wang-Long Li's, and Dr. Jui-Chao Kuo's valuable comments and discussions. The kind support from Teledyne Princeton Instruments for the discontinued spectrometer is specially appreciated.
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Li, Zejun; Lyu, Pin; Chen, Zhaolong; Guan, Dandan; Yu, Shuang; Zhao, Jinpei; Huang, Pengru; Zhou, Xin; Qiu, Zhizhan; Fang, Hanyan; Hashimoto, Makoto; Lu, Donghui; Song, Fei; Loh, Kian Ping; Zheng, Yi; Shen, Zhi-Xun; Novoselov, Kostya S; Lu, Jiong Beyond Conventional Charge Density Wave for Strongly Enhanced 2D Superconductivity in 1H-TaS2 Superlattices ADVANCED MATERIALS, 2024, DOI: 10.1002/adma.202312341. Abstract | BibTeX | Endnote @article{ISI:001199944200001,
title = {Beyond Conventional Charge Density Wave for Strongly Enhanced 2D Superconductivity in 1H-TaS_{2} Superlattices},
author = {Zejun Li and Pin Lyu and Zhaolong Chen and Dandan Guan and Shuang Yu and Jinpei Zhao and Pengru Huang and Xin Zhou and Zhizhan Qiu and Hanyan Fang and Makoto Hashimoto and Donghui Lu and Fei Song and Kian Ping Loh and Yi Zheng and Zhi-Xun Shen and Kostya S Novoselov and Jiong Lu},
doi = {10.1002/adma.202312341},
times_cited = {0},
issn = {0935-9648},
year = {2024},
date = {2024-04-11},
journal = {ADVANCED MATERIALS},
publisher = {WILEY-V C H VERLAG GMBH},
address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY},
abstract = {Noncentrosymmetric transition metal dichalcogenide (TMD) monolayers offer a fertile platform for exploring unconventional Ising superconductivity (SC) and charge density waves (CDWs). However, the vulnerability of isolated monolayers to structural disorder and environmental oxidation often degrade their electronic coherence. Herein, an alternative approach is reported for fabricating stable and intrinsic monolayers of 1H-TaS2 sandwiched between SnS blocks in a (SnS)(1.15)TaS2 van der Waals (vdW) superlattice. The SnS block layers not only decouple individual 1H-TaS2 sublayers to endow them with monolayer-like electronic characteristics, but also protect the 1H-TaS2 layers from electronic degradation. The results reveal the characteristic 3 x 3 CDW order in 1H-TaS2 sublayers associated with electronic rearrangement in the low-lying sulfur p band, which uncovers a previously undiscovered CDW mechanism rather than the conventional Fermi surface-related framework. Additionally, the (SnS)(1.15)TaS2 superlattice exhibits a strongly enhanced Ising-like SC with a layer-independent T-c of approximate to 3.0 K, comparable to that of the isolated monolayer 1H-TaS2 sample, presumably attributed to their monolayer-like characteristics and retained Fermi states. These results provide new insights into the long-debated CDW order and enhanced SC of monolayer 1H-TaS2, establishing bulk vdW superlattices as promising platforms for investigating exotic collective quantum phases in the 2D limit.},
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Noncentrosymmetric transition metal dichalcogenide (TMD) monolayers offer a fertile platform for exploring unconventional Ising superconductivity (SC) and charge density waves (CDWs). However, the vulnerability of isolated monolayers to structural disorder and environmental oxidation often degrade their electronic coherence. Herein, an alternative approach is reported for fabricating stable and intrinsic monolayers of 1H-TaS2 sandwiched between SnS blocks in a (SnS)(1.15)TaS2 van der Waals (vdW) superlattice. The SnS block layers not only decouple individual 1H-TaS2 sublayers to endow them with monolayer-like electronic characteristics, but also protect the 1H-TaS2 layers from electronic degradation. The results reveal the characteristic 3 x 3 CDW order in 1H-TaS2 sublayers associated with electronic rearrangement in the low-lying sulfur p band, which uncovers a previously undiscovered CDW mechanism rather than the conventional Fermi surface-related framework. Additionally, the (SnS)(1.15)TaS2 superlattice exhibits a strongly enhanced Ising-like SC with a layer-independent T-c of approximate to 3.0 K, comparable to that of the isolated monolayer 1H-TaS2 sample, presumably attributed to their monolayer-like characteristics and retained Fermi states. These results provide new insights into the long-debated CDW order and enhanced SC of monolayer 1H-TaS2, establishing bulk vdW superlattices as promising platforms for investigating exotic collective quantum phases in the 2D limit. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AULi, ZJ
Lyu, P
Chen, ZL
Guan, DD
Yu, S
Zhao, JP
Huang, PR
Zhou, X
Qiu, ZZ
Fang, HY
Hashimoto, M
Lu, DH
Song, F
Loh, KP
Zheng, Y
Shen, ZX
Novoselov, KS
Lu, J
- AFZejun Li
Pin Lyu
Zhaolong Chen
Dandan Guan
Shuang Yu
Jinpei Zhao
Pengru Huang
Xin Zhou
Zhizhan Qiu
Hanyan Fang
Makoto Hashimoto
Donghui Lu
Fei Song
Kian Ping Loh
Yi Zheng
Zhi-Xun Shen
Kostya S Novoselov
Jiong Lu
- TIBeyond Conventional Charge Density Wave for Strongly Enhanced 2D Superconductivity in 1H-TaS2 Superlattices
- SOADVANCED MATERIALS
- LAEnglish
- DTArticle
- DE2D Superconductivity; 2D Van Der Waals Superlattices; Charge Density Wave; Electronic Rearrangement; Monolayer-like Electronic Characteristics
- IDISING SUPERCONDUCTIVITY; METAL; SPIN
- ABNoncentrosymmetric transition metal dichalcogenide (TMD) monolayers offer a fertile platform for exploring unconventional Ising superconductivity (SC) and charge density waves (CDWs). However, the vulnerability of isolated monolayers to structural disorder and environmental oxidation often degrade their electronic coherence. Herein, an alternative approach is reported for fabricating stable and intrinsic monolayers of 1H-TaS2 sandwiched between SnS blocks in a (SnS)(1.15)TaS2 van der Waals (vdW) superlattice. The SnS block layers not only decouple individual 1H-TaS2 sublayers to endow them with monolayer-like electronic characteristics, but also protect the 1H-TaS2 layers from electronic degradation. The results reveal the characteristic 3 x 3 CDW order in 1H-TaS2 sublayers associated with electronic rearrangement in the low-lying sulfur p band, which uncovers a previously undiscovered CDW mechanism rather than the conventional Fermi surface-related framework. Additionally, the (SnS)(1.15)TaS2 superlattice exhibits a strongly enhanced Ising-like SC with a layer-independent T-c of approximate to 3.0 K, comparable to that of the isolated monolayer 1H-TaS2 sample, presumably attributed to their monolayer-like characteristics and retained Fermi states. These results provide new insights into the long-debated CDW order and enhanced SC of monolayer 1H-TaS2, establishing bulk vdW superlattices as promising platforms for investigating exotic collective quantum phases in the 2D limit.
- C1[Li, Zejun] Southeast Univ, Sch Phys, Key Lab Quantum Mat & Devices, Minist Educ, Nanjing 211189, Peoples R China.
[Li, Zejun; Lyu, Pin; Zhou, Xin; Fang, Hanyan; Loh, Kian Ping; Lu, Jiong] Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore.
[Li, Zejun] Purple Mt Labs, Nanjing 211111, Peoples R China.
[Chen, Zhaolong; Zhao, Jinpei; Huang, Pengru; Qiu, Zhizhan; Novoselov, Kostya S.; Lu, Jiong] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore.
[Chen, Zhaolong] Peking Univ, Shenzhen Grad Sch, Sch Adv Mat, Shenzhen 518055, Peoples R China.
[Guan, Dandan] Shanghai Jiao Tong Univ, Sch Phys & Astron, Key Lab Artificial Struct & Quantum Control, Minist Educ,TD Lee Inst, Shanghai 200240, Peoples R China.
[Yu, Shuang; Zheng, Yi] Zhejiang Univ, Sch Phys, Zhejiang Prov Key Lab Quantum Technol & Device, Hangzhou 310027, Peoples R China.
[Yu, Shuang; Zheng, Yi] Zhejiang Univ, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R China.
[Huang, Pengru] Guilin Univ Elect Technol, Sch Mat Sci & Engn, Guangxi Key Lab Informat Mat, Guilin 541004, Peoples R China.
[Hashimoto, Makoto; Lu, Donghui; Shen, Zhi-Xun] SLAC Natl Accelerator Lab, Stanford Inst Mat & Energy Sci, Menlo Pk, CA 94025 USA.
[Song, Fei] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facial, Shanghai 201204, Peoples R China.
[Shen, Zhi-Xun] Stanford Univ, Dept Phys & Appl Phys, Geballe Lab Adv Mat, Stanford, CA 94305 USA - C3Southeast University - China; National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); Peking University; Shanghai Jiao Tong University; Zhejiang University; Zhejiang University; Guilin University of Electronic Technology; Stanford University; United States Department of Energy (DOE); SLAC National Accelerator Laboratory; Chinese Academy of Sciences; Shanghai Advanced Research Institute, CAS; Stanford University
- RPLu, J (corresponding author), Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore; Huang, PR (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore; Zheng, Y (corresponding author), Zhejiang Univ, Sch Phys, Zhejiang Prov Key Lab Quantum Technol & Device, Hangzhou 310027, Peoples R China; Zheng, Y (corresponding author), Zhejiang Univ, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R China; Huang, PR (corresponding author), Guilin Univ Elect Technol, Sch Mat Sci & Engn, Guangxi Key Lab Informat Mat, Guilin 541004, Peoples R China
- FUResearch Fund of Southeast University [MOE T2EP50121-0008, MOE-T2EP10221-0005]; MOE Tier 2 grants [EDUNC-33-18-279-V12]; Ministry of Education, Singapore, under the Research Centre of Excellence award from the Institute for Functional Intelligent Materials [22375041]; National Nature Science Foundation of China [RF1028623202]; Start-up Research Fund of Southeast University [2021YFB3802400]; Open Research Fund of the Key Laboratory of Quantum Materials and Devices (Southeast University), Ministry of Education [52161037]; National Key Research and Development Program; National Natural Science Foundation of China; US DOE Office of Basic Energy Sciences, Division of Materials Science and Engineering
- FXZ.L., P.L., Z.C., D.G., S.Y., J.Z. contributed equally to this work. J.L. acknowledges the support from MOE Tier 2 grants (MOE T2EP50121-0008 and MOE-T2EP10221-0005). This work was supported by the Ministry of Education, Singapore, under the Research Centre of Excellence award from the Institute for Functional Intelligent Materials (I-FIM, project No. EDUNC-33-18-279-V12). Z.L. acknowledges support from the National Nature Science Foundation of China (Grant No. 22375041), the Start-up Research Fund of Southeast University (Grant No. RF1028623202), and the Open Research Fund of the Key Laboratory of Quantum Materials and Devices (Southeast University), Ministry of Education. P.R.H. acknowledges the support from the National Key Research and Development Program (No. 2021YFB3802400) and the National Natural Science Foundation of China (No. 52161037). The ARPES work was supported by the US DOE Office of Basic Energy Sciences, Division of Materials Science and Engineering.
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Lin, Fanrong; Liu, Jiawei; Lu, Huan; Liu, Xin; Liu, Ying; Hu, Zhili; Lyu, Pin; Zhang, Zhuhua; Martin, Jens; Guo, Wanlin; Liu, Yanpeng Evolution of Graphene Dirac Fermions in Electric Double-Layer Transistors with a Soft Barrier ADVANCED FUNCTIONAL MATERIALS, 2024, DOI: 10.1002/adfm.202400553. Abstract | BibTeX | Endnote @article{ISI:001195156600001,
title = {Evolution of Graphene Dirac Fermions in Electric Double-Layer Transistors with a Soft Barrier},
author = {Fanrong Lin and Jiawei Liu and Huan Lu and Xin Liu and Ying Liu and Zhili Hu and Pin Lyu and Zhuhua Zhang and Jens Martin and Wanlin Guo and Yanpeng Liu},
doi = {10.1002/adfm.202400553},
times_cited = {0},
issn = {1616-301X},
year = {2024},
date = {2024-04-02},
journal = {ADVANCED FUNCTIONAL MATERIALS},
publisher = {WILEY-V C H VERLAG GMBH},
address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY},
abstract = {The interface and dielectric environment of graphene transistors are of great importance to commercial circuit integrations. The tangling bond in oxide-based dielectric severely lagged the carrier mobility while the 2D dielectric layer (for instance, hexagonal boron nitride) unavoidably hastened complicated condensed physics even at room temperature. Herein, multilayer black phosphorus (BP) a versatile and widely-tunable dielectric candidate for manifesting graphene fermions is demonstrated. Because of hetero-interfacial charge redistributions, a vertical electric double-layer between the bottom BP layer and top graphene spontaneously forms with the central BP layer as a soft barrier. Under dual-gate modulation, abnormal step-like evolution of Dirac fermions and charge-transfer quantum Hall effect arises while the intrinsic Dirac behavior of graphene is preserved, ascribing to the gate-tunable charge redistributions of dielectric BP layer. Moreover, the electric double-layer transistors apply equally well to bilayer graphene with similar Dirac behavior but an enhanced interfacial charge interference. The findings not only create a new avenue to manipulate the fermions by assembling graphene with narrow-gapped 2D layered materials but also promote electric double-layer transistors as a new build block to design multifunctional devices.},
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The interface and dielectric environment of graphene transistors are of great importance to commercial circuit integrations. The tangling bond in oxide-based dielectric severely lagged the carrier mobility while the 2D dielectric layer (for instance, hexagonal boron nitride) unavoidably hastened complicated condensed physics even at room temperature. Herein, multilayer black phosphorus (BP) a versatile and widely-tunable dielectric candidate for manifesting graphene fermions is demonstrated. Because of hetero-interfacial charge redistributions, a vertical electric double-layer between the bottom BP layer and top graphene spontaneously forms with the central BP layer as a soft barrier. Under dual-gate modulation, abnormal step-like evolution of Dirac fermions and charge-transfer quantum Hall effect arises while the intrinsic Dirac behavior of graphene is preserved, ascribing to the gate-tunable charge redistributions of dielectric BP layer. Moreover, the electric double-layer transistors apply equally well to bilayer graphene with similar Dirac behavior but an enhanced interfacial charge interference. The findings not only create a new avenue to manipulate the fermions by assembling graphene with narrow-gapped 2D layered materials but also promote electric double-layer transistors as a new build block to design multifunctional devices. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AULin, FR
Liu, JW
Lu, H
Liu, X
Liu, Y
Hu, ZL
Lyu, P
Zhang, ZH
Martin, J
Guo, WL
Liu, YP
- AFFanrong Lin
Jiawei Liu
Huan Lu
Xin Liu
Ying Liu
Zhili Hu
Pin Lyu
Zhuhua Zhang
Jens Martin
Wanlin Guo
Yanpeng Liu
- TIEvolution of Graphene Dirac Fermions in Electric Double-Layer Transistors with a Soft Barrier
- SOADVANCED FUNCTIONAL MATERIALS
- LAEnglish
- DTArticle
- DEBlack Phosphorus; Electric Double-layer; Gate-tunable; Graphene; Surface States
- IDBLACK; BANDGAP; BORON
- ABThe interface and dielectric environment of graphene transistors are of great importance to commercial circuit integrations. The tangling bond in oxide-based dielectric severely lagged the carrier mobility while the 2D dielectric layer (for instance, hexagonal boron nitride) unavoidably hastened complicated condensed physics even at room temperature. Herein, multilayer black phosphorus (BP) a versatile and widely-tunable dielectric candidate for manifesting graphene fermions is demonstrated. Because of hetero-interfacial charge redistributions, a vertical electric double-layer between the bottom BP layer and top graphene spontaneously forms with the central BP layer as a soft barrier. Under dual-gate modulation, abnormal step-like evolution of Dirac fermions and charge-transfer quantum Hall effect arises while the intrinsic Dirac behavior of graphene is preserved, ascribing to the gate-tunable charge redistributions of dielectric BP layer. Moreover, the electric double-layer transistors apply equally well to bilayer graphene with similar Dirac behavior but an enhanced interfacial charge interference. The findings not only create a new avenue to manipulate the fermions by assembling graphene with narrow-gapped 2D layered materials but also promote electric double-layer transistors as a new build block to design multifunctional devices.
- C3Nanjing University of Aeronautics & Astronautics; Nanjing University of Aeronautics & Astronautics; National University of Singapore; National University of Singapore; Leibniz Institut fur Kristallzuchtung (IKZ)
- RPGuo, WL (corresponding author), Nanjing Univ Aeronaut & Astronaut, Key Lab Intelligent Nano Mat & Devices, State Key Lab Mech & Control Mech Struct, Minist Educ, Nanjing 210016, Peoples R China
- FXThe authors wish to acknowledge the financial support provided by the National Natural Science Foundation of China (Grant No. 12372111, 12304106, 12104228), the financial support provided by the National Key Research and Development Program of China (2019YFA0705400), the Natural Science Foundation of Jiangsu Province (Grant Nos. BK20210312), the Fundamental Research Funds for the Central Universities and the State Administration of Science, Technology and Industry for National Defense (NE2023006, NC2023001, NJ2023002, NJ2022002, ILF23010, THB24004), the Program for Innovative Talents and Entrepreneur in Jiangsu, Research Fund of State Key Laboratory of Mechanics and Control of Mechanical Structures (MCMS-I-0422K01), a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions and the Postdoctoral Science Foundation of Jiangsu Province (YBA21046).
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Cai, Xiaofan; Li, Ming; Chen, Chao; Du, Renjun; Guo, Zijing; Wang, Ping; Ma, Guodong; Wu, Xinglong; Wang, Zhiyuan; Han, Yaqing; Lian, Fuzhuo; Xiao, Jingkuan; Jiang, Siqi; Wang, Lei; Mayorov, Alexander S; Gao, Libo; Novoselov, Kostya S; Yu, Geliang Blood for Graphene Production ACS APPLIED NANO MATERIALS, 7 (7), pp. 8238-8246, 2024, DOI: 10.1021/acsanm.4c00914. Abstract | BibTeX | Endnote @article{ISI:001195925500001,
title = {Blood for Graphene Production},
author = {Xiaofan Cai and Ming Li and Chao Chen and Renjun Du and Zijing Guo and Ping Wang and Guodong Ma and Xinglong Wu and Zhiyuan Wang and Yaqing Han and Fuzhuo Lian and Jingkuan Xiao and Siqi Jiang and Lei Wang and Alexander S Mayorov and Libo Gao and Kostya S Novoselov and Geliang Yu},
doi = {10.1021/acsanm.4c00914},
times_cited = {0},
year = {2024},
date = {2024-04-02},
journal = {ACS APPLIED NANO MATERIALS},
volume = {7},
number = {7},
pages = {8238-8246},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Blood, a ubiquitous and fundamental carbohydrate material composed of plasma, red blood cells, white blood cells, and platelets, has been playing an important role in biology, life science, history, and religious studies, while graphene has garnered significant attention due to its exceptional properties and extensive range of potential applications. Achieving environmentally friendly, cost-effective growth using hybrid precursors and obtaining high-quality graphene through a straightforward chemical vapor deposition process have been traditionally considered mutually exclusive. This study demonstrates that we can produce high-quality graphene domains with controlled thickness through a one-step growth process at atmospheric pressure using blood as a precursor. Raman spectroscopy confirms the uniformity of the blood-grown graphene films, and observing the half-integer quantum Hall effect in the measured devices highlights their outstanding electronic properties. This unprecedented approach opens possibilities for blood application, facilitating an unconventional route for graphene growth applications.},
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Blood, a ubiquitous and fundamental carbohydrate material composed of plasma, red blood cells, white blood cells, and platelets, has been playing an important role in biology, life science, history, and religious studies, while graphene has garnered significant attention due to its exceptional properties and extensive range of potential applications. Achieving environmentally friendly, cost-effective growth using hybrid precursors and obtaining high-quality graphene through a straightforward chemical vapor deposition process have been traditionally considered mutually exclusive. This study demonstrates that we can produce high-quality graphene domains with controlled thickness through a one-step growth process at atmospheric pressure using blood as a precursor. Raman spectroscopy confirms the uniformity of the blood-grown graphene films, and observing the half-integer quantum Hall effect in the measured devices highlights their outstanding electronic properties. This unprecedented approach opens possibilities for blood application, facilitating an unconventional route for graphene growth applications. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUCai, XF
Li, M
Chen, C
Du, RJ
Guo, ZJ
Wang, P
Ma, GD
Wu, XL
Wang, ZY
Han, YQ
Lian, FZ
Xiao, JK
Jiang, SQ
Wang, L
Mayorov, AS
Gao, LB
Novoselov, KS
Yu, GL
- AFXiaofan Cai
Ming Li
Chao Chen
Renjun Du
Zijing Guo
Ping Wang
Guodong Ma
Xinglong Wu
Zhiyuan Wang
Yaqing Han
Fuzhuo Lian
Jingkuan Xiao
Siqi Jiang
Lei Wang
Alexander S Mayorov
Libo Gao
Kostya S Novoselov
Geliang Yu
- TIBlood for Graphene Production
- SOACS APPLIED NANO MATERIALS
- LAEnglish
- DTArticle
- DEBlood; Graphene; CVD; One-stepgrowth; Cost-effective
- IDVAPOR-DEPOSITION GROWTH; FEW-LAYER GRAPHENE; ELECTRONIC-PROPERTIES; COPPER; HYDROGEN; SINGLE
- ABBlood, a ubiquitous and fundamental carbohydrate material composed of plasma, red blood cells, white blood cells, and platelets, has been playing an important role in biology, life science, history, and religious studies, while graphene has garnered significant attention due to its exceptional properties and extensive range of potential applications. Achieving environmentally friendly, cost-effective growth using hybrid precursors and obtaining high-quality graphene through a straightforward chemical vapor deposition process have been traditionally considered mutually exclusive. This study demonstrates that we can produce high-quality graphene domains with controlled thickness through a one-step growth process at atmospheric pressure using blood as a precursor. Raman spectroscopy confirms the uniformity of the blood-grown graphene films, and observing the half-integer quantum Hall effect in the measured devices highlights their outstanding electronic properties. This unprecedented approach opens possibilities for blood application, facilitating an unconventional route for graphene growth applications.
- C1[Cai, Xiaofan; Li, Ming; Chen, Chao; Du, Renjun; Guo, Zijing; Wang, Ping; Ma, Guodong; Wu, Xinglong; Wang, Zhiyuan; Han, Yaqing; Lian, Fuzhuo; Xiao, Jingkuan; Jiang, Siqi; Wang, Lei; Mayorov, Alexander S.; Gao, Libo; Yu, Geliang] Nanjing Univ, Sch Phys, Natl Lab Solid State Microstruct, Nanjing 210093, Peoples R China.
[Lian, Fuzhuo] Chongqing 2D Mat Inst, Chongqing 400714, Peoples R China.
[Novoselov, Kostya S.] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore - C3Nanjing University; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore
- RPMayorov, AS (corresponding author), Nanjing Univ, Sch Phys, Natl Lab Solid State Microstruct, Nanjing 210093, Peoples R China; Novoselov, KS (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore
- FURoyal Society [EDUNC-33-18-279-V12]; Ministry of Education, Singapore (Research Centre of Excellence award) [RSRPR190000]; Royal Society (UK) [2022YFA120470, 2021YFA1400400]; National Key R&D Program of China [12004173, 11974169]; National Natural Science Foundation of China [020414380087, 020414913201]; Fundamental Research Funds for the Central Universities; Mono Technology Co, Ltd
- FXK.S.N. is grateful to the Ministry of Education, Singapore (Research Centre of Excellence award to the Institute for Functional Intelligent Materials, I-FIM, project no. EDUNC-33-18-279-V12) and to the Royal Society (UK, grant number RSRPR190000) for support. G.Y. acknowledges the financial support from the National Key R&D Program of China (nos. 2022YFA120470 and 2021YFA1400400), the National Natural Science Foundation of China (nos. 12004173 and 11974169), and the Fundamental Research Funds for the Central Universities (nos. 020414380087 and 020414913201). And the authors would like to thank Mono Technology Co, Ltd (http://www.wuximono.com) for the CVD growth system, which was used for graphene and 2D materials production.
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Kipczak, Lucja; Karmakar, Arka; Grzeszczyk, Magdalena; Janiszewska, Roza; Wozniak, Tomasz; Chen, Zhaolong; Pawlowski, Jan; Watanabe, Kenji; Taniguchi, Takashi; Babinski, Adam; Koperski, Maciej; Molas, Maciej R Resonant Raman scattering of few layers CrBr3 SCIENTIFIC REPORTS, 14 (1), 2024, DOI: 10.1038/s41598-024-57622-w. Abstract | BibTeX | Endnote @article{ISI:001195862400057,
title = {Resonant Raman scattering of few layers CrBr_{3}},
author = {Lucja Kipczak and Arka Karmakar and Magdalena Grzeszczyk and Roza Janiszewska and Tomasz Wozniak and Zhaolong Chen and Jan Pawlowski and Kenji Watanabe and Takashi Taniguchi and Adam Babinski and Maciej Koperski and Maciej R Molas},
doi = {10.1038/s41598-024-57622-w},
times_cited = {0},
issn = {2045-2322},
year = {2024},
date = {2024-03-29},
journal = {SCIENTIFIC REPORTS},
volume = {14},
number = {1},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {We investigate the vibrational and magnetic properties of thin layers of chromium tribromide (CrBr3) with a thickness ranging from three to twenty layers (3-20 L) revealed by the Raman scattering (RS) technique. Systematic dependence of the RS process efficiency on the energy of the laser excitation is explored for four different excitation energies: 1.96 eV, 2.21 eV, 2.41 eV, and 3.06 eV. Our characterization demonstrates that for 12 L CrBr3, 3.06 eV excitation could be considered resonant with interband electronic transitions due to the enhanced intensity of the Raman-active scattering resonances and the qualitative change in the Raman spectra. Polarization-resolved RS measurements for 12 L CrBr3 and first-principles calculations allow us to identify five observable phonon modes characterized by distinct symmetries, classified as the Ag and Eg modes. The evolution of phonon modes with temperature for a 16 L CrBr3 encapsulated in hexagonal boron nitride flakes demonstrates alterations of phonon energies and/or linewidths of resonances indicative of a transition between the paramagnetic and ferromagnetic state at Curie temperature (T-C approximate to 50 K). The exploration of the effects of thickness on the phonon energies demonstrated small variations pronounces exclusively for the thinnest layers in the vicinity of 3-5 L. We propose that this observation can be due to the strong localization in the real space of interband electronic excitations, limiting the effects of confinement for resonantly excited Raman modes to atomically thin layers.},
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We investigate the vibrational and magnetic properties of thin layers of chromium tribromide (CrBr3) with a thickness ranging from three to twenty layers (3-20 L) revealed by the Raman scattering (RS) technique. Systematic dependence of the RS process efficiency on the energy of the laser excitation is explored for four different excitation energies: 1.96 eV, 2.21 eV, 2.41 eV, and 3.06 eV. Our characterization demonstrates that for 12 L CrBr3, 3.06 eV excitation could be considered resonant with interband electronic transitions due to the enhanced intensity of the Raman-active scattering resonances and the qualitative change in the Raman spectra. Polarization-resolved RS measurements for 12 L CrBr3 and first-principles calculations allow us to identify five observable phonon modes characterized by distinct symmetries, classified as the Ag and Eg modes. The evolution of phonon modes with temperature for a 16 L CrBr3 encapsulated in hexagonal boron nitride flakes demonstrates alterations of phonon energies and/or linewidths of resonances indicative of a transition between the paramagnetic and ferromagnetic state at Curie temperature (T-C approximate to 50 K). The exploration of the effects of thickness on the phonon energies demonstrated small variations pronounces exclusively for the thinnest layers in the vicinity of 3-5 L. We propose that this observation can be due to the strong localization in the real space of interband electronic excitations, limiting the effects of confinement for resonantly excited Raman modes to atomically thin layers. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUKipczak, L
Karmakar, A
Grzeszczyk, M
Janiszewska, R
Wozniak, T
Chen, ZL
Pawlowski, J
Watanabe, K
Taniguchi, T
Babinski, A
Koperski, M
Molas, MR
- AFLucja Kipczak
Arka Karmakar
Magdalena Grzeszczyk
Roza Janiszewska
Tomasz Wozniak
Zhaolong Chen
Jan Pawlowski
Kenji Watanabe
Takashi Taniguchi
Adam Babinski
Maciej Koperski
Maciej R Molas
- TIResonant Raman scattering of few layers CrBr3
- SOSCIENTIFIC REPORTS
- LAEnglish
- DTArticle
- IDINITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; MAGNETIC-PROPERTIES; PHONON; TRANSITION; SPECTRA
- ABWe investigate the vibrational and magnetic properties of thin layers of chromium tribromide (CrBr3) with a thickness ranging from three to twenty layers (3-20 L) revealed by the Raman scattering (RS) technique. Systematic dependence of the RS process efficiency on the energy of the laser excitation is explored for four different excitation energies: 1.96 eV, 2.21 eV, 2.41 eV, and 3.06 eV. Our characterization demonstrates that for 12 L CrBr3, 3.06 eV excitation could be considered resonant with interband electronic transitions due to the enhanced intensity of the Raman-active scattering resonances and the qualitative change in the Raman spectra. Polarization-resolved RS measurements for 12 L CrBr3 and first-principles calculations allow us to identify five observable phonon modes characterized by distinct symmetries, classified as the Ag and Eg modes. The evolution of phonon modes with temperature for a 16 L CrBr3 encapsulated in hexagonal boron nitride flakes demonstrates alterations of phonon energies and/or linewidths of resonances indicative of a transition between the paramagnetic and ferromagnetic state at Curie temperature (T-C approximate to 50 K). The exploration of the effects of thickness on the phonon energies demonstrated small variations pronounces exclusively for the thinnest layers in the vicinity of 3-5 L. We propose that this observation can be due to the strong localization in the real space of interband electronic excitations, limiting the effects of confinement for resonantly excited Raman modes to atomically thin layers.
- C3University of Warsaw; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; Wroclaw University of Science & Technology; University of Warsaw; Peking University; National Institute for Materials Science; National Institute for Materials Science; National University of Singapore
- RPKipczak, L (corresponding author), Warsaw Univ, Fac Phys, Inst Expt Phys, Pasteura 5, PL-02 093 Warsaw, Poland
- FXThe work was supported by the National Science Centre, Poland (Grant No. 2020/37/B/ST3/02311), the Ministry of Education (Singapore) through the Research Centre of Excellence program (Grant EDUN C-33-18-279-V12, I-FIM) and under its Academic Research Fund Tier 2 (MOE-T2EP50122-0012), and the Air Force Office of Scientific Research and the Office of Naval Research Global under award number FA8655-21-1-7026. The calculations were carried out with the support of the Interdisciplinary Centre for Mathematical and Computational Modelling University of Warsaw (ICM UW) under computational allocation no G95-1773. T. W. acknowledge support form the National Science Centre Grant No. 2023/48/C/ST3/00309. K.W. and T.T. acknowledge support from the JSPS KAKENHI (Grant Numbers 21H05233 and 23H02052) and World Premier International Research Center Initiative (WPI), MEXT, Japan.
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Bong, Jia Hui; Grebenchuk, Sergey; Nikolaev, Konstantin G; Chee, Celestine P T; Yang, Kou; Chen, Siyu; Baranov, Denis; Woods, Colin R; Andreeva, Daria V; Novoselov, Kostya S Graphene oxide-DNA/graphene oxide-PDDA sandwiched membranes with neuromorphic function NANOSCALE HORIZONS, 9 (5), pp. 863-872, 2024, DOI: 10.1039/d3nh00570d. Abstract | BibTeX | Endnote @article{ISI:001191219100001,
title = {Graphene oxide-DNA/graphene oxide-PDDA sandwiched membranes with neuromorphic function},
author = {Jia Hui Bong and Sergey Grebenchuk and Konstantin G Nikolaev and Celestine P T Chee and Kou Yang and Siyu Chen and Denis Baranov and Colin R Woods and Daria V Andreeva and Kostya S Novoselov},
doi = {10.1039/d3nh00570d},
times_cited = {0},
issn = {2055-6756},
year = {2024},
date = {2024-03-27},
journal = {NANOSCALE HORIZONS},
volume = {9},
number = {5},
pages = {863-872},
publisher = {ROYAL SOC CHEMISTRY},
address = {THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND},
abstract = {The behavior of polyelectrolytes in confined spaces has direct relevance to the protein mediated ion transport in living organisms. In this paper, we govern lithium chloride transport by the interface provided by polyelectrolytes, polycation, poly(diallyldimethylammonium chloride) (PDDA) and, polyanion, double stranded deoxyribonucleic acid (dsDNA), in confined graphene oxide (GO) membranes. Polyelectrolyte-GO interfaces demonstrate neuromorphic functions that were successfully applied with nanochannel ion interactions contributed, resulting in ion memory effects. Excitatory and inhibitory post-synaptic currents were tuned continuously as the number of pulses applied increased accordingly, increasing decay times. Furthermore, we demonstrated the short-term memory of a trained vs untrained device in computation. On account of its simple and safe production along with its robustness and stability, we anticipate our device to be a low dimensional building block for arrays to embed artificial neural networks in hardware for neuromorphic computing. Additionally, incorporating such devices with sensing and actuating parts for a complete feedback loop produces robotics with its own ability to learn by modifying actuation based on sensing data.},
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The behavior of polyelectrolytes in confined spaces has direct relevance to the protein mediated ion transport in living organisms. In this paper, we govern lithium chloride transport by the interface provided by polyelectrolytes, polycation, poly(diallyldimethylammonium chloride) (PDDA) and, polyanion, double stranded deoxyribonucleic acid (dsDNA), in confined graphene oxide (GO) membranes. Polyelectrolyte-GO interfaces demonstrate neuromorphic functions that were successfully applied with nanochannel ion interactions contributed, resulting in ion memory effects. Excitatory and inhibitory post-synaptic currents were tuned continuously as the number of pulses applied increased accordingly, increasing decay times. Furthermore, we demonstrated the short-term memory of a trained vs untrained device in computation. On account of its simple and safe production along with its robustness and stability, we anticipate our device to be a low dimensional building block for arrays to embed artificial neural networks in hardware for neuromorphic computing. Additionally, incorporating such devices with sensing and actuating parts for a complete feedback loop produces robotics with its own ability to learn by modifying actuation based on sensing data. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUBong, JH
Grebenchuk, S
Nikolaev, KG
Chee, CPT
Yang, K
Chen, SY
Baranov, D
Woods, CR
Andreeva, DV
Novoselov, KS
- AFJia Hui Bong
Sergey Grebenchuk
Konstantin G Nikolaev
Celestine P T Chee
Kou Yang
Siyu Chen
Denis Baranov
Colin R Woods
Daria V Andreeva
Kostya S Novoselov
- TIGraphene oxide-DNA/graphene oxide-PDDA sandwiched membranes with neuromorphic function
- SONANOSCALE HORIZONS
- LAEnglish
- DTArticle
- IDLOW-VOLTAGE; SYNAPSES; NETWORK; NEURONS; DNA; PH
- ABThe behavior of polyelectrolytes in confined spaces has direct relevance to the protein mediated ion transport in living organisms. In this paper, we govern lithium chloride transport by the interface provided by polyelectrolytes, polycation, poly(diallyldimethylammonium chloride) (PDDA) and, polyanion, double stranded deoxyribonucleic acid (dsDNA), in confined graphene oxide (GO) membranes. Polyelectrolyte-GO interfaces demonstrate neuromorphic functions that were successfully applied with nanochannel ion interactions contributed, resulting in ion memory effects. Excitatory and inhibitory post-synaptic currents were tuned continuously as the number of pulses applied increased accordingly, increasing decay times. Furthermore, we demonstrated the short-term memory of a trained vs untrained device in computation. On account of its simple and safe production along with its robustness and stability, we anticipate our device to be a low dimensional building block for arrays to embed artificial neural networks in hardware for neuromorphic computing. Additionally, incorporating such devices with sensing and actuating parts for a complete feedback loop produces robotics with its own ability to learn by modifying actuation based on sensing data.
- C3Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National University of Singapore
- RPAndreeva, DV (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore; Andreeva, DV (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore
- FXThis research is supported by the Ministry of Education, Singapore, under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (I-FIM, project no. EDUNC-33-18-279-V12).
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Meshkov, Aleksei V; Nikitina, Anna A; Aliev, Timur A; Gromov, Vladislav S; Chen, Siyu; Yang, Kou; Wang, Qian; Novoselov, Kostya S; Andreeva, Daria V; Skorb, Ekaterina V Robotization of Synthesis and Analysis Process of Graphene Oxide-Based Membrane ADVANCED INTELLIGENT SYSTEMS, 2024, DOI: 10.1002/aisy.202300655. Abstract | BibTeX | Endnote @article{ISI:001188990000001,
title = {Robotization of Synthesis and Analysis Process of Graphene Oxide-Based Membrane},
author = {Aleksei V Meshkov and Anna A Nikitina and Timur A Aliev and Vladislav S Gromov and Siyu Chen and Kou Yang and Qian Wang and Kostya S Novoselov and Daria V Andreeva and Ekaterina V Skorb},
doi = {10.1002/aisy.202300655},
times_cited = {0},
year = {2024},
date = {2024-03-22},
journal = {ADVANCED INTELLIGENT SYSTEMS},
publisher = {WILEY},
address = {111 RIVER ST, HOBOKEN 07030-5774, NJ USA},
abstract = {The use of collaborative robots (Cobots) for materials development in chemical laboratories is currently of high priority. Herein, the Cobot is used for autonomous continued analysis and synthesis of graphene oxide-polyethyleneimine-based membrane to unify a method and prospects for big data collection are shown. Membranes have already demonstrated a selective affinity to potassium cations and promised to adjust permeability for other cations by changing pH. The Cobot allows a variation of membrane properties by its composition modification. The present strategy combines a novel perspective of material production by Cobots and the application of machine learning. Moreover, the current approach can be adapted for different modern chemical laboratories for various scientific research, and the proper workflow is provided.},
keywords = {},
pubstate = {published},
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The use of collaborative robots (Cobots) for materials development in chemical laboratories is currently of high priority. Herein, the Cobot is used for autonomous continued analysis and synthesis of graphene oxide-polyethyleneimine-based membrane to unify a method and prospects for big data collection are shown. Membranes have already demonstrated a selective affinity to potassium cations and promised to adjust permeability for other cations by changing pH. The Cobot allows a variation of membrane properties by its composition modification. The present strategy combines a novel perspective of material production by Cobots and the application of machine learning. Moreover, the current approach can be adapted for different modern chemical laboratories for various scientific research, and the proper workflow is provided. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUMeshkov, AV
Nikitina, AA
Aliev, TA
Gromov, VS
Chen, SY
Yang, K
Wang, Q
Novoselov, KS
Andreeva, DV
Skorb, EV
- AFAleksei V Meshkov
Anna A Nikitina
Timur A Aliev
Vladislav S Gromov
Siyu Chen
Kou Yang
Qian Wang
Kostya S Novoselov
Daria V Andreeva
Ekaterina V Skorb
- TIRobotization of Synthesis and Analysis Process of Graphene Oxide-Based Membrane
- SOADVANCED INTELLIGENT SYSTEMS
- LAEnglish
- DTArticle
- DEArtificial Vision; Graphene Oxide; Machine Learning; Polyethyleneimine; Robotization
- ABThe use of collaborative robots (Cobots) for materials development in chemical laboratories is currently of high priority. Herein, the Cobot is used for autonomous continued analysis and synthesis of graphene oxide-polyethyleneimine-based membrane to unify a method and prospects for big data collection are shown. Membranes have already demonstrated a selective affinity to potassium cations and promised to adjust permeability for other cations by changing pH. The Cobot allows a variation of membrane properties by its composition modification. The present strategy combines a novel perspective of material production by Cobots and the application of machine learning. Moreover, the current approach can be adapted for different modern chemical laboratories for various scientific research, and the proper workflow is provided.
- C1[Meshkov, Aleksei V.; Nikitina, Anna A.; Aliev, Timur A.; Gromov, Vladislav S.; Skorb, Ekaterina V.] ITMO Univ, Infochem Sci Ctr, 9 Lomonosova St, St Petersburg 191002, Russia.
[Chen, Siyu; Yang, Kou; Wang, Qian; Novoselov, Kostya S.; Andreeva, Daria V.] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore.
[Chen, Siyu; Yang, Kou; Wang, Qian; Novoselov, Kostya S.; Andreeva, Daria V.] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore - C3ITMO University; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National University of Singapore
- RPSkorb, EV (corresponding author), ITMO Univ, Infochem Sci Ctr, 9 Lomonosova St, St Petersburg 191002, Russia; Andreeva, DV (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore; Andreeva, DV (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore
- FURussian Science Foundation [EDUN C-33-18-279-V12]; Research Centre of Excellence Program [21-13-00403]; Ministry of Education (Singapore); RSF
- FXThe authors acknowledge the Research Centre of Excellence Program (Award EDUN C-33-18-279-V12, Institute for Functional Intelligent Materials) of the Ministry of Education (Singapore) and RSF grant no. 21-13-00403. Priority 2030 is acknowledged for infrastructure support.
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- SCAutomation & Control Systems; Computer Science; Robotics
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|
Tan, Hui Li; Donato, Katarzyna Z; Costa, Mariana C F; Carvalho, Alexandra; Trushin, Maxim; Ng, Pei Rou; Yau, Xin Hui; Koon, Gavin K W; Tolasz, Jakub; Nemeckova, Zuzana; Ecorchard, Petra; Donato, Ricardo K; Neto, Antonio Castro H Fibrillation of Pristine 2D Materials by 2D-Confined Electrolytes ADVANCED FUNCTIONAL MATERIALS, 2024, DOI: 10.1002/adfm.202315038. Abstract | BibTeX | Endnote @article{ISI:001186210500001,
title = {Fibrillation of Pristine 2D Materials by 2D-Confined Electrolytes},
author = {Hui Li Tan and Katarzyna Z Donato and Mariana C F Costa and Alexandra Carvalho and Maxim Trushin and Pei Rou Ng and Xin Hui Yau and Gavin K W Koon and Jakub Tolasz and Zuzana Nemeckova and Petra Ecorchard and Ricardo K Donato and Antonio Castro H Neto},
doi = {10.1002/adfm.202315038},
times_cited = {0},
issn = {1616-301X},
year = {2024},
date = {2024-03-18},
journal = {ADVANCED FUNCTIONAL MATERIALS},
publisher = {WILEY-V C H VERLAG GMBH},
address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY},
abstract = {2D materials are solid microscopic flakes with a-few-Angstrom thickness possessing some of the largest surface-to-volume ratios known. Altering their conformation state from a flat flake to a scroll or fiber offers a synergistic association of properties arising from 2D and 1D nanomaterials. However, a combination of the long-range electrostatic and short-range solvation forces produces an interlayer repulsion that has to be overcome, making scrolling 2D materials without disrupting the pristine structure a challenging task. Herein, a facile method is presented to alter the 2D materials' inter-layer interactions by confining organic salts onto their basal area, forming 2D-confined electrolytes. The confined electrolytes produce local charge inhomogeneities, which can conjugate across the interlayer gap, binding the two surfaces. This allows the 2D-confined electrolytes to behave as polyelectrolytes within a higher dimensional order (2D -> 1D) and form robust nanofibers with distinct electronic properties. The method is not material-specific and the resulting fibers are tightly bound even though the crystal structure of the basal plane remains unaltered.},
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2D materials are solid microscopic flakes with a-few-Angstrom thickness possessing some of the largest surface-to-volume ratios known. Altering their conformation state from a flat flake to a scroll or fiber offers a synergistic association of properties arising from 2D and 1D nanomaterials. However, a combination of the long-range electrostatic and short-range solvation forces produces an interlayer repulsion that has to be overcome, making scrolling 2D materials without disrupting the pristine structure a challenging task. Herein, a facile method is presented to alter the 2D materials' inter-layer interactions by confining organic salts onto their basal area, forming 2D-confined electrolytes. The confined electrolytes produce local charge inhomogeneities, which can conjugate across the interlayer gap, binding the two surfaces. This allows the 2D-confined electrolytes to behave as polyelectrolytes within a higher dimensional order (2D -> 1D) and form robust nanofibers with distinct electronic properties. The method is not material-specific and the resulting fibers are tightly bound even though the crystal structure of the basal plane remains unaltered. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUTan, HL
Donato, KZ
Costa, MCF
Carvalho, A
Trushin, M
Ng, PR
Yau, XH
Koon, GKW
Tolasz, J
Nemecková, Z
Ecorchard, P
Donato, RK
Neto, AHC
- AFHui Li Tan
Katarzyna Z Donato
Mariana C F Costa
Alexandra Carvalho
Maxim Trushin
Pei Rou Ng
Xin Hui Yau
Gavin K W Koon
Jakub Tolasz
Zuzana Nemeckova
Petra Ecorchard
Ricardo K Donato
Antonio Castro H Neto
- TIFibrillation of Pristine 2D Materials by 2D-Confined Electrolytes
- SOADVANCED FUNCTIONAL MATERIALS
- LAEnglish
- DTArticle
- DEBoron Nitride; Fiber; Graphene; MoS2; Scrolling; Self-assembly
- IDIONIC LIQUIDS; GRAPHENE OXIDE; NANOSCROLLS
- AB2D materials are solid microscopic flakes with a-few-Angstrom thickness possessing some of the largest surface-to-volume ratios known. Altering their conformation state from a flat flake to a scroll or fiber offers a synergistic association of properties arising from 2D and 1D nanomaterials. However, a combination of the long-range electrostatic and short-range solvation forces produces an interlayer repulsion that has to be overcome, making scrolling 2D materials without disrupting the pristine structure a challenging task. Herein, a facile method is presented to alter the 2D materials' inter-layer interactions by confining organic salts onto their basal area, forming 2D-confined electrolytes. The confined electrolytes produce local charge inhomogeneities, which can conjugate across the interlayer gap, binding the two surfaces. This allows the 2D-confined electrolytes to behave as polyelectrolytes within a higher dimensional order (2D -> 1D) and form robust nanofibers with distinct electronic properties. The method is not material-specific and the resulting fibers are tightly bound even though the crystal structure of the basal plane remains unaltered.
- C1[Tan, Hui Li; Donato, Katarzyna Z.; Costa, Mariana C. F.; Carvalho, Alexandra; Trushin, Maxim; Ng, Pei Rou; Yau, Xin Hui; Koon, Gavin K. W.; Donato, Ricardo K.; Neto, Antonio H. Castro] Natl Univ Singapore, Ctr Adv Mat 2D, Singapore 117546, Singapore.
[Costa, Mariana C. F.; Trushin, Maxim; Neto, Antonio H. Castro] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore.
[Costa, Mariana C. F.; Carvalho, Alexandra; Trushin, Maxim; Ng, Pei Rou; Neto, Antonio H. Castro] Natl Univ Singapore, Inst Funct Intelligent Mat I FIM, Singapore 117544, Singapore.
[Tolasz, Jakub; Nemeckova, Zuzana; Ecorchard, Petra] Czech Acad Sci, Inst Inorgan Chem, Husinec Rez 1001, Rez 25068, Czech Republic - C3National University of Singapore; National University of Singapore; National University of Singapore; Czech Academy of Sciences; Institute of Inorganic Chemistry of the Czech Academy of Sciences
- RPDonato, RK (corresponding author), Natl Univ Singapore, Ctr Adv Mat 2D, Singapore 117546, Singapore; Neto, AHC (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore; Neto, AHC (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat I FIM, Singapore 117544, Singapore; Ecorchard, P (corresponding author), Czech Acad Sci, Inst Inorgan Chem, Husinec Rez 1001, Rez 25068, Czech Republic
- FUNational Research Foundation [CA2DM]; National Research Foundation, Prime Minister's Office, Singapore [EDUNC-33-18-279-V12]; Singapore Ministry of Education [22-05244S]; National University of Singapore [LM2023066]; National Supercomputing Centre, Singapore; Czech Science Foundation; Ministry of Education, Youth and Sports of the Czech Republic
- FXThis research, including the computational calculations, was carried out at the Centre for Advanced 2D Materials (CA2DM), funded by the National Research Foundation, Prime Minister's Office, Singapore, under its Medium-Sized Centre Programme, and by the Singapore Ministry of Education under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials, National University of Singapore (I-FIM, project No. EDUNC-33-18-279-V12). The National Supercomputing Centre, Singapore (NSCC) is acknowledged for providing computational resources. P.E. and J.T. acknowledge the support of the Czech Science Foundation (grant number 22-05244S) and also the assistance provided by the Research Infrastructure NanoEnviCz, supported by the Ministry of Education, Youth and Sports of the Czech Republic under Project No. LM2023066.
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Quek, Glenn; Ohayon, David; Ng, Pei Rou; Bazan, Guillermo C A Cross-linked n-Type Conjugated Polymer with Polar Side Chains Enables Ultrafast Pseudocapacitive Energy Storage SMALL, 2024, DOI: 10.1002/smll.202401395. Abstract | BibTeX | Endnote @article{ISI:001186407400001,
title = {A Cross-linked n-Type Conjugated Polymer with Polar Side Chains Enables Ultrafast Pseudocapacitive Energy Storage},
author = {Glenn Quek and David Ohayon and Pei Rou Ng and Guillermo C Bazan},
doi = {10.1002/smll.202401395},
times_cited = {0},
issn = {1613-6810},
year = {2024},
date = {2024-03-18},
journal = {SMALL},
publisher = {WILEY-V C H VERLAG GMBH},
address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY},
abstract = {Pseudocapacitors bridge the performance gap between batteries and electric double-layer capacitors by storing energy via a combination of fast surface/near-surface Faradaic redox processes and electrical double-layer capacitance. Organic semiconductors are an emerging class of pseudocapacitive materials that benefit from facile synthetic tunability and mixed ionic-electronic conduction. Reported examples are mostly limited to p-type (electron-donating) conjugated polymers, while n-type (electron-accepting) examples remain comparatively underexplored. This work introduces a new cross-linked n-type conjugated polymer, spiro-NDI-N, strategically designed with polar tertiary amine side chains. This molecular design aims to synergistically increase the electroactive surface area and boost ion transport for efficient ionic-electronic coupling. Spiro-NDI-N demonstrates excellent pseudocapacitive energy storage performance in pH-neutral aqueous electrolytes, with specific capacitance values of up to 532 F g-1 at 5 A g-1 and stable cycling over 5000 cycles. Moreover, it maintains a rate capability of 307 F g-1 at 350 A g-1. The superior pseudocapacitive performance of spiro-NDI-N, compared to strategically designed structural analogues lacking either the cross-linked backbone or polar side chains, validates the essential role of its molecular design elements. More broadly, the design and performance of spiro-NDI-N provide a novel strategy for developing high-performance organic pseudocapacitors.},
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Pseudocapacitors bridge the performance gap between batteries and electric double-layer capacitors by storing energy via a combination of fast surface/near-surface Faradaic redox processes and electrical double-layer capacitance. Organic semiconductors are an emerging class of pseudocapacitive materials that benefit from facile synthetic tunability and mixed ionic-electronic conduction. Reported examples are mostly limited to p-type (electron-donating) conjugated polymers, while n-type (electron-accepting) examples remain comparatively underexplored. This work introduces a new cross-linked n-type conjugated polymer, spiro-NDI-N, strategically designed with polar tertiary amine side chains. This molecular design aims to synergistically increase the electroactive surface area and boost ion transport for efficient ionic-electronic coupling. Spiro-NDI-N demonstrates excellent pseudocapacitive energy storage performance in pH-neutral aqueous electrolytes, with specific capacitance values of up to 532 F g-1 at 5 A g-1 and stable cycling over 5000 cycles. Moreover, it maintains a rate capability of 307 F g-1 at 350 A g-1. The superior pseudocapacitive performance of spiro-NDI-N, compared to strategically designed structural analogues lacking either the cross-linked backbone or polar side chains, validates the essential role of its molecular design elements. More broadly, the design and performance of spiro-NDI-N provide a novel strategy for developing high-performance organic pseudocapacitors. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUQuek, G
Ohayon, D
Ng, PR
Bazan, GC
- AFGlenn Quek
David Ohayon
Pei Rou Ng
Guillermo C Bazan
- TIA Cross-linked n-Type Conjugated Polymer with Polar Side Chains Enables Ultrafast Pseudocapacitive Energy Storage
- SOSMALL
- LAEnglish
- DTArticle
- DEElectrochemical Energy Storage; High-rate Capability; N-type Conjugated Polymers; Organic Semiconductors; Pseudocapacitors
- IDMICROPOROUS POLYMERS
- ABPseudocapacitors bridge the performance gap between batteries and electric double-layer capacitors by storing energy via a combination of fast surface/near-surface Faradaic redox processes and electrical double-layer capacitance. Organic semiconductors are an emerging class of pseudocapacitive materials that benefit from facile synthetic tunability and mixed ionic-electronic conduction. Reported examples are mostly limited to p-type (electron-donating) conjugated polymers, while n-type (electron-accepting) examples remain comparatively underexplored. This work introduces a new cross-linked n-type conjugated polymer, spiro-NDI-N, strategically designed with polar tertiary amine side chains. This molecular design aims to synergistically increase the electroactive surface area and boost ion transport for efficient ionic-electronic coupling. Spiro-NDI-N demonstrates excellent pseudocapacitive energy storage performance in pH-neutral aqueous electrolytes, with specific capacitance values of up to 532 F g-1 at 5 A g-1 and stable cycling over 5000 cycles. Moreover, it maintains a rate capability of 307 F g-1 at 350 A g-1. The superior pseudocapacitive performance of spiro-NDI-N, compared to strategically designed structural analogues lacking either the cross-linked backbone or polar side chains, validates the essential role of its molecular design elements. More broadly, the design and performance of spiro-NDI-N provide a novel strategy for developing high-performance organic pseudocapacitors.
- C3National University of Singapore; National University of Singapore; National University of Singapore; National University of Singapore
- RPBazan, GC (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat I FIM, Singapore 117544, Singapore; Bazan, GC (corresponding author), Natl Univ Singapore, Dept Chem & Chem, Singapore 119077, Singapore
- FXG.Q. and G.C.B. conceived the idea, designed the experiments, and wrote the manuscript. G.Q. set up experiments, collected and analyzed data, and synthesized and characterized the polymers. D.O. assisted with XPS and spectroelectrochemical measurements. P.R.N. assisted with SEM imaging. All authors discussed the results and revised the manuscript. This work was supported by the National University of Singapore start-up grant R143-000-A97-133, the Research Centre of Excellence award to the Institute for Functional Intelligent Materials from the Singapore Ministry of Education (I-FIM, project No. EDUNC-33-18-279-V12), and the Office of Naval Research (ONR-Global, N62909-22-1-2016). G.Q. acknowledges funding from the President's Graduate Fellowship (PGF) under the National University of Singapore.
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- JISmall
- PDMAR 18
- PY2024
- DI10.1002/smll.202401395
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- WCChemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter
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Voronin, Kirill V; Toksumakov, Adilet N; Ermolaev, Georgy A; Slavich, Aleksandr S; Tatmyshevskiy, Mikhail K; Novikov, Sergey M; Vyshnevyy, Andrey A; Arsenin, Aleksey V; Novoselov, Kostya S; Ghazaryan, Davit A; Volkov, Valentyn S; Baranov, Denis G Chiral Photonic Super-Crystals Based on Helical van der Waals Homostructures LASER & PHOTONICS REVIEWS, 2024, DOI: 10.1002/lpor.202301113. Abstract | BibTeX | Endnote @article{ISI:001184877700001,
title = {Chiral Photonic Super-Crystals Based on Helical van der Waals Homostructures},
author = {Kirill V Voronin and Adilet N Toksumakov and Georgy A Ermolaev and Aleksandr S Slavich and Mikhail K Tatmyshevskiy and Sergey M Novikov and Andrey A Vyshnevyy and Aleksey V Arsenin and Kostya S Novoselov and Davit A Ghazaryan and Valentyn S Volkov and Denis G Baranov},
doi = {10.1002/lpor.202301113},
times_cited = {0},
issn = {1863-8880},
year = {2024},
date = {2024-03-14},
journal = {LASER & PHOTONICS REVIEWS},
publisher = {WILEY-V C H VERLAG GMBH},
address = {POSTFACH 101161, 69451 WEINHEIM, GERMANY},
abstract = {Chirality is one of the most mysterious symmetry transformations. Very readily broken in biological systems, it is practically absent in naturally occurring inorganic materials and is very challenging to create artificially. Chiral optical wavefronts are often used for the identification, control, and discrimination of left- and right-handed biological and other molecules. Thus, it is crucially important to create materials capable of chiral interaction with light, which would allow one to assign arbitrary chiral properties to a light field. This study utilizes van der Waals technology to assemble helical homostructures with chiral properties (e.g., circular dichroism). Because of the large range of van der Waals materials available, such helical homostructures can be assigned with very flexible optical properties. The approach is demonstrated by creating helical homostructures based on multilayer As2S3${rm As}_2{rm S}_3$ (arsenic trisulfide), which offers the most pronounced chiral properties even in thin structures due to its strong biaxial optically anisotropy. The work showcases that the chirality of an electromagnetic system may emerge at an intermediate level between the molecular and the mesoscopic one due to the tailored arrangement of non-chiral layers of van der Waals crystals and without additional patterning.},
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Chirality is one of the most mysterious symmetry transformations. Very readily broken in biological systems, it is practically absent in naturally occurring inorganic materials and is very challenging to create artificially. Chiral optical wavefronts are often used for the identification, control, and discrimination of left- and right-handed biological and other molecules. Thus, it is crucially important to create materials capable of chiral interaction with light, which would allow one to assign arbitrary chiral properties to a light field. This study utilizes van der Waals technology to assemble helical homostructures with chiral properties (e.g., circular dichroism). Because of the large range of van der Waals materials available, such helical homostructures can be assigned with very flexible optical properties. The approach is demonstrated by creating helical homostructures based on multilayer As2S3${rm As}_2{rm S}_3$ (arsenic trisulfide), which offers the most pronounced chiral properties even in thin structures due to its strong biaxial optically anisotropy. The work showcases that the chirality of an electromagnetic system may emerge at an intermediate level between the molecular and the mesoscopic one due to the tailored arrangement of non-chiral layers of van der Waals crystals and without additional patterning. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUVoronin, KV
Toksumakov, AN
Ermolaev, GA
Slavich, AS
Tatmyshevskiy, MK
Novikov, SM
Vyshnevyy, AA
Arsenin, AV
Novoselov, KS
Ghazaryan, DA
Volkov, VS
Baranov, DG
- AFKirill V Voronin
Adilet N Toksumakov
Georgy A Ermolaev
Aleksandr S Slavich
Mikhail K Tatmyshevskiy
Sergey M Novikov
Andrey A Vyshnevyy
Aleksey V Arsenin
Kostya S Novoselov
Davit A Ghazaryan
Valentyn S Volkov
Denis G Baranov
- TIChiral Photonic Super-Crystals Based on Helical van der Waals Homostructures
- SOLASER & PHOTONICS REVIEWS
- LAEnglish
- DTArticle
- DEChirality; Nanophotonics; Optical Anisotropy; Twistronics; Van Der Waals Crystals
- IDPOLARITONS; EXCITONS; STATES
- ABChirality is one of the most mysterious symmetry transformations. Very readily broken in biological systems, it is practically absent in naturally occurring inorganic materials and is very challenging to create artificially. Chiral optical wavefronts are often used for the identification, control, and discrimination of left- and right-handed biological and other molecules. Thus, it is crucially important to create materials capable of chiral interaction with light, which would allow one to assign arbitrary chiral properties to a light field. This study utilizes van der Waals technology to assemble helical homostructures with chiral properties (e.g., circular dichroism). Because of the large range of van der Waals materials available, such helical homostructures can be assigned with very flexible optical properties. The approach is demonstrated by creating helical homostructures based on multilayer As2S3${rm As}_2{rm S}_3$ (arsenic trisulfide), which offers the most pronounced chiral properties even in thin structures due to its strong biaxial optically anisotropy. The work showcases that the chirality of an electromagnetic system may emerge at an intermediate level between the molecular and the mesoscopic one due to the tailored arrangement of non-chiral layers of van der Waals crystals and without additional patterning.
- C3Russian Academy of Sciences; Emanuel Institute of Biochemical Physics; Yerevan State University; University of Manchester; National University of Singapore
- RPGhazaryan, DA (corresponding author), Moscow Ctr Adv Studies, Moscow 123592, Russia; Ghazaryan, DA (corresponding author), Yerevan State Univ, Lab Adv Funct Mat, Yerevan 0025, Armenia
- FXThe work was supported by the Russian Science Foundation (project No. 23-72-10005) and by the Ministry of Science and Higher Education of the Russian Federation (FSMG-2024-0014 and 075-15-2021-606). K.S.N. acknowledges support from the Ministry of Education, Singapore (Research Centre of Excellence award to the Institute for Functional Intelligent Materials, I-FIM, project No. EDUNC-33-18-279-V12) and from the Royal Society (UK, grant number RSRPR190000). D.G.B. acknowledges financial support from BASIS Foundation (grant 22-1-3-2-1).
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Scott, James M; Dale, Stephen G; Mcbroom, James; Gould, Tim; Li, Qin Size Isn't Everything: Geometric Tuning in Polycyclic Aromatic Hydrocarbons and Its Implications for Carbon Nanodots JOURNAL OF PHYSICAL CHEMISTRY A, 128 (11), pp. 2003-2014, 2024, DOI: 10.1021/acs.jpca.3c07416. Abstract | BibTeX | Endnote @article{ISI:001183881800001,
title = {Size Isn't Everything: Geometric Tuning in Polycyclic Aromatic Hydrocarbons and Its Implications for Carbon Nanodots},
author = {James M Scott and Stephen G Dale and James Mcbroom and Tim Gould and Qin Li},
doi = {10.1021/acs.jpca.3c07416},
times_cited = {0},
issn = {1089-5639},
year = {2024},
date = {2024-03-12},
journal = {JOURNAL OF PHYSICAL CHEMISTRY A},
volume = {128},
number = {11},
pages = {2003-2014},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Recent developments in light-emitting carbon nanodots and molecular organic semiconductors have seen renewed interest in the properties of polycyclic aromatic hydrocarbons (PAHs) as a family. The networks of delocalized pi electrons in sp2-hybridized carbon grant PAHs light-emissive properties right across the visible spectrum. However, the mechanistic understanding of their emission energy has been limited due to the ground state-focused methods of determination. This computational chemistry work, therefore, seeks to validate existing rules and elucidate new features and characteristics of PAHs that influence their emissions. Predictions based on (time-dependent) density functional theory account for the full 3-dimensional electronic structure of ground and excited states and reveal that twisting and near-degeneracies strongly influence emission spectra and may therefore be used to tune the color of PAHs and, hence, carbon nanodots. We particularly note that the influence of twisting goes beyond torsional destabilization of the ground-state and geometric relaxation of the excited state, with a third contribution associated with the electric transition dipole. Symmetries and peri-condensation may also have an effect, but this could not be statistically confirmed. In pursuing this goal, we demonstrate that with minimal changes to molecular size, the entire visible spectrum may be spanned by geometric modification alone; we have also provided a first estimate of emission energy for 35 molecules currently lacking published emission spectra as well as clear guidelines for when more sophisticated computational techniques are required to predict the properties of PAHs accurately.},
keywords = {},
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Recent developments in light-emitting carbon nanodots and molecular organic semiconductors have seen renewed interest in the properties of polycyclic aromatic hydrocarbons (PAHs) as a family. The networks of delocalized pi electrons in sp2-hybridized carbon grant PAHs light-emissive properties right across the visible spectrum. However, the mechanistic understanding of their emission energy has been limited due to the ground state-focused methods of determination. This computational chemistry work, therefore, seeks to validate existing rules and elucidate new features and characteristics of PAHs that influence their emissions. Predictions based on (time-dependent) density functional theory account for the full 3-dimensional electronic structure of ground and excited states and reveal that twisting and near-degeneracies strongly influence emission spectra and may therefore be used to tune the color of PAHs and, hence, carbon nanodots. We particularly note that the influence of twisting goes beyond torsional destabilization of the ground-state and geometric relaxation of the excited state, with a third contribution associated with the electric transition dipole. Symmetries and peri-condensation may also have an effect, but this could not be statistically confirmed. In pursuing this goal, we demonstrate that with minimal changes to molecular size, the entire visible spectrum may be spanned by geometric modification alone; we have also provided a first estimate of emission energy for 35 molecules currently lacking published emission spectra as well as clear guidelines for when more sophisticated computational techniques are required to predict the properties of PAHs accurately. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUScott, JM
Dale, SG
Mcbroom, J
Gould, T
Li, Q
- AFJames M Scott
Stephen G Dale
James Mcbroom
Tim Gould
Qin Li
- TISize Isn't Everything: Geometric Tuning in Polycyclic Aromatic Hydrocarbons and Its Implications for Carbon Nanodots
- SOJOURNAL OF PHYSICAL CHEMISTRY A
- LAEnglish
- DTArticle
- IDDENSITY-FUNCTIONAL THEORY; STRUCTURE-PROPERTY RELATIONSHIPS; EXCITATION-ENERGIES; ELECTRONIC-PROPERTIES; ANNELLATION THEORY; PREDICTIVE POWER; SINGLET FISSION; FLUORESCENCE; DOTS; EMISSION
- ABRecent developments in light-emitting carbon nanodots and molecular organic semiconductors have seen renewed interest in the properties of polycyclic aromatic hydrocarbons (PAHs) as a family. The networks of delocalized pi electrons in sp2-hybridized carbon grant PAHs light-emissive properties right across the visible spectrum. However, the mechanistic understanding of their emission energy has been limited due to the ground state-focused methods of determination. This computational chemistry work, therefore, seeks to validate existing rules and elucidate new features and characteristics of PAHs that influence their emissions. Predictions based on (time-dependent) density functional theory account for the full 3-dimensional electronic structure of ground and excited states and reveal that twisting and near-degeneracies strongly influence emission spectra and may therefore be used to tune the color of PAHs and, hence, carbon nanodots. We particularly note that the influence of twisting goes beyond torsional destabilization of the ground-state and geometric relaxation of the excited state, with a third contribution associated with the electric transition dipole. Symmetries and peri-condensation may also have an effect, but this could not be statistically confirmed. In pursuing this goal, we demonstrate that with minimal changes to molecular size, the entire visible spectrum may be spanned by geometric modification alone; we have also provided a first estimate of emission energy for 35 molecules currently lacking published emission spectra as well as clear guidelines for when more sophisticated computational techniques are required to predict the properties of PAHs accurately.
- C1[Scott, James M.; Dale, Stephen G.; Gould, Tim; Li, Qin] Griffith Univ, Queensland Micro & Nanotechnol Ctr, Nathan, Qld 4111, Australia.
[Scott, James M.; Li, Qin] Griffith Univ, Sch Engn & Built Environm, Nathan, Qld 4111, Australia.
[Mcbroom, James; Gould, Tim] Griffith Univ, Sch Environm & Sci, Nathan, Qld 4111, Australia.
[Dale, Stephen G.] Natl Univ Singapore, Inst Funct Intelligent Mat I FIM, Singapore 117544, Singapore - C3Griffith University; Griffith University; Griffith University; National University of Singapore
- RPScott, JM (corresponding author), Griffith Univ, Queensland Micro & Nanotechnol Ctr, Nathan, Qld 4111, Australia; Scott, JM (corresponding author), Griffith Univ, Sch Engn & Built Environm, Nathan, Qld 4111, Australia; Gould, T (corresponding author), Griffith Univ, Sch Environm & Sci, Nathan, Qld 4111, Australia
- FUAustralian Research Council [DP200100033, DP200101105, DP230100479, FT210100663]; Australia Research Council Discovery Projects
- FXThe authors gratefully acknowledge the financial support from the Australia Research Council Discovery Projects (DP200100033, DP200101105, DP230100479) and Future Fellowship (FT210100663) of Australia.
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Slavich, Aleksandr S; Ermolaev, Georgy A; Tatmyshevskiy, Mikhail K; Toksumakov, Adilet N; Matveeva, Olga G; Grudinin, Dmitriy V; Voronin, Kirill V; Mazitov, Arslan; Kravtsov, Konstantin V; Syuy, Alexander V; Tsymbarenko, Dmitry M; Mironov, Mikhail S; Novikov, Sergey M; Kruglov, Ivan; Ghazaryan, Davit A; Vyshnevyy, Andrey A; Arsenin, Aleksey V; Volkov, Valentyn S; Novoselov, Kostya S Exploring van der Waals materials with high anisotropy: geometrical and optical approaches LIGHT-SCIENCE & APPLICATIONS, 13 (1), 2024, DOI: 10.1038/s41377-024-01407-3. Abstract | BibTeX | Endnote @article{ISI:001180455600003,
title = {Exploring van der Waals materials with high anisotropy: geometrical and optical approaches},
author = {Aleksandr S Slavich and Georgy A Ermolaev and Mikhail K Tatmyshevskiy and Adilet N Toksumakov and Olga G Matveeva and Dmitriy V Grudinin and Kirill V Voronin and Arslan Mazitov and Konstantin V Kravtsov and Alexander V Syuy and Dmitry M Tsymbarenko and Mikhail S Mironov and Sergey M Novikov and Ivan Kruglov and Davit A Ghazaryan and Andrey A Vyshnevyy and Aleksey V Arsenin and Valentyn S Volkov and Kostya S Novoselov},
doi = {10.1038/s41377-024-01407-3},
times_cited = {1},
issn = {2095-5545},
year = {2024},
date = {2024-03-08},
journal = {LIGHT-SCIENCE & APPLICATIONS},
volume = {13},
number = {1},
publisher = {SPRINGERNATURE},
address = {CAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND},
abstract = {The emergence of van der Waals (vdW) materials resulted in the discovery of their high optical, mechanical, and electronic anisotropic properties, immediately enabling countless novel phenomena and applications. Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials. Furthermore, the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches. Here, we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization. Using our approach, we found As2S3 as a highly anisotropic vdW material. It demonstrates high in-plane optical anisotropy that is similar to 20% larger than for rutile and over two times as large as calcite, high refractive index, and transparency in the visible range, overcoming the century-long record set by rutile. Given these benefits, As2S3 opens a pathway towards next-generation nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry-Perot optical phase accumulations. Hence, our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties.},
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The emergence of van der Waals (vdW) materials resulted in the discovery of their high optical, mechanical, and electronic anisotropic properties, immediately enabling countless novel phenomena and applications. Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials. Furthermore, the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches. Here, we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization. Using our approach, we found As2S3 as a highly anisotropic vdW material. It demonstrates high in-plane optical anisotropy that is similar to 20% larger than for rutile and over two times as large as calcite, high refractive index, and transparency in the visible range, overcoming the century-long record set by rutile. Given these benefits, As2S3 opens a pathway towards next-generation nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry-Perot optical phase accumulations. Hence, our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUSlavich, AS
Ermolaev, GA
Tatmyshevskiy, MK
Toksumakov, AN
Matveeva, OG
Grudinin, DV
Voronin, KV
Mazitov, A
Kravtsov, KV
Syuy, AV
Tsymbarenko, DM
Mironov, MS
Novikov, SM
Kruglov, I
Ghazaryan, DA
Vyshnevyy, AA
Arsenin, AV
Volkov, VS
Novoselov, KS
- AFAleksandr S Slavich
Georgy A Ermolaev
Mikhail K Tatmyshevskiy
Adilet N Toksumakov
Olga G Matveeva
Dmitriy V Grudinin
Kirill V Voronin
Arslan Mazitov
Konstantin V Kravtsov
Alexander V Syuy
Dmitry M Tsymbarenko
Mikhail S Mironov
Sergey M Novikov
Ivan Kruglov
Davit A Ghazaryan
Andrey A Vyshnevyy
Aleksey V Arsenin
Valentyn S Volkov
Kostya S Novoselov
- TIExploring van der Waals materials with high anisotropy: geometrical and optical approaches
- SOLIGHT-SCIENCE & APPLICATIONS
- LAEnglish
- DTArticle
- ID2-DIMENSIONAL MATERIALS; POLARITONS; CRYSTALS; GIANT; AS2S3
- ABThe emergence of van der Waals (vdW) materials resulted in the discovery of their high optical, mechanical, and electronic anisotropic properties, immediately enabling countless novel phenomena and applications. Such success inspired an intensive search for the highest possible anisotropic properties among vdW materials. Furthermore, the identification of the most promising among the huge family of vdW materials is a challenging quest requiring innovative approaches. Here, we suggest an easy-to-use method for such a survey based on the crystallographic geometrical perspective of vdW materials followed by their optical characterization. Using our approach, we found As2S3 as a highly anisotropic vdW material. It demonstrates high in-plane optical anisotropy that is similar to 20% larger than for rutile and over two times as large as calcite, high refractive index, and transparency in the visible range, overcoming the century-long record set by rutile. Given these benefits, As2S3 opens a pathway towards next-generation nanophotonics as demonstrated by an ultrathin true zero-order quarter-wave plate that combines classical and the Fabry-Perot optical phase accumulations. Hence, our approach provides an effective and easy-to-use method to find vdW materials with the utmost anisotropic properties.
- C1[Slavich, Aleksandr S.; Tatmyshevskiy, Mikhail K.; Toksumakov, Adilet N.; Matveeva, Olga G.; Kravtsov, Konstantin V.; Novikov, Sergey M.; Ghazaryan, Davit A.] Moscow Ctr Adv Studies, Kulakova Str 20, Moscow 123592, Russia.
[Ermolaev, Georgy A.; Grudinin, Dmitriy V.; Syuy, Alexander V.; Mironov, Mikhail S.; Kruglov, Ivan; Vyshnevyy, Andrey A.; Arsenin, Aleksey V.; Volkov, Valentyn S.] XPANCEO, Emerging Technol Res Ctr, Emmay Tower, Dubai, U Arab Emirates.
[Voronin, Kirill V.] Donostia Int Phys Ctr DIPC, San Sebastian 20018, Spain.
[Mazitov, Arslan] Ecole Polytech Fed Lausanne, Inst Mat, CH-1015 Lausanne, Switzerland.
[Tsymbarenko, Dmitry M.] Lomonosov Moscow State Univ, Dept Chem, Moscow 119991, Russia.
[Ghazaryan, Davit A.; Arsenin, Aleksey V.; Volkov, Valentyn S.] Yerevan State Univ, Lab Adv Funct Mat, Yerevan 0025, Armenia.
[Novoselov, Kostya S.] Univ Manchester, Natl Graphene Inst NGI, Manchester M13 9PL, Lancs, England.
[Novoselov, Kostya S.] Natl Univ Singapore, Dept Mat Sci & Engn, 03-09 EA, Singapore 117579, Singapore.
[Novoselov, Kostya S.] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore - C3Swiss Federal Institutes of Technology Domain; Ecole Polytechnique Federale de Lausanne; Lomonosov Moscow State University; Yerevan State University; University of Manchester; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore
- RPNovoselov, KS (corresponding author), Univ Manchester, Natl Graphene Inst NGI, Manchester M13 9PL, Lancs, England; Novoselov, KS (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, 03-09 EA, Singapore 117579, Singapore; Novoselov, KS (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore
- FUMinistry of Education, Singapore (Research Centre of Excellence award) [EDUNC-33-18-279-V12]; Royal Society (UK) [RSRPR190000]; Ministry of Science and Higher Education [075-15-2022-1150]; RSF [22-19-00558]; Higher Education and Science Committee of the Ministry of Education, Science, Culture, and Sport of the Republic of Armenia Project [23RL-2A031]; M.V. Lomonosov Moscow State University Program of Development
- FXK.S.N. acknowledges support from the Ministry of Education, Singapore (Research Centre of Excellence award to the Institute for Functional Intelligent Materials, I-FIM, project No. EDUNC-33-18-279-V12) and from the Royal Society (UK, grant number RSRPR190000). S.M.N. acknowledges the financial support from the Ministry of Science and Higher Education (agreement No. 075-15-2022-1150). A.S.S. and A.N.T. gratefully acknowledge the financial support from the RSF (grant No. 22-19-00558). D.A.G., A.V.A., and V.S.V. acknowledge support from the Higher Education and Science Committee of the Ministry of Education, Science, Culture, and Sport of the Republic of Armenia Project No. 23RL-2A031. D.M.T. acknowledges support from the M.V. Lomonosov Moscow State University Program of Development.
- NR67
- TC1
- Z91
- U18
- U28
- PUSPRINGERNATURE
- PILONDON
- PACAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND
- SN2095-5545
- J9LIGHT-SCI APPL
- JILight-Sci. Appl.
- PDMAR 8
- PY2024
- VL13
- DI10.1038/s41377-024-01407-3
- PG9
- WCOptics
- SCOptics
- UTWOS:001180455600003
- ER
- EF
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