2024
|
Wu, Ao; Badrtdinov, Danis I; Lee, Woncheol; Rosner, Malte; Dreyer, Cyrus E; Koperski, Maciej Ab initio methods applied to carbon-containing defects in hexagonal boron nitride MATERIALS TODAY SUSTAINABILITY, 28 , 2024, DOI: 10.1016/j.mtsust.2024.100988. Abstract | BibTeX | Endnote @article{ISI:001334063800001,
title = {Ab initio methods applied to carbon-containing defects in hexagonal boron nitride},
author = {Ao Wu and Danis I Badrtdinov and Woncheol Lee and Malte Rosner and Cyrus E Dreyer and Maciej Koperski},
doi = {10.1016/j.mtsust.2024.100988},
times_cited = {0},
issn = {2589-2347},
year = {2024},
date = {2024-12-01},
journal = {MATERIALS TODAY SUSTAINABILITY},
volume = {28},
publisher = {ELSEVIER},
address = {RADARWEG 29, 1043 NX AMSTERDAM, NETHERLANDS},
abstract = {The functionalities activated by defect centers in solids are constantly growing, opening new avenues for sustainable future technologies. These may extend to quantum optoelectronics if suitable defect centers are created and their properties understood. Recent progress in developing quantum emitters in hexagonal boron nitride (hBN) associated with carbon impurities enabled the realization of such concepts in atomically thin films, where the defect centers exhibit an unprecedented level of sensitivity toward the environment. The complexity of defects, together with new control knobs provided by van der Waals technology, poses a challenge for theory to accurately predict the properties of defect centers and to match them with experimental results. Here, we review the ab initio methods applied to carbon-containing defect centers in hBN, exploring the predictive capabilities of different levels of theory for their structural and optoelectronic properties.},
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pubstate = {published},
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The functionalities activated by defect centers in solids are constantly growing, opening new avenues for sustainable future technologies. These may extend to quantum optoelectronics if suitable defect centers are created and their properties understood. Recent progress in developing quantum emitters in hexagonal boron nitride (hBN) associated with carbon impurities enabled the realization of such concepts in atomically thin films, where the defect centers exhibit an unprecedented level of sensitivity toward the environment. The complexity of defects, together with new control knobs provided by van der Waals technology, poses a challenge for theory to accurately predict the properties of defect centers and to match them with experimental results. Here, we review the ab initio methods applied to carbon-containing defect centers in hBN, exploring the predictive capabilities of different levels of theory for their structural and optoelectronic properties. - FNClarivate Analytics Web of Science
- VR1.0
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- AUWu, A
Badrtdinov, DI
Lee, WC
Rösner, M
Dreyer, CE
Koperski, M
- AFAo Wu
Danis I Badrtdinov
Woncheol Lee
Malte Rosner
Cyrus E Dreyer
Maciej Koperski
- TIAb initio methods applied to carbon-containing defects in hexagonal boron nitride
- SOMATERIALS TODAY SUSTAINABILITY
- LAEnglish
- DTArticle
- DEQuantum Defects; Ab Initio Methods; Density Functional Theory; Quantum Embedding; Structural And Electronic Properties
- IDELECTRONIC-STRUCTURE CALCULATIONS; STRONGLY CORRELATED STATES; DENSITY-FUNCTIONAL-THEORY; SINGLE-PHOTON EMITTERS; GREENS-FUNCTION; EMBEDDING METHODS; QUANTUM EMITTERS; POINT-DEFECTS; ENERGY; FIELD
- ABThe functionalities activated by defect centers in solids are constantly growing, opening new avenues for sustainable future technologies. These may extend to quantum optoelectronics if suitable defect centers are created and their properties understood. Recent progress in developing quantum emitters in hexagonal boron nitride (hBN) associated with carbon impurities enabled the realization of such concepts in atomically thin films, where the defect centers exhibit an unprecedented level of sensitivity toward the environment. The complexity of defects, together with new control knobs provided by van der Waals technology, poses a challenge for theory to accurately predict the properties of defect centers and to match them with experimental results. Here, we review the ab initio methods applied to carbon-containing defect centers in hBN, exploring the predictive capabilities of different levels of theory for their structural and optoelectronic properties.
- C1[Wu, Ao; Koperski, Maciej] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore.
[Wu, Ao; Koperski, Maciej] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore.
[Badrtdinov, Danis I.; Rosner, Malte] Radboud Univ Nijmegen, Inst Mol & Mat, Heijendaalseweg 135, NL-6525 AJ Nijmegen, Netherlands.
[Lee, Woncheol] Univ Calif Santa Barbara, Mat Dept, Santa Barbara, CA 93106 USA.
[Dreyer, Cyrus E.] Flatiron Inst, Ctr Computat Quantum Phys, 162 5th Ave, New York, NY 10010 USA.
[Dreyer, Cyrus E.] SUNY Stony Brook, Dept Phys & Astron, Stony Brook, NY 11794 USA - C3National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; Radboud University Nijmegen; University of California System; University of California Santa Barbara; State University of New York (SUNY) System; Stony Brook University
- RPKoperski, M (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore
- FUMinistry of Education (Singapore) through the Research Centre of Excellence program [EDUN C-33-18-279-V12]; AcRF Tier 3, Singapore [MOE2018-T3-1-005]; Ministry of Education, Singapore [MOE-T2EP50122-0012]; Air Force Office of Scientific Research [FA8655-21-1-7026]; Office of Naval Research Global, United States [DMR-2237674]; Simons Foundation; National Science Foundation, United States
- FXThis project was supported by the Ministry of Education (Singapore) through the Research Centre of Excellence program (grant EDUN C-33-18-279-V12, I-FIM) , AcRF Tier 3, Singapore (MOE2018-T3-1-005) . This research is supported by the Ministry of Education, Singapore, under its Academic Research Fund Tier 2 (MOE-T2EP50122-0012) . This material is based upon work supported by the Air Force Office of Scientific Research and the Office of Naval Research Global, United States under award number FA8655-21-1-7026. MR thanks the Simons Foundation for hospitality. CED acknowledges support from National Science Foundation, United States Grant No. DMR-2237674. The Flatiron Institute is a division of the Simons Foundation.
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Loh, Leyi; Ho, Yi Wei; Xuan, Fengyuan; del Aguila, Andres Granados; Chen, Yuan; Wong, See Yoong; Zhang, Jingda; Wang, Zhe; Watanabe, Kenji; Taniguchi, Takashi; Pigram, Paul J; Bosman, Michel; Quek, Su Ying; Koperski, Maciej; Eda, Goki Nb impurity-bound excitons as quantum emitters in monolayer WS2 NATURE COMMUNICATIONS, 15 (1), 2024, DOI: 10.1038/s41467-024-54360-5. Abstract | BibTeX | Endnote @article{ISI:001360396900001,
title = {Nb impurity-bound excitons as quantum emitters in monolayer WS_{2}},
author = {Leyi Loh and Yi Wei Ho and Fengyuan Xuan and Andres Granados del Aguila and Yuan Chen and See Yoong Wong and Jingda Zhang and Zhe Wang and Kenji Watanabe and Takashi Taniguchi and Paul J Pigram and Michel Bosman and Su Ying Quek and Maciej Koperski and Goki Eda},
doi = {10.1038/s41467-024-54360-5},
times_cited = {0},
year = {2024},
date = {2024-11-20},
journal = {NATURE COMMUNICATIONS},
volume = {15},
number = {1},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Point defects in crystalline solids behave as optically addressable individual quantum systems when present in sufficiently low concentrations. In two-dimensional (2D) semiconductors, such quantum defects hold potential as versatile single photon sources. Here, we report the synthesis and optical properties of Nb-doped monolayer WS2 in the dilute limit where the average spacing between individual dopants exceeds the optical diffraction limit, allowing the emission spectrum to be studied at the single-dopant level. We show that these individual dopants exhibit common features of quantum emitters, including narrow emission lines (with linewidths <1 meV), strong spatial confinement, and photon antibunching. These emitters consistently occur within a narrow spectral range across multiple samples, distinct from common quantum emitters in van der Waals (vdW) materials that show large ensemble broadening. Analysis of the Zeeman splitting reveals that they can be attributed to bound exciton complexes comprising dark excitons and negatively charged Nb.},
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Point defects in crystalline solids behave as optically addressable individual quantum systems when present in sufficiently low concentrations. In two-dimensional (2D) semiconductors, such quantum defects hold potential as versatile single photon sources. Here, we report the synthesis and optical properties of Nb-doped monolayer WS2 in the dilute limit where the average spacing between individual dopants exceeds the optical diffraction limit, allowing the emission spectrum to be studied at the single-dopant level. We show that these individual dopants exhibit common features of quantum emitters, including narrow emission lines (with linewidths <1 meV), strong spatial confinement, and photon antibunching. These emitters consistently occur within a narrow spectral range across multiple samples, distinct from common quantum emitters in van der Waals (vdW) materials that show large ensemble broadening. Analysis of the Zeeman splitting reveals that they can be attributed to bound exciton complexes comprising dark excitons and negatively charged Nb. - FNClarivate Analytics Web of Science
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- AULoh, L
Ho, YW
Xuan, FY
del Aguila, AG
Chen, Y
Wong, SY
Zhang, JD
Wang, Z
Watanabe, K
Taniguchi, T
Pigram, PJ
Bosman, M
Quek, SY
Koperski, M
Eda, G
- AFLeyi Loh
Yi Wei Ho
Fengyuan Xuan
Andres Granados del Aguila
Yuan Chen
See Yoong Wong
Jingda Zhang
Zhe Wang
Kenji Watanabe
Takashi Taniguchi
Paul J Pigram
Michel Bosman
Su Ying Quek
Maciej Koperski
Goki Eda
- TINb impurity-bound excitons as quantum emitters in monolayer WS2
- SONATURE COMMUNICATIONS
- LAEnglish
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- IDCOLOR-CENTERS; ENERGY
- ABPoint defects in crystalline solids behave as optically addressable individual quantum systems when present in sufficiently low concentrations. In two-dimensional (2D) semiconductors, such quantum defects hold potential as versatile single photon sources. Here, we report the synthesis and optical properties of Nb-doped monolayer WS2 in the dilute limit where the average spacing between individual dopants exceeds the optical diffraction limit, allowing the emission spectrum to be studied at the single-dopant level. We show that these individual dopants exhibit common features of quantum emitters, including narrow emission lines (with linewidths <1 meV), strong spatial confinement, and photon antibunching. These emitters consistently occur within a narrow spectral range across multiple samples, distinct from common quantum emitters in van der Waals (vdW) materials that show large ensemble broadening. Analysis of the Zeeman splitting reveals that they can be attributed to bound exciton complexes comprising dark excitons and negatively charged Nb.
- C1[Loh, Leyi; Ho, Yi Wei; Zhang, Jingda; Quek, Su Ying; Eda, Goki] Natl Univ Singapore, Dept Phys, Singapore, Singapore.
[Loh, Leyi; Bosman, Michel; Quek, Su Ying; Koperski, Maciej] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore, Singapore.
[Ho, Yi Wei; del Aguila, Andres Granados; Koperski, Maciej] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore.
[Xuan, Fengyuan; Quek, Su Ying; Eda, Goki] Natl Univ Singapore, Ctr Adv 2D Mat, Singapore, Singapore.
[Chen, Yuan; Wang, Zhe; Eda, Goki] Natl Univ Singapore, Dept Chem, Singapore, Singapore.
[Wong, See Yoong; Pigram, Paul J.] La Trobe Univ Melbourne, Ctr Mat & Surface Sci, Melbourne, Vic, Australia.
[Wong, See Yoong; Pigram, Paul J.] La Trobe Univ Melbourne, Dept Math & Phys Sci, Melbourne, Vic, Australia.
[Watanabe, Kenji] Natl Inst Mat Sci, Res Ctr Funct Mat, Tsukuba, Japan.
[Taniguchi, Takashi] Natl Inst Mat Sci, Int Ctr Mat Nanoarchitectron, Tsukuba, Japan.
[Quek, Su Ying] Natl Univ Singapore, NUS Grad Sch, Integrat Sci & Engn Programme, Singapore, Singapore.
[Quek, Su Ying] Natl Univ Singapore, NUS Coll, Singapore, Singapore - C3National 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; La Trobe University; La Trobe University; National Institute for Materials Science; National Institute for Materials Science; National University of Singapore; National University of Singapore
- RPQuek, SY (corresponding author), Natl Univ Singapore, Dept Phys, Singapore, Singapore; Quek, SY (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore, Singapore; Koperski, M (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore; Quek, SY (corresponding author), Natl Univ Singapore, Ctr Adv 2D Mat, Singapore, Singapore; Eda, G (corresponding author), Natl Univ Singapore, Dept Chem, Singapore, Singapore; Quek, SY (corresponding author), Natl Univ Singapore, NUS Grad Sch, Integrat Sci & Engn Programme, Singapore, Singapore; Quek, SY (corresponding author), Natl Univ Singapore, NUS Coll, Singapore, Singapore
- FUMinistry of Education (MOE), Singapore under AcRF Tier 3 [MOE2018-T3-1-005]; Singapore National Research Foundation [EDUN C-33-18-279-V12]; Ministry of Education (Singapore) through the Research Centre of Excellence program [FA8655-21-1-7026]; Air Force European Office of Aerospace Research and Development Office of Scientific Research [T2EP50122-0012]; Office of Naval Research Global [2022/46/E/ST3/00166]; Ministry of Education, Singapore [R-284-000-179-133]; National Science Centre, Poland [19H05790, 20H00354, 21H05233]; National University of Singapore; MOE; MOE's AcRF Tier 1; JSPS KAKENHI
- FXThe authors acknowledge support from the Ministry of Education (MOE), Singapore, under AcRF Tier 3 (MOE2018-T3-1-005) and the Singapore National Research Foundation for funding the research under medium-sized centre programme. This project was supported by the Ministry of Education (Singapore) through the Research Centre of Excellence program (grant EDUN C-33-18-279-V12, I-FIM). This material was based upon work supported by the Air Force European Office of Aerospace Research and Development Office of Scientific Research and the Office of Naval Research Global under award number FA8655-21-1-7026. This research is supported by the Ministry of Education, Singapore, under its Academic Research Fund Tier 2 (T2EP50122-0012). The work was supported by the National Science Centre, Poland (grant no. 2022/46/E/ST3/00166). S.Y.Q. acknowledges computational resources at the CA2DM cluster and at the National Supercomputing Centre (NSCC) in Singapore, and funding from the National University of Singapore and MOE. L.L. and M.B. acknowledge support from MOE's AcRF Tier 1 (R-284-000-179-133). This work was performed in part at the Australian National Fabrication Facility (ANFF), a company established under the National Collaborative Research Infrastructure Strategy, through the La Trobe University Centre for Materials and Surface Science. K.W. and T.T. acknowledge support from JSPS KAKENHI (Grant Numbers 19H05790, 20H00354 and 21H05233).
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Qiu, Zhizhan; Vaklinova, Kristina; Huang, Pengru; Grzeszczyk, Magdalena; Watanabe, Kenji; Taniguchi, Takashi; Novoselov, Kostya S; Lu, Jiong; Koperski, Maciej Atomic and Electronic Structure of Defects in hBN: Enhancing Single-Defect Functionalities ACS NANO, 18 (35), pp. 24035-24043, 2024, DOI: 10.1021/acsnano.4c03640. Abstract | BibTeX | Endnote @article{ISI:001295117800001,
title = {Atomic and Electronic Structure of Defects in hBN: Enhancing Single-Defect Functionalities},
author = {Zhizhan Qiu and Kristina Vaklinova and Pengru Huang and Magdalena Grzeszczyk and Kenji Watanabe and Takashi Taniguchi and Kostya S Novoselov and Jiong Lu and Maciej Koperski},
doi = {10.1021/acsnano.4c03640},
times_cited = {0},
issn = {1936-0851},
year = {2024},
date = {2024-08-20},
journal = {ACS NANO},
volume = {18},
number = {35},
pages = {24035-24043},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Defect centers in insulators play a critical role in creating important functionalities in materials: prototype qubits, single-photon sources, magnetic field probes, and pressure sensors. These functionalities are highly dependent on their midgap electronic structure and orbital/spin wave function contributions. However, in most cases, these fundamental properties remain unknown or speculative due to the defects being deeply embedded beneath the surface of highly resistive host crystals, thus impeding access through surface probes. Here, we directly inspected the atomic and electronic structures of defects in thin carbon-doped hexagonal boron nitride (hBN:C) by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Such investigation adds direct information about the electronic midgap states to the well-established photoluminescence response (including single-photon emission) of intentionally created carbon defects in the most commonly investigated van der Waals insulator. Our joint atomic-scale experimental and theoretical investigations reveal two main categories of defects: (1) single-site defects manifesting as donor-like states with atomically resolved structures observable via STM and (2) multisite defect complexes exhibiting a ladder of empty and occupied midgap states characterized by distinct spatial geometries. Combining direct probing of midgap states through tunneling spectroscopy with the inspection of the optical response of insulators hosting specific defect structures holds promise for creating and enhancing functionalities realized with individual defects in the quantum limit. These findings underscore not only the versatility of hBN:C as a platform for quantum defect engineering but also its potential to drive advancements in atomic-scale optoelectronics.},
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pubstate = {published},
tppubtype = {article}
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Defect centers in insulators play a critical role in creating important functionalities in materials: prototype qubits, single-photon sources, magnetic field probes, and pressure sensors. These functionalities are highly dependent on their midgap electronic structure and orbital/spin wave function contributions. However, in most cases, these fundamental properties remain unknown or speculative due to the defects being deeply embedded beneath the surface of highly resistive host crystals, thus impeding access through surface probes. Here, we directly inspected the atomic and electronic structures of defects in thin carbon-doped hexagonal boron nitride (hBN:C) by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Such investigation adds direct information about the electronic midgap states to the well-established photoluminescence response (including single-photon emission) of intentionally created carbon defects in the most commonly investigated van der Waals insulator. Our joint atomic-scale experimental and theoretical investigations reveal two main categories of defects: (1) single-site defects manifesting as donor-like states with atomically resolved structures observable via STM and (2) multisite defect complexes exhibiting a ladder of empty and occupied midgap states characterized by distinct spatial geometries. Combining direct probing of midgap states through tunneling spectroscopy with the inspection of the optical response of insulators hosting specific defect structures holds promise for creating and enhancing functionalities realized with individual defects in the quantum limit. These findings underscore not only the versatility of hBN:C as a platform for quantum defect engineering but also its potential to drive advancements in atomic-scale optoelectronics. - FNClarivate Analytics Web of Science
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Vaklinova, K
Huang, PR
Grzeszczyk, M
Watanabe, K
Taniguchi, T
Novoselov, KS
Lu, J
Koperski, M
- AFZhizhan Qiu
Kristina Vaklinova
Pengru Huang
Magdalena Grzeszczyk
Kenji Watanabe
Takashi Taniguchi
Kostya S Novoselov
Jiong Lu
Maciej Koperski
- TIAtomic and Electronic Structure of Defects in hBN: Enhancing Single-Defect Functionalities
- SOACS NANO
- LAEnglish
- DTArticle
- DE2D Insulators; Hexagonal Boron Nitride; Singledefects; Discrete Midgap States; Wave Function Imaging
- IDBORON-NITRIDE; CENTERS
- ABDefect centers in insulators play a critical role in creating important functionalities in materials: prototype qubits, single-photon sources, magnetic field probes, and pressure sensors. These functionalities are highly dependent on their midgap electronic structure and orbital/spin wave function contributions. However, in most cases, these fundamental properties remain unknown or speculative due to the defects being deeply embedded beneath the surface of highly resistive host crystals, thus impeding access through surface probes. Here, we directly inspected the atomic and electronic structures of defects in thin carbon-doped hexagonal boron nitride (hBN:C) by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Such investigation adds direct information about the electronic midgap states to the well-established photoluminescence response (including single-photon emission) of intentionally created carbon defects in the most commonly investigated van der Waals insulator. Our joint atomic-scale experimental and theoretical investigations reveal two main categories of defects: (1) single-site defects manifesting as donor-like states with atomically resolved structures observable via STM and (2) multisite defect complexes exhibiting a ladder of empty and occupied midgap states characterized by distinct spatial geometries. Combining direct probing of midgap states through tunneling spectroscopy with the inspection of the optical response of insulators hosting specific defect structures holds promise for creating and enhancing functionalities realized with individual defects in the quantum limit. These findings underscore not only the versatility of hBN:C as a platform for quantum defect engineering but also its potential to drive advancements in atomic-scale optoelectronics.
- C1[Qiu, Zhizhan; Huang, Pengru; Grzeszczyk, Magdalena; Novoselov, Kostya S.; Koperski, Maciej] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore.
[Qiu, Zhizhan; Vaklinova, Kristina; Huang, Pengru; Grzeszczyk, Magdalena; Novoselov, Kostya S.; Lu, Jiong; Koperski, Maciej] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore.
[Watanabe, Kenji] Natl Inst Mat Sci, Res Ctr Elect & Opt Mat, Tsukuba 3050044, Japan.
[Taniguchi, Takashi] Natl Inst Mat Sci, Res Ctr Mat Nanoarchitecton, Tsukuba 3050044, Japan.
[Lu, Jiong] Natl Univ Singapore, Dept Chem, Singapore 117543, Singapore - C3National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); National Institute for Materials Science; National Institute for Materials Science; National University of Singapore
- RPKoperski, M (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Dept Chem, Singapore 117543, Singapore
- FUMinistry of Education (Singapore) [EDUN C-33-18-279-V12]; AcRF Tier 3 [MOE2018-T3-1-005]; MOE Tier 2 [MOE-T2EP10223-0004, MOE-T2EP10123-0004, MOE-T2EP50122-0012]; Agency for Science, Technology and Research (A*STAR) [M21K2c0113]; Air Force Office of Scientific Research [FA8655-21-1-7026]; Office of Naval Research Global [20H00354, 23H02052]; JSPS KAKENHI [2021YFB3802400]; World Premier International Research Center Initiative (WPI), MEXT, Japan [52161037]; National Key Research and Development Program; National Natural Science Foundation of China
- FXThis project was supported by the Ministry of Education (Singapore) through the Research Centre of Excellence program (grant EDUN C-33-18-279-V12, I-FIM), AcRF Tier 3 (MOE2018-T3-1-005) and MOE Tier 2 grants (MOE-T2EP10223-0004, MOE-T2EP10123-0004, and MOE-T2EP50122-0012), and Agency for Science, Technology and Research (A*STAR) under MTC Individual Research Grants (M21K2c0113). This material is based upon work supported by the Air Force Office of Scientific Research and the Office of Naval Research Global under award number FA8655-21-1-7026. K.W. and T.T. acknowledge support from the JSPS KAKENHI (Grant Numbers 20H00354 and 23H02052) and World Premier International Research Center Initiative (WPI), MEXT, Japan. P.H. acknowledges the support from the National Key Research and Development Program (2021YFB3802400) and the National Natural Science Foundation of China (52161037). The computational work for this article was performed on computational resources at the National Supercomputing Center of Singapore (NSCC).
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Qi, Rongrong; You, Yi; Grzeszczyk, Magdalena; Jyothilal, Hiran; Bera, Achintya; Laverock, Jude; Natera-Cordero, Noel; Huang, Pengru; Nam, Gwang-Hyeon; Kravets, Vasyl G; Burrow, Daniel; Figueroa, Jesus Carlos Toscano; Ho, Yi Wei; Fox, Neil A; Grigorenko, Alexander N; Vera-Marun, Ivan J; Keerthi, Ashok; Koperski, Maciej; Radha, Boya Versatile Method for Preparing Two-Dimensional Metal Dihalides ACS NANO, 18 (33), pp. 22034-22044, 2024, DOI: 10.1021/acsnano.4c04397. Abstract | BibTeX | Endnote @article{ISI:001285545300001,
title = {Versatile Method for Preparing Two-Dimensional Metal Dihalides},
author = {Rongrong Qi and Yi You and Magdalena Grzeszczyk and Hiran Jyothilal and Achintya Bera and Jude Laverock and Noel Natera-Cordero and Pengru Huang and Gwang-Hyeon Nam and Vasyl G Kravets and Daniel Burrow and Jesus Carlos Toscano Figueroa and Yi Wei Ho and Neil A Fox and Alexander N Grigorenko and Ivan J Vera-Marun and Ashok Keerthi and Maciej Koperski and Boya Radha},
doi = {10.1021/acsnano.4c04397},
times_cited = {0},
issn = {1936-0851},
year = {2024},
date = {2024-08-06},
journal = {ACS NANO},
volume = {18},
number = {33},
pages = {22034-22044},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Ever since the ground-breaking isolation of graphene, numerous two-dimensional (2D) materials have emerged with 2D metal dihalides gaining significant attention due to their intriguing electrical and magnetic properties. In this study, we introduce an innovative approach via anhydrous solvent-induced recrystallization of bulk powders to obtain crystals of metal dihalides (MX2, with M = Cu, Ni, Co and X = Br, Cl, I), which can be exfoliated to 2D flakes. We demonstrate the effectiveness of our method using CuBr2 as an example, which forms large layered crystals. We investigate the structural properties of both the bulk and 2D CuBr2 using X-ray diffraction, along with Raman scattering and optical spectroscopy, revealing its quasi-1D chain structure, which translates to distinct emission and scattering characteristics. Furthermore, microultraviolet photoemission spectroscopy and electronic transport reveal the electronic properties of CuBr2 flakes, including their valence band structure. We extend our methodology to other metal halides and assess the stability of the metal halide flakes in controlled environments. We show that optical contrast can be used to characterize the flake thicknesses for these materials. Our findings demonstrate the versatility and potential applications of the proposed methodology for preparing and studying 2D metal halide flakes.},
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Ever since the ground-breaking isolation of graphene, numerous two-dimensional (2D) materials have emerged with 2D metal dihalides gaining significant attention due to their intriguing electrical and magnetic properties. In this study, we introduce an innovative approach via anhydrous solvent-induced recrystallization of bulk powders to obtain crystals of metal dihalides (MX2, with M = Cu, Ni, Co and X = Br, Cl, I), which can be exfoliated to 2D flakes. We demonstrate the effectiveness of our method using CuBr2 as an example, which forms large layered crystals. We investigate the structural properties of both the bulk and 2D CuBr2 using X-ray diffraction, along with Raman scattering and optical spectroscopy, revealing its quasi-1D chain structure, which translates to distinct emission and scattering characteristics. Furthermore, microultraviolet photoemission spectroscopy and electronic transport reveal the electronic properties of CuBr2 flakes, including their valence band structure. We extend our methodology to other metal halides and assess the stability of the metal halide flakes in controlled environments. We show that optical contrast can be used to characterize the flake thicknesses for these materials. Our findings demonstrate the versatility and potential applications of the proposed methodology for preparing and studying 2D metal halide flakes. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUQi, RR
You, Y
Grzeszczyk, M
Jyothilal, H
Bera, A
Laverock, J
Natera-Cordero, N
Huang, PR
Nam, GH
Kravets, VG
Burrow, D
Figueroa, JCT
Ho, YW
Fox, NA
Grigorenko, AN
Vera-Marun, IJ
Keerthi, A
Koperski, M
Radha, B
- AFRongrong Qi
Yi You
Magdalena Grzeszczyk
Hiran Jyothilal
Achintya Bera
Jude Laverock
Noel Natera-Cordero
Pengru Huang
Gwang-Hyeon Nam
Vasyl G Kravets
Daniel Burrow
Jesus Carlos Toscano Figueroa
Yi Wei Ho
Neil A Fox
Alexander N Grigorenko
Ivan J Vera-Marun
Ashok Keerthi
Maciej Koperski
Boya Radha
- TIVersatile Method for Preparing Two-Dimensional Metal Dihalides
- SOACS NANO
- LAEnglish
- DTArticle
- DETwo-dimensional Materials; Metal Dihalides; Mechanical Exfoliation; Solvent-assisted Recrystallization; Photoemission; Raman Scattering Spectroscopy
- IDMAGNETIC-PROPERTIES; EXFOLIATION; CRYSTAL
- ABEver since the ground-breaking isolation of graphene, numerous two-dimensional (2D) materials have emerged with 2D metal dihalides gaining significant attention due to their intriguing electrical and magnetic properties. In this study, we introduce an innovative approach via anhydrous solvent-induced recrystallization of bulk powders to obtain crystals of metal dihalides (MX2, with M = Cu, Ni, Co and X = Br, Cl, I), which can be exfoliated to 2D flakes. We demonstrate the effectiveness of our method using CuBr2 as an example, which forms large layered crystals. We investigate the structural properties of both the bulk and 2D CuBr2 using X-ray diffraction, along with Raman scattering and optical spectroscopy, revealing its quasi-1D chain structure, which translates to distinct emission and scattering characteristics. Furthermore, microultraviolet photoemission spectroscopy and electronic transport reveal the electronic properties of CuBr2 flakes, including their valence band structure. We extend our methodology to other metal halides and assess the stability of the metal halide flakes in controlled environments. We show that optical contrast can be used to characterize the flake thicknesses for these materials. Our findings demonstrate the versatility and potential applications of the proposed methodology for preparing and studying 2D metal halide flakes.
- C1[Qi, Rongrong; You, Yi; Jyothilal, Hiran; Bera, Achintya; Natera-Cordero, Noel; Nam, Gwang-Hyeon; Kravets, Vasyl G.; Burrow, Daniel; Figueroa, Jesus Carlos Toscano; Grigorenko, Alexander N.; Vera-Marun, Ivan J.; Radha, Boya] Univ Manchester, Dept Phys & Astron, Manchester M13 9PL, England.
[Qi, Rongrong; You, Yi; Jyothilal, Hiran; Bera, Achintya; Natera-Cordero, Noel; Nam, Gwang-Hyeon; Burrow, Daniel; Vera-Marun, Ivan J.; Keerthi, Ashok; Radha, Boya] Univ Manchester, Natl Graphene Inst, Manchester M13 9PL, England.
[Grzeszczyk, Magdalena; Huang, Pengru; Koperski, Maciej] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore.
[Grzeszczyk, Magdalena; Huang, Pengru; Ho, Yi Wei; Koperski, Maciej] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore.
[Bera, Achintya] Univ Manchester, Photon Sci Inst, Manchester M13 9PL, England.
[Laverock, Jude; Fox, Neil A.] Univ Bristol, Sch Chem, Bristol BS8 1TS, England.
[Ho, Yi Wei] Natl Univ Singapore, Dept Phys, Singapore 117542, Singapore.
[Keerthi, Ashok] Univ Manchester, Dept Chem, Manchester M13 9PL, England - C3University of Manchester; University of Manchester; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; University of Manchester; University of Bristol; National University of Singapore; University of Manchester
- RPRadha, B (corresponding author), Univ Manchester, Dept Phys & Astron, Manchester M13 9PL, England; Radha, B (corresponding author), Univ Manchester, Natl Graphene Inst, Manchester M13 9PL, England; Koperski, M (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore; Koperski, M (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore
- FUEuropean Union's H2020 Framework Programme/European Research Council Starting Grant [852674 - AngstroCAP]; Royal Society University Research Fellowship [URF/R1/180127, RFERE210016]; Philip Leverhulme Prize [PLP-2021-262]; EPSRC New Horizons grant [EP/X019225/1]; University of Manchester-China Scholarship Council scheme [EP/V048112/1, EP/W006502/1]; EPSRC [EDUN C-33-18-279-V12]; Ministry of Education (Singapore) through the Research Centre of Excellence program [MOE-T2EP50122-0012]; Academic Research Fund Tier 2 [FA8655-21-1-7026]; Air Force Office of Scientific Research; Office of Naval Research Global; Consejo Nacional de Ciencia y Tecnologia (Mexico); EPSRC Doctoral Training Partnership (DTP)
- FXB.R. acknowledges funding from the European Union's H2020 Framework Programme/European Research Council Starting Grant (852674 - AngstroCAP), Royal Society University Research Fellowship (URF/R1/180127, RFERE210016), Philip Leverhulme Prize PLP-2021-262, EPSRC New Horizons grant EP/X019225/1. R.Q. acknowledges funding from the University of Manchester-China Scholarship Council scheme. A.K. acknowledges EPSRC's new horizons grant (EP/V048112/1). M.K. acknowledges the support from the Ministry of Education (Singapore) through the Research Centre of Excellence program (grant EDUN C-33-18-279-V12, I-FIM); Academic Research Fund Tier 2 (MOE-T2EP50122-0012); and Air Force Office of Scientific Research and the Office of Naval Research Global under award number FA8655-21-1-7026. J.C.T.F. and N.N.-C. acknowledge support from the Consejo Nacional de Ciencia y Tecnologia (Mexico). D.B. acknowledges support from the EPSRC Doctoral Training Partnership (DTP). The authors acknowledge the support from J. Pandey and A. Soni for their MATLAB codes of optical contrast simulation, as well as from E. Navarro-Moratalla, D. R. Klein, and P. Jarillo-Herrero from MIT for discussion on Kramers-Kronig relation and sharing their codes. The authors acknowledge the use of the Bristol Ultraquiet NanoESCA Laboratory (BrUNEL) and lithography, in situ AFM imaging facility of EPSRC strategic equipment grant (EP/W006502/1). From the University of Manchester, the authors acknowledge G. Whitehead and G. Harrison for the XRD measurements; N. Hewitson and I. T. Wilson for assisting with optical contrast simulation; and D. Mccullagh and M. Sellers for the fabrication of hermetic cells.
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- PUAMER CHEMICAL SOC
- PIWASHINGTON
- PA1155 16TH ST, NW, WASHINGTON, DC 20036 USA
- SN1936-0851
- J9ACS NANO
- JIACS Nano
- PDAUG 6
- PY2024
- VL18
- BP22034
- EP22044
- DI10.1021/acsnano.4c04397
- PG11
- WCChemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary
- SCChemistry; Science & Technology - Other Topics; Materials Science
- GAD2L4J
- UTWOS:001285545300001
- ER
- EF
|
Grzeszczyk, Magdalena; Vaklinova, Kristina; Watanabe, Kenji; Taniguchi, Takashi; Novoselov, Konstantin S; Koperski, Maciej Electroluminescence from pure resonant states in hBN-based vertical tunneling junctions LIGHT-SCIENCE & APPLICATIONS, 13 (1), 2024, DOI: 10.1038/s41377-024-01491-5. Abstract | BibTeX | Endnote @article{ISI:001265495000003,
title = {Electroluminescence from pure resonant states in hBN-based vertical tunneling junctions},
author = {Magdalena Grzeszczyk and Kristina Vaklinova and Kenji Watanabe and Takashi Taniguchi and Konstantin S Novoselov and Maciej Koperski},
doi = {10.1038/s41377-024-01491-5},
times_cited = {1},
issn = {2095-5545},
year = {2024},
date = {2024-07-08},
journal = {LIGHT-SCIENCE & APPLICATIONS},
volume = {13},
number = {1},
publisher = {SPRINGERNATURE},
address = {CAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND},
abstract = {Defect centers in wide-band-gap crystals have garnered interest for their potential in applications among optoelectronic and sensor technologies. However, defects embedded in highly insulating crystals, like diamond, silicon carbide, or aluminum oxide, have been notoriously difficult to excite electrically due to their large internal resistance. To address this challenge, we realized a new paradigm of exciting defects in vertical tunneling junctions based on carbon centers in hexagonal boron nitride (hBN). The rational design of the devices via van der Waals technology enabled us to raise and control optical processes related to defect-to-band and intradefect electroluminescence. The fundamental understanding of the tunneling events was based on the transfer of the electronic wave function amplitude between resonant defect states in hBN to the metallic state in graphene, which leads to dramatic changes in the characteristics of electrons due to different band structures of constituent materials. In our devices, the decay of electrons via tunneling pathways competed with radiative recombination, resulting in an unprecedented degree of tuneability of carrier dynamics due to the significant sensitivity of the characteristic tunneling times on the thickness and structure of the barrier. This enabled us to achieve a high-efficiency electrical excitation of intradefect transitions, exceeding by several orders of magnitude the efficiency of optical excitation in the sub-band-gap regime. This work represents a significant advancement towards a universal and scalable platform for electrically driven devices utilizing defect centers in wide-band-gap crystals with properties modulated via activation of different tunneling mechanisms at a level of device engineering.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Defect centers in wide-band-gap crystals have garnered interest for their potential in applications among optoelectronic and sensor technologies. However, defects embedded in highly insulating crystals, like diamond, silicon carbide, or aluminum oxide, have been notoriously difficult to excite electrically due to their large internal resistance. To address this challenge, we realized a new paradigm of exciting defects in vertical tunneling junctions based on carbon centers in hexagonal boron nitride (hBN). The rational design of the devices via van der Waals technology enabled us to raise and control optical processes related to defect-to-band and intradefect electroluminescence. The fundamental understanding of the tunneling events was based on the transfer of the electronic wave function amplitude between resonant defect states in hBN to the metallic state in graphene, which leads to dramatic changes in the characteristics of electrons due to different band structures of constituent materials. In our devices, the decay of electrons via tunneling pathways competed with radiative recombination, resulting in an unprecedented degree of tuneability of carrier dynamics due to the significant sensitivity of the characteristic tunneling times on the thickness and structure of the barrier. This enabled us to achieve a high-efficiency electrical excitation of intradefect transitions, exceeding by several orders of magnitude the efficiency of optical excitation in the sub-band-gap regime. This work represents a significant advancement towards a universal and scalable platform for electrically driven devices utilizing defect centers in wide-band-gap crystals with properties modulated via activation of different tunneling mechanisms at a level of device engineering. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUGrzeszczyk, M
Vaklinova, K
Watanabe, K
Taniguchi, T
Novoselov, KS
Koperski, M
- AFMagdalena Grzeszczyk
Kristina Vaklinova
Kenji Watanabe
Takashi Taniguchi
Konstantin S Novoselov
Maciej Koperski
- TIElectroluminescence from pure resonant states in hBN-based vertical tunneling junctions
- SOLIGHT-SCIENCE & APPLICATIONS
- LAEnglish
- DTArticle
- IDNUCLEAR-SPIN QUBITS; BORON-NITRIDE; ELECTRON; EMISSION; DYNAMICS; DIAMOND; CENTERS
- ABDefect centers in wide-band-gap crystals have garnered interest for their potential in applications among optoelectronic and sensor technologies. However, defects embedded in highly insulating crystals, like diamond, silicon carbide, or aluminum oxide, have been notoriously difficult to excite electrically due to their large internal resistance. To address this challenge, we realized a new paradigm of exciting defects in vertical tunneling junctions based on carbon centers in hexagonal boron nitride (hBN). The rational design of the devices via van der Waals technology enabled us to raise and control optical processes related to defect-to-band and intradefect electroluminescence. The fundamental understanding of the tunneling events was based on the transfer of the electronic wave function amplitude between resonant defect states in hBN to the metallic state in graphene, which leads to dramatic changes in the characteristics of electrons due to different band structures of constituent materials. In our devices, the decay of electrons via tunneling pathways competed with radiative recombination, resulting in an unprecedented degree of tuneability of carrier dynamics due to the significant sensitivity of the characteristic tunneling times on the thickness and structure of the barrier. This enabled us to achieve a high-efficiency electrical excitation of intradefect transitions, exceeding by several orders of magnitude the efficiency of optical excitation in the sub-band-gap regime. This work represents a significant advancement towards a universal and scalable platform for electrically driven devices utilizing defect centers in wide-band-gap crystals with properties modulated via activation of different tunneling mechanisms at a level of device engineering.
- C1[Grzeszczyk, Magdalena; Vaklinova, Kristina; Novoselov, Konstantin S.; Koperski, Maciej] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore.
[Watanabe, Kenji] Natl Inst Mat Sci, Res Ctr Funct Mat, Tsukuba 3050044, Japan.
[Taniguchi, Takashi] Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton, Tsukuba 3050044, Japan.
[Novoselov, Konstantin S.; Koperski, Maciej] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore - C3Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National Institute for Materials Science; National Institute for Materials Science; National University of Singapore
- RPGrzeszczyk, M (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore; Koperski, M (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore
- FUMinistry of Education (Singapore) through the Research Centre of Excellence program (grant EDUN C-33-18-279-V12, I-FIM), AcRF Tier 3 (MOE2018- T3-1-005). [EDUN C-33-18-279-V12, MOE2018-T3-1-005]; Ministry of Education (Singapore) through the Research Centre of Excellence program [MOE-T2EP50122-0012]; Ministry of Education, Singapore [FA8655-21-1-7026]; Air Force Office of Scientific Research [19H05790, 20H00354, 21H05233]; Office of Naval Research Global; JSPS KAKENHI
- FXThis project was supported by the Ministry of Education (Singapore) through the Research Centre of Excellence program (grant EDUN C-33-18-279-V12, I-FIM), AcRF Tier 3 (MOE2018-T3-1-005). This research is supported by the Ministry of Education, Singapore, under its Academic Research Fund Tier 2 (MOE-T2EP50122-0012). This material is based upon work supported by the Air Force Office of Scientific Research and the Office of Naval Research Global under award number FA8655-21-1-7026. K.W. and T.T. acknowledge support from JSPS KAKENHI (Grant Numbers 19H05790, 20H00354, and 21H05233).
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- PUSPRINGERNATURE
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- SN2095-5545
- J9LIGHT-SCI APPL
- JILight-Sci. Appl.
- PDJUL 8
- PY2024
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- DI10.1038/s41377-024-01491-5
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- UTWOS:001265495000003
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