2024
|
Qiu, Zhizhan; Han, Yixuan; Noori, Keian; Chen, Zhaolong; Kashchenko, Mikhail; Lin, Li; Olsen, Thomas; Li, Jing; Fang, Hanyan; Lyu, Pin; Telychko, Mykola; Gu, Xingyu; Adam, Shaffique; Quek, Su Ying; Rodin, Aleksandr; Neto, Castro A H; Novoselov, Kostya S; Lu, Jiong Evidence for electron-hole crystals in a Mott insulator NATURE MATERIALS, 2024, DOI: 10.1038/s41563-024-01910-3. Abstract | BibTeX | Endnote @article{ISI:001237790900002,
title = {Evidence for electron-hole crystals in a Mott insulator},
author = {Zhizhan Qiu and Yixuan Han and Keian Noori and Zhaolong Chen and Mikhail Kashchenko and Li Lin and Thomas Olsen and Jing Li and Hanyan Fang and Pin Lyu and Mykola Telychko and Xingyu Gu and Shaffique Adam and Su Ying Quek and Aleksandr Rodin and Castro A H Neto and Kostya S Novoselov and Jiong Lu},
doi = {10.1038/s41563-024-01910-3},
times_cited = {0},
issn = {1476-1122},
year = {2024},
date = {2024-06-03},
journal = {NATURE MATERIALS},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {The coexistence of correlated electron and hole crystals enables the realization of quantum excitonic states, capable of hosting counterflow superfluidity and topological orders with long-range quantum entanglement. Here we report evidence for imbalanced electron-hole crystals in a doped Mott insulator, namely, alpha-RuCl3, through gate-tunable non-invasive van der Waals doping from graphene. Real-space imaging via scanning tunnelling microscopy reveals two distinct charge orderings at the lower and upper Hubbard band energies, whose origin is attributed to the correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru-Ru bonds, respectively. Moreover, a gate-induced transition of electron-hole crystals is directly visualized, further corroborating their nature as correlation-driven charge crystals. The realization and atom-resolved visualization of imbalanced electron-hole crystals in a doped Mott insulator opens new doors in the search for correlated bosonic states within strongly correlated materials.},
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The coexistence of correlated electron and hole crystals enables the realization of quantum excitonic states, capable of hosting counterflow superfluidity and topological orders with long-range quantum entanglement. Here we report evidence for imbalanced electron-hole crystals in a doped Mott insulator, namely, alpha-RuCl3, through gate-tunable non-invasive van der Waals doping from graphene. Real-space imaging via scanning tunnelling microscopy reveals two distinct charge orderings at the lower and upper Hubbard band energies, whose origin is attributed to the correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru-Ru bonds, respectively. Moreover, a gate-induced transition of electron-hole crystals is directly visualized, further corroborating their nature as correlation-driven charge crystals. The realization and atom-resolved visualization of imbalanced electron-hole crystals in a doped Mott insulator opens new doors in the search for correlated bosonic states within strongly correlated materials. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUQiu, ZZ
Han, YX
Noori, K
Chen, ZL
Kashchenko, M
Lin, L
Olsen, T
Li, J
Fang, HY
Lyu, P
Telychko, M
Gu, XY
Adam, S
Quek, SY
Rodin, A
Neto, AHC
Novoselov, KS
Lu, J
- AFZhizhan Qiu
Yixuan Han
Keian Noori
Zhaolong Chen
Mikhail Kashchenko
Li Lin
Thomas Olsen
Jing Li
Hanyan Fang
Pin Lyu
Mykola Telychko
Xingyu Gu
Shaffique Adam
Su Ying Quek
Aleksandr Rodin
Castro A H Neto
Kostya S Novoselov
Jiong Lu
- TIEvidence for electron-hole crystals in a Mott insulator
- SONATURE MATERIALS
- LAEnglish
- DTArticle
- IDWIGNER CRYSTAL
- ABThe coexistence of correlated electron and hole crystals enables the realization of quantum excitonic states, capable of hosting counterflow superfluidity and topological orders with long-range quantum entanglement. Here we report evidence for imbalanced electron-hole crystals in a doped Mott insulator, namely, alpha-RuCl3, through gate-tunable non-invasive van der Waals doping from graphene. Real-space imaging via scanning tunnelling microscopy reveals two distinct charge orderings at the lower and upper Hubbard band energies, whose origin is attributed to the correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru-Ru bonds, respectively. Moreover, a gate-induced transition of electron-hole crystals is directly visualized, further corroborating their nature as correlation-driven charge crystals. The realization and atom-resolved visualization of imbalanced electron-hole crystals in a doped Mott insulator opens new doors in the search for correlated bosonic states within strongly correlated materials.
- C1[Qiu, Zhizhan; Noori, Keian; Chen, Zhaolong; Lin, Li; Neto, A. H. Castro; Novoselov, Kostya S.; Lu, Jiong] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore.
[Han, Yixuan; Fang, Hanyan; Lyu, Pin; Telychko, Mykola; Lu, Jiong] Natl Univ Singapore, Dept Chem, Singapore, Singapore. [Noori, Keian; Gu, Xingyu; Adam, Shaffique; Quek, Su Ying; Rodin, Aleksandr; Neto, A. H. Castro; Lu, Jiong] Natl Univ Singapore, Ctr Adv Mat 2D CA2DM, Singapore, Singapore. [Chen, Zhaolong] Peking Univ, Shenzhen Grad Sch, Sch Adv Mat, Shenzhen, Peoples R China. [Kashchenko, Mikhail] Brain & Consciousness Res Ctr, Programmable Funct Mat Lab, Moscow, Russia. [Kashchenko, Mikhail] Moscow Inst Phys & Technol, Ctr Photon & Mat 2D, Dolgoprudnyi 141700, Russia. [Lin, Li] Peking Univ, Sch Mat Sci & Engn, Beijing, Peoples R China. [Olsen, Thomas] Tech Univ Denmark, Dept Phys, CAMD, Lyngby, Denmark. [Li, Jing] Beihang Univ, Sch Chem, Beijing, Peoples R China. [Gu, Xingyu; Adam, Shaffique; Quek, Su Ying] Natl Univ Singapore, Dept Phys, Singapore, Singapore. [Adam, Shaffique; Rodin, Aleksandr] Yale NUS Coll, Singapore, Singapore. [Adam, Shaffique; Quek, Su Ying; Neto, A. H. Castro; Novoselov, Kostya S.] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore, Singapore. [Quek, Su Ying] Natl Univ Singapore, NUS Grad Sch, Integrat Sci & Engn Programme, Singapore, Singapore - C3National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National University of Singapore; Peking University; Moscow Institute of Physics & Technology; Peking University; Technical University of Denmark; Beihang University; National University of Singapore; Yale NUS College; National University of Singapore; National University of Singapore
- RPNovoselov, KS (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Dept Chem, Singapore, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Ctr Adv Mat 2D CA2DM, Singapore, Singapore; Novoselov, KS (corresponding author), Natl Univ Singapore, Dept Mat Sci & Engn, Singapore, Singapore
- FUMinistry of Education - Singapore (MOE) [MOE-T2EP50121-0008, MOE-T2EP10221-0005, MOE-T2EP10123-0004]; Ministry of Education [M21K2c0113]; Agency for Science, Technology and Research (A*STAR) under its AME IRG Grant [EDUNC-33-18-279-V12]; Ministry of Education, Singapore (Research Centre of Excellence award) [RSRPR190000]; Royal Society, UK [21-79-20225]; Russian Science Foundation
- FXJ. Lu acknowledges support from Ministry of Education grants (MOE-T2EP50121-0008, MOE-T2EP10221-0005, MOE-T2EP10123-0004) and Agency for Science, Technology and Research (A*STAR) under its AME IRG Grant (M21K2c0113). 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 the Royal Society, UK (grant no. RSRPR190000). M.K. acknowledges support from the Russian Science Foundation (grant no. 21-79-20225) and Vladimir Potanin (through Brain and Consciousness Research Center).
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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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- SCChemistry; Science & Technology - Other Topics; Materials Science; Physics
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Li, Zejun; Li, Jing; Lu, Jiong Building artificial quantum solids via electrostatic assembly MATTER, 7 (3), pp. 739-742, 2024, DOI: 10.1016/j.matt.2024.02.007. Abstract | BibTeX | Endnote @article{ISI:001202831400001,
title = {Building artificial quantum solids via electrostatic assembly},
author = {Zejun Li and Jing Li and Jiong Lu},
doi = {10.1016/j.matt.2024.02.007},
times_cited = {0},
issn = {2590-2393},
year = {2024},
date = {2024-03-06},
journal = {MATTER},
volume = {7},
number = {3},
pages = {739-742},
publisher = {CELL PRESS},
address = {50 HAMPSHIRE ST, FLOOR 5, CAMBRIDGE, MA 02139 USA},
abstract = {Hybrid superlattices, comprised of alternatively stacked two-dimensional atomic crystals and molecular layers, serve as a promising platform for artificial quantum solids with desired properties. In this issue of Matter, Zhou et al. present a novel electrostatic co -assembly method that enables the synthesis of an extensive library encompassing 53 artificial hybrid superlattices.},
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Hybrid superlattices, comprised of alternatively stacked two-dimensional atomic crystals and molecular layers, serve as a promising platform for artificial quantum solids with desired properties. In this issue of Matter, Zhou et al. present a novel electrostatic co -assembly method that enables the synthesis of an extensive library encompassing 53 artificial hybrid superlattices. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AULi, ZJ
Li, J
Lu, J
- AFZejun Li
Jing Li
Jiong Lu
- TIBuilding artificial quantum solids via electrostatic assembly
- SOMATTER
- LAEnglish
- DTArticle
- ABHybrid superlattices, comprised of alternatively stacked two-dimensional atomic crystals and molecular layers, serve as a promising platform for artificial quantum solids with desired properties. In this issue of Matter, Zhou et al. present a novel electrostatic co -assembly method that enables the synthesis of an extensive library encompassing 53 artificial hybrid superlattices.
- C3Southeast University - China; National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); Beihang University
- RPLu, J (corresponding author), Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, 4 Sci Dr 2, Singapore 117544, Singapore
- FXJ. Lu acknowledges the support from MOE Tier 2 grants (MOE-T2EP10221-0005 and MOE-T2EP10123-0004) and the Agency for Science, Technology and Research (A*STAR) under MTC Individual Research Grants (project ID: M21K2c0113) . Z.L. acknowledges the support from National Nature Science Foundation of China (grant no. 22375041) , Start-up Research Fund of Southeast University (grant no. RF1028623202) , and the open research fund of Key Laboratory of Quantum Materials and Devices (Southeast University) , Ministry of Education.r fund of Key Laboratory of Quantum Ma-terials and Devices (Southeast Univer-sity) , Ministry of Education.
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Su, Jie; Li, Jiali; Guo, Na; Peng, Xinnan; Yin, Jun; Wang, Jiahao; Lyu, Pin; Luo, Zhiyao; Mouthaan, Koen; Wu, Jishan; Zhang, Chun; Wang, Xiaonan; Lu, Jiong Intelligent synthesis of magnetic nanographenes via chemist-intuited atomic robotic probe NATURE SYNTHESIS, 3 (3), pp. 280-280, 2024, DOI: 10.1038/s44160-024-00488-7. Abstract | BibTeX | Endnote @article{ISI:001178534900003,
title = {Intelligent synthesis of magnetic nanographenes via chemist-intuited atomic robotic probe},
author = {Jie Su and Jiali Li and Na Guo and Xinnan Peng and Jun Yin and Jiahao Wang and Pin Lyu and Zhiyao Luo and Koen Mouthaan and Jishan Wu and Chun Zhang and Xiaonan Wang and Jiong Lu},
doi = {10.1038/s44160-024-00488-7},
times_cited = {1},
year = {2024},
date = {2024-02-29},
journal = {NATURE SYNTHESIS},
volume = {3},
number = {3},
pages = {280-280},
publisher = {SPRINGERNATURE},
address = {CAMPUS, 4 CRINAN ST, LONDON, N1 9XW, ENGLAND},
abstract = {Atomic-scale manufacturing of carbon-based quantum materials with single-bond precision holds immense potential in advancing tailor-made quantum materials with unconventional properties, which are crucial in developing next-generation spintronic devices and quantum information technologies. On-surface chemistry approaches, including surface-assisted synthesis and probe-assisted manipulation, are impeded by challenges in reaction selectivity control or restricted by scalability and production efficiency. Here we demonstrate the concept of the chemist-intuited atomic robotic probe by integrating probe chemistry knowledge and artificial intelligence, allowing for atomically precise single-molecule manipulation to fabricate single-molecule quantum pi-magnets with single-bond precision. Our deep neural networks not only transform complex probe chemistry into machine-understandable tasks but also provide chemist intuition to elusive reaction mechanisms by extracting the critical chemical information within the data. A joint experimental and theoretical investigation demonstrates that a voltage-controlled two-electron-assisted electronic excitation enables synchronous six-bond transformations to extend the zigzag edge topology of single-molecule quantum pi-magnets, triggered by phenyl C(sp2)-H bond activation, which aligns with initial conjectures given by the deep neural models. Our work represents a transition from autonomous fabrication to intelligent synthesis with levels of selectivity and precision beyond current synthetic tools for improved synthesis of organic quantum materials towards on-chip integration.},
keywords = {},
pubstate = {published},
tppubtype = {article}
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Atomic-scale manufacturing of carbon-based quantum materials with single-bond precision holds immense potential in advancing tailor-made quantum materials with unconventional properties, which are crucial in developing next-generation spintronic devices and quantum information technologies. On-surface chemistry approaches, including surface-assisted synthesis and probe-assisted manipulation, are impeded by challenges in reaction selectivity control or restricted by scalability and production efficiency. Here we demonstrate the concept of the chemist-intuited atomic robotic probe by integrating probe chemistry knowledge and artificial intelligence, allowing for atomically precise single-molecule manipulation to fabricate single-molecule quantum pi-magnets with single-bond precision. Our deep neural networks not only transform complex probe chemistry into machine-understandable tasks but also provide chemist intuition to elusive reaction mechanisms by extracting the critical chemical information within the data. A joint experimental and theoretical investigation demonstrates that a voltage-controlled two-electron-assisted electronic excitation enables synchronous six-bond transformations to extend the zigzag edge topology of single-molecule quantum pi-magnets, triggered by phenyl C(sp2)-H bond activation, which aligns with initial conjectures given by the deep neural models. Our work represents a transition from autonomous fabrication to intelligent synthesis with levels of selectivity and precision beyond current synthetic tools for improved synthesis of organic quantum materials towards on-chip integration. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUSu, J
Li, JL
Guo, N
Peng, XN
Yin, J
Wang, JH
Lyu, P
Luo, ZY
Mouthaan, K
Wu, JS
Zhang, C
Wang, XN
Lu, J
- AFJie Su
Jiali Li
Na Guo
Xinnan Peng
Jun Yin
Jiahao Wang
Pin Lyu
Zhiyao Luo
Koen Mouthaan
Jishan Wu
Chun Zhang
Xiaonan Wang
Jiong Lu
- TIIntelligent synthesis of magnetic nanographenes via chemist-intuited atomic robotic probe
- SONATURE SYNTHESIS
- LAEnglish
- DTArticle
- IDON-SURFACE SYNTHESIS; SINGLE-MOLECULE; FORCE; TIP; STEPS
- ABAtomic-scale manufacturing of carbon-based quantum materials with single-bond precision holds immense potential in advancing tailor-made quantum materials with unconventional properties, which are crucial in developing next-generation spintronic devices and quantum information technologies. On-surface chemistry approaches, including surface-assisted synthesis and probe-assisted manipulation, are impeded by challenges in reaction selectivity control or restricted by scalability and production efficiency. Here we demonstrate the concept of the chemist-intuited atomic robotic probe by integrating probe chemistry knowledge and artificial intelligence, allowing for atomically precise single-molecule manipulation to fabricate single-molecule quantum pi-magnets with single-bond precision. Our deep neural networks not only transform complex probe chemistry into machine-understandable tasks but also provide chemist intuition to elusive reaction mechanisms by extracting the critical chemical information within the data. A joint experimental and theoretical investigation demonstrates that a voltage-controlled two-electron-assisted electronic excitation enables synchronous six-bond transformations to extend the zigzag edge topology of single-molecule quantum pi-magnets, triggered by phenyl C(sp2)-H bond activation, which aligns with initial conjectures given by the deep neural models. Our work represents a transition from autonomous fabrication to intelligent synthesis with levels of selectivity and precision beyond current synthetic tools for improved synthesis of organic quantum materials towards on-chip integration.
- C1[Su, Jie; Peng, Xinnan; Lyu, Pin; Wu, Jishan; Zhang, Chun; Lu, Jiong] Natl Univ Singapore, Dept Chem, Singapore, Singapore.
[Li, Jiali; Yin, Jun; Luo, Zhiyao] Natl Univ Singapore, Coll Design & Engn, Dept Chem & Biomol Engn, Singapore, Singapore. [Guo, Na; Zhang, Chun] Natl Univ Singapore, Chongqing Res Inst, Chongqing, Peoples R China. [Guo, Na; Zhang, Chun] Natl Univ Singapore, Dept Phys, Singapore, Singapore. [Wang, Jiahao; Mouthaan, Koen] Natl Univ Singapore, Coll Design & Engn, Dept Elect & Comp Engn, Singapore, Singapore. [Wang, Xiaonan] Tsinghua Univ, Dept Chem Engn, Beijing, Peoples R China. [Lu, Jiong] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore. [Lu, Jiong] Natl Univ Singapore, Suzhou Res Inst, Suzhou, Peoples R China - C3National University of Singapore; National University of Singapore; National University of Singapore; National University of Singapore; National University of Singapore; Tsinghua University; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National University of Singapore
- RPZhang, C (corresponding author), Natl Univ Singapore, Dept Chem, Singapore, Singapore; Zhang, C (corresponding author), Natl Univ Singapore, Chongqing Res Inst, Chongqing, Peoples R China; Zhang, C (corresponding author), Natl Univ Singapore, Dept Phys, Singapore, Singapore; Wang, XN (corresponding author), Tsinghua Univ, Dept Chem Engn, Beijing, Peoples R China; Lu, J (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Suzhou Res Inst, Suzhou, Peoples R China
- FUNational Research Foundation Singapore (National Research Foundation-Prime Minister's office, Republic of Singapore) [NRF-CRP29-2022-0004]; NRF, Prime Minister's Office, Singapore, under the Competitive Research Program Award [MOE2019-T2-2-030]; MOE Tier 2 grants [M21K2c0113]; Agency for Science, Technology and Research (A*STAR) under MTC Individual Research Grants [BZ2022056]; Science and Technology Project of Jiangsu Province [2022ZD0117501]; National Key R&D Program of China [A1898b0043]; Agency for Science, Technology and Research (A*STAR) Singapore RIE2020 Advanced Manufacturing and Engineering Programmatic [A2084c0171]; Tsinghua University Initiative Scientific Research Program; Agency for Science, Technology and Research (A*STAR) Advanced Manufacturing & Engineering (AME) Young Individual Research Grant (YIRG)
- FXJ.L. acknowledges the support from the NRF, Prime Minister's Office, Singapore, under the Competitive Research Program Award (NRF-CRP29-2022-0004), MOE Tier 2 grants (MOE-T2EP10221-0005 and MOE-T2EP10123-0004), Agency for Science, Technology and Research (A*STAR) under MTC Individual Research Grants (Project ID M21K2c0113) and Science and Technology Project of Jiangsu Province (grant number BZ2022056). X.W. acknowledges the support from the National Key R&D Program of China (no. 2022ZD0117501), Agency for Science, Technology and Research (A*STAR) Singapore RIE2020 Advanced Manufacturing and Engineering Programmatic Grant A1898b0043, and Tsinghua University Initiative Scientific Research Program. J.S. acknowledges the support from Agency for Science, Technology and Research (A*STAR) Advanced Manufacturing & Engineering (AME) Young Individual Research Grant (YIRG) A2084c0171. C.Z. acknowledges the support from MOE Tier 2 grants (MOE2019-T2-2-030), and computational resources in NUS High Performance Computing (HPC) facilities and National Supercomputing Centre (NSCC) in Singapore.
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Song, Shaotang; Sole, Andres Pinar; Matej, Adam; Li, Guangwu; Stetsovych, Oleksandr; Soler, Diego; Yang, Huimin; Telychko, Mykola; Li, Jing; Kumar, Manish; Chen, Qifan; Edalatmanesh, Shayan; Brabec, Jiri; Veis, Libor; Wu, Jishan; Jelinek, Pavel; Lu, Jiong Highly entangled polyradical nanographene with coexisting strong correlation and topological frustration NATURE CHEMISTRY, 2024, DOI: 10.1038/s41557-024-01453-9. Abstract | BibTeX | Endnote @article{ISI:001169656100002,
title = {Highly entangled polyradical nanographene with coexisting strong correlation and topological frustration},
author = {Shaotang Song and Andres Pinar Sole and Adam Matej and Guangwu Li and Oleksandr Stetsovych and Diego Soler and Huimin Yang and Mykola Telychko and Jing Li and Manish Kumar and Qifan Chen and Shayan Edalatmanesh and Jiri Brabec and Libor Veis and Jishan Wu and Pavel Jelinek and Jiong Lu},
doi = {10.1038/s41557-024-01453-9},
times_cited = {1},
issn = {1755-4330},
year = {2024},
date = {2024-02-19},
journal = {NATURE CHEMISTRY},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Open-shell nanographenes exhibit unconventional pi-magnetism arising from topological frustration or strong electron-electron interaction. However, conventional design approaches are typically limited to a single magnetic origin, which can restrict the number of correlated spins or the type of magnetic ordering in open-shell nanographenes. Here we present a design strategy that combines topological frustration and electron-electron interactions to fabricate a large fully fused 'butterfly'-shaped tetraradical nanographene on Au(111). We employ bond-resolved scanning tunnelling microscopy and spin-excitation spectroscopy to resolve the molecular backbone and reveal the strongly correlated open-shell character, respectively. This nanographene contains four unpaired electrons with both ferromagnetic and anti-ferromagnetic interactions, harbouring a many-body singlet ground state and strong multi-spin entanglement, which is well described by many-body calculations. Furthermore, we study the magnetic properties and spin states in the nanographene using a nickelocene magnetic probe. The ability to imprint and characterize many-body strongly correlated spins in polyradical nanographenes paves the way for future advancements in quantum information technologies.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Open-shell nanographenes exhibit unconventional pi-magnetism arising from topological frustration or strong electron-electron interaction. However, conventional design approaches are typically limited to a single magnetic origin, which can restrict the number of correlated spins or the type of magnetic ordering in open-shell nanographenes. Here we present a design strategy that combines topological frustration and electron-electron interactions to fabricate a large fully fused 'butterfly'-shaped tetraradical nanographene on Au(111). We employ bond-resolved scanning tunnelling microscopy and spin-excitation spectroscopy to resolve the molecular backbone and reveal the strongly correlated open-shell character, respectively. This nanographene contains four unpaired electrons with both ferromagnetic and anti-ferromagnetic interactions, harbouring a many-body singlet ground state and strong multi-spin entanglement, which is well described by many-body calculations. Furthermore, we study the magnetic properties and spin states in the nanographene using a nickelocene magnetic probe. The ability to imprint and characterize many-body strongly correlated spins in polyradical nanographenes paves the way for future advancements in quantum information technologies. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUSong, ST
Solé, AP
Matej, A
Li, GW
Stetsovych, O
Soler, D
Yang, HM
Telychko, M
Li, J
Kumar, M
Chen, QF
Edalatmanesh, S
Brabec, J
Veis, L
Wu, JS
Jelinek, P
Lu, J
- AFShaotang Song
Andres Pinar Sole
Adam Matej
Guangwu Li
Oleksandr Stetsovych
Diego Soler
Huimin Yang
Mykola Telychko
Jing Li
Manish Kumar
Qifan Chen
Shayan Edalatmanesh
Jiri Brabec
Libor Veis
Jishan Wu
Pavel Jelinek
Jiong Lu
- TIHighly entangled polyradical nanographene with coexisting strong correlation and topological frustration
- SONATURE CHEMISTRY
- LAEnglish
- DTArticle
- IDON-SURFACE SYNTHESIS; SINGLE-MOLECULE; SPIN; STATE
- ABOpen-shell nanographenes exhibit unconventional pi-magnetism arising from topological frustration or strong electron-electron interaction. However, conventional design approaches are typically limited to a single magnetic origin, which can restrict the number of correlated spins or the type of magnetic ordering in open-shell nanographenes. Here we present a design strategy that combines topological frustration and electron-electron interactions to fabricate a large fully fused 'butterfly'-shaped tetraradical nanographene on Au(111). We employ bond-resolved scanning tunnelling microscopy and spin-excitation spectroscopy to resolve the molecular backbone and reveal the strongly correlated open-shell character, respectively. This nanographene contains four unpaired electrons with both ferromagnetic and anti-ferromagnetic interactions, harbouring a many-body singlet ground state and strong multi-spin entanglement, which is well described by many-body calculations. Furthermore, we study the magnetic properties and spin states in the nanographene using a nickelocene magnetic probe. The ability to imprint and characterize many-body strongly correlated spins in polyradical nanographenes paves the way for future advancements in quantum information technologies.
- C1[Song, Shaotang; Li, Guangwu; Yang, Huimin; Telychko, Mykola; Li, Jing; Wu, Jishan; Lu, Jiong] Natl Univ Singapore, Dept Chem, Singapore, Singapore.
[Sole, Andres Pinar; Matej, Adam; Stetsovych, Oleksandr; Soler, Diego; Kumar, Manish; Chen, Qifan; Edalatmanesh, Shayan; Jelinek, Pavel] Czech Acad Sci, Inst Phys, Prague, Czech Republic. [Sole, Andres Pinar; Matej, Adam; Jelinek, Pavel] Palacky Univ Olomouc, Czech Adv Technol & Res Inst, Reg Ctr Adv Technol & Mat, Olomouc, Czech Republic. [Li, Guangwu] Nankai Univ, Coll Elect Informat & Opt Engn, Ctr Single Mol Sci, Frontiers Sci Ctr New Organ Matter,Inst Modern Opt, Tianjin, Peoples R China. [Brabec, Jiri; Veis, Libor] Czech Acad Sci, Dept Theoret Chem, J Heyrovsky Inst Phys Chem, Prague, Czech Republic. [Lu, Jiong] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore. [Lu, Jiong] Natl Univ Singapore, Suzhou Res Inst, Suzhou, Peoples R China - C3National University of Singapore; Czech Academy of Sciences; Institute of Physics of the Czech Academy of Sciences; Palacky University Olomouc; Nankai University; Czech Academy of Sciences; J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; National University of Singapore
- RPWu, JS (corresponding author), Natl Univ Singapore, Dept Chem, Singapore, Singapore; Jelinek, P (corresponding author), Czech Acad Sci, Inst Phys, Prague, Czech Republic; Jelinek, P (corresponding author), Palacky Univ Olomouc, Czech Adv Technol & Res Inst, Reg Ctr Adv Technol & Mat, Olomouc, Czech Republic; Veis, L (corresponding author), Czech Acad Sci, Dept Theoret Chem, J Heyrovsky Inst Phys Chem, Prague, Czech Republic; Lu, J (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Suzhou Res Inst, Suzhou, Peoples R China
- FUAgency for Science, Technology and Research (A*STAR) [MOE T2EP50121-0008, MOE-T2EP10221-0005, MOE-T2EP10123-0004]; Ministry of Education (MOE) [NRF-CRP29-2022-0004]; National Research Foundation (NRF), Prime Minister's Office, Singapore, under the Competitive Research Program Award [715, M21K2c0113]; Agency for Science, Technology and Research (A*STAR) under its Advanced Manufacturing and Engineering Individual Research Grants (AME IRG) [BZ2022056]; Science and Technology Project of Jiangsu Province [LM2023051]; MEYS CR [23-05486 S.]; Grant Agency of Czech Republic (GACR) [A20E5c0089]; A*STAR AME IRG grant [NRF-NRFI05-2019-0005]; NRF Investigatorship award [M22K3c0094]; A*STAR under its AME Young Individual Research Grants (YIRG) grant [LM2015070]; Czech Ministry of Education, Youth and Sports from the Large Infrastructures for Research, Experimental Development and Innovations project 'IT4 Innovations National Supercomputing Center-; Computational Chemical Sciences Program of the US Department of Energy, Office of Science, Basic Energy Science (BES), Chemical Sciences, Geosciences and Biosciences Division in the Center for Scalable and Predictive methods for Excitations
- FXJ. Lu acknowledges the support from Ministry of Education (MOE) grants (MOE T2EP50121-0008, MOE-T2EP10221-0005 and MOE-T2EP10123-0004), and National Research Foundation (NRF), Prime Minister's Office, Singapore, under the Competitive Research Program Award (NRF-CRP29-2022-0004), Agency for Science, Technology and Research (A*STAR) under its Advanced Manufacturing and Engineering Individual Research Grants (AME IRG) grant (project 715 no. M21K2c0113). This work was supported by Science and Technology Project of Jiangsu Province, grant number BZ2022056. We acknowledge support from the CzechNanoLab Research Infrastructure supported by MEYS CR (LM2023051) and the Grant Agency of Czech Republic (GACR) project no. 23-05486 S. J.W. acknowledges the financial support from an A*STAR AME IRG grant (A20E5c0089) and NRF Investigatorship award (NRF-NRFI05-2019-0005). S.S. acknowledges the support from A*STAR under its AME Young Individual Research Grants (YIRG) grant (M22K3c0094). This work was supported by the Czech Ministry of Education, Youth and Sports from the Large Infrastructures for Research, Experimental Development and Innovations project 'IT4 Innovations National Supercomputing Center-LM2015070', and the Computational Chemical Sciences Program of the US Department of Energy, Office of Science, Basic Energy Science (BES), Chemical Sciences, Geosciences and Biosciences Division in the Center for Scalable and Predictive methods for Excitations and Correlated phenomena (SPEC) at Pacific Northwest National Laboratory (PNNL).
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