2024
|
Cheng, Man; Hu, Qifeng; Huang, Yuqiang; Ding, Chenyang; Qiang, Xiao-Bin; Hua, Chenqiang; Fang, Hanyan; Lu, Jiong; Peng, Yuxuan; Yang, Jinbo; Xi, Chuanying; Pi, Li; Watanabe, Kenji; Taniguchi, Takashi; Lu, Hai-Zhou; Novoselov, Kostya S; Lu, Yunhao; Zheng, Yi Quantum tunnelling with tunable spin geometric phases in van der Waals antiferromagnets NATURE PHYSICS, 2024, DOI: 10.1038/s41567-024-02675-x. Abstract | BibTeX | Endnote @article{ISI:001338064100001,
title = {Quantum tunnelling with tunable spin geometric phases in van der Waals antiferromagnets},
author = {Man Cheng and Qifeng Hu and Yuqiang Huang and Chenyang Ding and Xiao-Bin Qiang and Chenqiang Hua and Hanyan Fang and Jiong Lu and Yuxuan Peng and Jinbo Yang and Chuanying Xi and Li Pi and Kenji Watanabe and Takashi Taniguchi and Hai-Zhou Lu and Kostya S Novoselov and Yunhao Lu and Yi Zheng},
doi = {10.1038/s41567-024-02675-x},
times_cited = {0},
issn = {1745-2473},
year = {2024},
date = {2024-10-22},
journal = {NATURE PHYSICS},
publisher = {NATURE PORTFOLIO},
address = {HEIDELBERGER PLATZ 3, BERLIN, 14197, GERMANY},
abstract = {Electron tunnelling in solids, a fundamental quantum phenomenon, lays the foundation for various modern technologies. The emergence of van der Waals magnets presents opportunities for discovering unconventional tunnelling phenomena. Here, we demonstrate quantum tunnelling with tunable spin geometric phases in a multilayer van der Waals antiferromagnet CrPS4. The spin geometric phase of electron tunnelling is controlled by magnetic-field-dependent metamagnetic phase transitions. The square lattice of a CrPS4 monolayer causes strong t2g-orbital delocalization near the conduction band minimum. This creates a one-dimensional spin system with reversed energy ordering between the t2g and eg spin channels, which prohibits both intralayer spin relaxation by means of collective magnon excitations and interlayer spin hopping between the t2g and eg spin channels. The resulting coherent electron transmission shows pronounced tunnel magnetoresistance oscillations, manifesting quantum interference of cyclic quantum evolutions of individual electron Bloch waves by means of the time-reversal symmetrical tunnelling loops. Our results suggest the appearance of Aharonov-Anandan phases that originate from the non-adiabatic generalization of the Berry's phase.},
keywords = {},
pubstate = {published},
tppubtype = {article}
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Electron tunnelling in solids, a fundamental quantum phenomenon, lays the foundation for various modern technologies. The emergence of van der Waals magnets presents opportunities for discovering unconventional tunnelling phenomena. Here, we demonstrate quantum tunnelling with tunable spin geometric phases in a multilayer van der Waals antiferromagnet CrPS4. The spin geometric phase of electron tunnelling is controlled by magnetic-field-dependent metamagnetic phase transitions. The square lattice of a CrPS4 monolayer causes strong t2g-orbital delocalization near the conduction band minimum. This creates a one-dimensional spin system with reversed energy ordering between the t2g and eg spin channels, which prohibits both intralayer spin relaxation by means of collective magnon excitations and interlayer spin hopping between the t2g and eg spin channels. The resulting coherent electron transmission shows pronounced tunnel magnetoresistance oscillations, manifesting quantum interference of cyclic quantum evolutions of individual electron Bloch waves by means of the time-reversal symmetrical tunnelling loops. Our results suggest the appearance of Aharonov-Anandan phases that originate from the non-adiabatic generalization of the Berry's phase. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUCheng, M
Hu, QF
Huang, YQ
Ding, CY
Qiang, XB
Hua, CQ
Fang, HY
Lu, J
Peng, YX
Yang, JB
Xi, CY
Pi, L
Watanabe, K
Taniguchi, T
Lu, HZ
Novoselov, KS
Lu, YH
Zheng, Y
- AFMan Cheng
Qifeng Hu
Yuqiang Huang
Chenyang Ding
Xiao-Bin Qiang
Chenqiang Hua
Hanyan Fang
Jiong Lu
Yuxuan Peng
Jinbo Yang
Chuanying Xi
Li Pi
Kenji Watanabe
Takashi Taniguchi
Hai-Zhou Lu
Kostya S Novoselov
Yunhao Lu
Yi Zheng
- TIQuantum tunnelling with tunable spin geometric phases in van der Waals antiferromagnets
- SONATURE PHYSICS
- LAEnglish
- DTArticle
- IDINTERFERENCE; FERROMAGNETISM
- ABElectron tunnelling in solids, a fundamental quantum phenomenon, lays the foundation for various modern technologies. The emergence of van der Waals magnets presents opportunities for discovering unconventional tunnelling phenomena. Here, we demonstrate quantum tunnelling with tunable spin geometric phases in a multilayer van der Waals antiferromagnet CrPS4. The spin geometric phase of electron tunnelling is controlled by magnetic-field-dependent metamagnetic phase transitions. The square lattice of a CrPS4 monolayer causes strong t2g-orbital delocalization near the conduction band minimum. This creates a one-dimensional spin system with reversed energy ordering between the t2g and eg spin channels, which prohibits both intralayer spin relaxation by means of collective magnon excitations and interlayer spin hopping between the t2g and eg spin channels. The resulting coherent electron transmission shows pronounced tunnel magnetoresistance oscillations, manifesting quantum interference of cyclic quantum evolutions of individual electron Bloch waves by means of the time-reversal symmetrical tunnelling loops. Our results suggest the appearance of Aharonov-Anandan phases that originate from the non-adiabatic generalization of the Berry's phase.
- C1[Cheng, Man; Hu, Qifeng; Huang, Yuqiang; Ding, Chenyang; Hua, Chenqiang; Lu, Yunhao; Zheng, Yi] Zhejiang Univ, Sch Phys, Hangzhou, Peoples R China.
[Cheng, Man; Hu, Qifeng; Huang, Yuqiang; Ding, Chenyang; Hua, Chenqiang; Lu, Yunhao; Zheng, Yi] Zhejiang Univ, State Key Lab Silicon Mat & Adv Semicond Mat, Hangzhou, Peoples R China. [Qiang, Xiao-Bin; Lu, Hai-Zhou] Southern Univ Sci & Technol SUSTech, Shenzhen Inst Quantum Sci & Engn, Shenzhen, Peoples R China. [Qiang, Xiao-Bin; Lu, Hai-Zhou] Southern Univ Sci & Technol SUSTech, Dept Phys, Shenzhen, Peoples R China. [Hua, Chenqiang] Beihang Hangzhou Innovat Inst Yuhang, Hangzhou, Peoples R China. [Fang, Hanyan; Lu, Jiong] Natl Univ Singapore, Dept Chem, Singapore, Singapore. [Fang, Hanyan; Lu, Jiong; Novoselov, Kostya S.] Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore, Singapore. [Peng, Yuxuan; Yang, Jinbo] Peking Univ, Sch Phys, State Key Lab Artificial Microstruct & Mesoscop Ph, Beijing, Peoples R China. [Xi, Chuanying; Pi, Li] Chinese Acad Sci, High Magnet Field Lab, Hefei, Peoples R China. [Watanabe, Kenji; Taniguchi, Takashi] Natl Inst Mat Sci, Tsukuba, Japan. [Novoselov, Kostya S.] Natl Univ Singapore, Coll Design & Engn, Fac Engn, Dept Mat Sci & Engn, Singapore, Singapore - C3Zhejiang University; Zhejiang University; Southern University of Science & Technology; Southern University of Science & Technology; National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); Peking University; Chinese Academy of Sciences; Hefei Institutes of Physical Science, CAS; National Institute for Materials Science; National University of Singapore
- RPLu, YH (corresponding author), Zhejiang Univ, Sch Phys, Hangzhou, Peoples R China; Lu, YH (corresponding author), Zhejiang Univ, State Key Lab Silicon Mat & Adv Semicond Mat, Hangzhou, Peoples R China
- FUNational Natural Science Foundation of China (National Science Foundation of China) [2023YFA1406302]; National Key R&D Programme of the MOST of China [12374194, 12241401]; National Science Foundation of China [D19A040001]; Zhejiang Provincial Natural Science Foundation [2021HSC-UE007]; Users with Excellence Project of Hefei Science Center CAS
- FXThis work was supported by the National Key R&D Programme of the MOST of China (Grant No. 2023YFA1406302 to Y.Z.), the National Science Foundation of China (Grant Nos. 12374194 and 12241401 to Y.Z. and J.B.Y., respectively) and the Zhejiang Provincial Natural Science Foundation (D19A040001 to Y.Z.). Y.Z. acknowledges support from the Users with Excellence Project of Hefei Science Center CAS, 2021HSC-UE007.
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- PUNATURE PORTFOLIO
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- PY2024
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- PG14
- WCPhysics, Multidisciplinary
- SCPhysics
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- EF
|
Cheung, Christopher T S; Goodwin, Zachary A H; Han, Yixuan; Lu, Jiong; Mostofi, Arash A; Lischner, Johannes Coexisting Charge Density Waves in Twisted Bilayer NbSe2 NANO LETTERS, 24 (39), pp. 12088-12094, 2024, DOI: 10.1021/acs.nanolett.4c02750. Abstract | BibTeX | Endnote @article{ISI:001317095600001,
title = {Coexisting Charge Density Waves in Twisted Bilayer NbSe_{2}},
author = {Christopher T S Cheung and Zachary A H Goodwin and Yixuan Han and Jiong Lu and Arash A Mostofi and Johannes Lischner},
doi = {10.1021/acs.nanolett.4c02750},
times_cited = {0},
issn = {1530-6984},
year = {2024},
date = {2024-09-19},
journal = {NANO LETTERS},
volume = {24},
number = {39},
pages = {12088-12094},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {Twisted bilayers of 2D materials have emerged as a tunable platform for studying broken symmetry phases. While most interest has been focused toward emergent states in systems whose constituent monolayers do not feature broken symmetry states, assembling monolayers that exhibit ordered states into twisted bilayers can also give rise to interesting phenomena. Here, we use first-principles density-functional theory calculations to study the atomic structure of twisted bilayer NbSe2 whose constituent monolayers feature a charge density wave. We find that different charge density wave states coexist in the ground state of the twisted bilayer: monolayer-like 3 x 3 triangular and hexagonal charge density waves are observed in low-energy stacking regions, while stripe charge density waves are found in the domain walls surrounding the low-energy stacking regions. These predictions, which can be tested by scanning tunneling microscopy experiments, highlight the potential to create complex charge density wave ground states in twisted bilayer systems.},
keywords = {},
pubstate = {published},
tppubtype = {article}
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Twisted bilayers of 2D materials have emerged as a tunable platform for studying broken symmetry phases. While most interest has been focused toward emergent states in systems whose constituent monolayers do not feature broken symmetry states, assembling monolayers that exhibit ordered states into twisted bilayers can also give rise to interesting phenomena. Here, we use first-principles density-functional theory calculations to study the atomic structure of twisted bilayer NbSe2 whose constituent monolayers feature a charge density wave. We find that different charge density wave states coexist in the ground state of the twisted bilayer: monolayer-like 3 x 3 triangular and hexagonal charge density waves are observed in low-energy stacking regions, while stripe charge density waves are found in the domain walls surrounding the low-energy stacking regions. These predictions, which can be tested by scanning tunneling microscopy experiments, highlight the potential to create complex charge density wave ground states in twisted bilayer systems. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AUCheung, CTS
Goodwin, ZAH
Han, YX
Lu, J
Mostofi, AA
Lischner, J
- AFChristopher T S Cheung
Zachary A H Goodwin
Yixuan Han
Jiong Lu
Arash A Mostofi
Johannes Lischner
- TICoexisting Charge Density Waves in Twisted Bilayer NbSe2
- SONANO LETTERS
- LAEnglish
- DTArticle
- DECharge Density Waves; Twistronics; First-principlessimulation; 2D Materials
- IDTRANSITION; SUPERCONDUCTIVITY; PHASES
- ABTwisted bilayers of 2D materials have emerged as a tunable platform for studying broken symmetry phases. While most interest has been focused toward emergent states in systems whose constituent monolayers do not feature broken symmetry states, assembling monolayers that exhibit ordered states into twisted bilayers can also give rise to interesting phenomena. Here, we use first-principles density-functional theory calculations to study the atomic structure of twisted bilayer NbSe2 whose constituent monolayers feature a charge density wave. We find that different charge density wave states coexist in the ground state of the twisted bilayer: monolayer-like 3 x 3 triangular and hexagonal charge density waves are observed in low-energy stacking regions, while stripe charge density waves are found in the domain walls surrounding the low-energy stacking regions. These predictions, which can be tested by scanning tunneling microscopy experiments, highlight the potential to create complex charge density wave ground states in twisted bilayer systems.
- C3Imperial College London; Imperial College London; Imperial College London; Harvard University; Institute for Functional Intelligent Materials (I-FIM); National University of Singapore
- RPLischner, J (corresponding author), Imperial Coll London, Dept Phys, London SW7 2AZ, England; Lischner, J (corresponding author), Imperial Coll London, Dept Mat, London SW7 2AZ, England; Lischner, J (corresponding author), Imperial Coll London, Thomas Young Ctr Theory & Simulat Mat, London SW7 2AZ, England
- FXWe thank Adolfo Fumega for useful discussions. C.T.S.C. acknowledges funding from the Croucher Foundation and an Imperial College President's Scholarship. This work used the ARCHER2 UK National Supercomputing Service (https://www.archer2.ac.uk) and the Imperial College Research Computing Service facility CX1 (DOI: 10.14469/hpc/2232). We acknowledge the Thomas Young Centre under Grant No. TYC-101.
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- PY2024
- VL24
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- EP12094
- DI10.1021/acs.nanolett.4c02750
- PG7
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- SCChemistry; Science & Technology - Other Topics; Materials Science; Physics
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- EF
|
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.},
keywords = {},
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
- VR1.0
- PTJ
- AUQiu, ZZ
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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- PIWASHINGTON
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- PY2024
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- BP24035
- EP24043
- DI10.1021/acsnano.4c03640
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- SCChemistry; Science & Technology - Other Topics; Materials Science
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|
Lyu, Pin; Wang, Ziying; Guo, Na; Su, Jie; Li, Jing; Qi, Dongchen; Xi, Shibo; Lin, Huihui; Zhang, Qihan; Pennycook, Stephen J; Chen, Jingsheng; Zhao, Xiaoxu; Zhang, Chun; Loh, Kian Ping; Lu, Jiong Air-Stable Wafer-Scale Ferromagnetic Metallo-Carbon Nitride Monolayer JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 146 (30), pp. 20604-20614, 2024, DOI: 10.1021/jacs.4c02160. Abstract | BibTeX | Endnote @article{ISI:001272808300001,
title = {Air-Stable Wafer-Scale Ferromagnetic Metallo-Carbon Nitride Monolayer},
author = {Pin Lyu and Ziying Wang and Na Guo and Jie Su and Jing Li and Dongchen Qi and Shibo Xi and Huihui Lin and Qihan Zhang and Stephen J Pennycook and Jingsheng Chen and Xiaoxu Zhao and Chun Zhang and Kian Ping Loh and Jiong Lu},
doi = {10.1021/jacs.4c02160},
times_cited = {0},
issn = {0002-7863},
year = {2024},
date = {2024-07-18},
journal = {JOURNAL OF THE AMERICAN CHEMICAL SOCIETY},
volume = {146},
number = {30},
pages = {20604-20614},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
abstract = {The pursuit of robust, long-range magnetic ordering in two-dimensional (2D) materials holds immense promise for driving technological advances. However, achieving this goal remains a grand challenge due to enhanced quantum and thermal fluctuations as well as chemical instability in the 2D limit. While magnetic ordering has been realized in atomically thin flakes of transition metal chalcogenides and metal halides, these materials often suffer from air instability. In contrast, 2D carbon-based materials are stable enough, yet the challenge lies in creating a high density of local magnetic moments and controlling their long-range magnetic ordering. Here, we report a novel wafer-scale synthesis of an air-stable metallo-carbon nitride monolayer (MCN, denoted as MN4/CNx), featuring ultradense single magnetic atoms and exhibiting robust room-temperature ferromagnetism. Under low-pressure chemical vapor deposition conditions, thermal dehydrogenation and polymerization of metal phthalocyanine (MPc) on copper foil at elevated temperature generate a substantial number of nitrogen coordination sites for anchoring magnetic single atoms in monolayer MN4/CNx (where M = Fe, Co, and Ni). The incorporation of densely populating MN4 sites into monolayer MCN networks leads to robust ferromagnetism up to room temperature, enabling the observation of anomalous Hall effects with excellent chemical stability. Detailed electronic structure calculations indicate that the presence of high-density metal sites results in the emergence of spin-split d-bands near the Fermi level, causing a favorable long-range ferromagnetic exchange coupling through direct exchange interactions. Our work demonstrates a novel synthesis approach for wafer-scale MCN monolayers with robust room-temperature ferromagnetism and may shed light on practical electronic and spintronic applications.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The pursuit of robust, long-range magnetic ordering in two-dimensional (2D) materials holds immense promise for driving technological advances. However, achieving this goal remains a grand challenge due to enhanced quantum and thermal fluctuations as well as chemical instability in the 2D limit. While magnetic ordering has been realized in atomically thin flakes of transition metal chalcogenides and metal halides, these materials often suffer from air instability. In contrast, 2D carbon-based materials are stable enough, yet the challenge lies in creating a high density of local magnetic moments and controlling their long-range magnetic ordering. Here, we report a novel wafer-scale synthesis of an air-stable metallo-carbon nitride monolayer (MCN, denoted as MN4/CNx), featuring ultradense single magnetic atoms and exhibiting robust room-temperature ferromagnetism. Under low-pressure chemical vapor deposition conditions, thermal dehydrogenation and polymerization of metal phthalocyanine (MPc) on copper foil at elevated temperature generate a substantial number of nitrogen coordination sites for anchoring magnetic single atoms in monolayer MN4/CNx (where M = Fe, Co, and Ni). The incorporation of densely populating MN4 sites into monolayer MCN networks leads to robust ferromagnetism up to room temperature, enabling the observation of anomalous Hall effects with excellent chemical stability. Detailed electronic structure calculations indicate that the presence of high-density metal sites results in the emergence of spin-split d-bands near the Fermi level, causing a favorable long-range ferromagnetic exchange coupling through direct exchange interactions. Our work demonstrates a novel synthesis approach for wafer-scale MCN monolayers with robust room-temperature ferromagnetism and may shed light on practical electronic and spintronic applications. - FNClarivate Analytics Web of Science
- VR1.0
- PTJ
- AULyu, P
Wang, ZY
Guo, N
Su, J
Li, J
Qi, DC
Xi, SB
Lin, HH
Zhang, QH
Pennycook, SJ
Chen, JS
Zhao, XX
Zhang, C
Loh, KP
Lu, J
- AFPin Lyu
Ziying Wang
Na Guo
Jie Su
Jing Li
Dongchen Qi
Shibo Xi
Huihui Lin
Qihan Zhang
Stephen J Pennycook
Jingsheng Chen
Xiaoxu Zhao
Chun Zhang
Kian Ping Loh
Jiong Lu
- TIAir-Stable Wafer-Scale Ferromagnetic Metallo-Carbon Nitride Monolayer
- SOJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- LAEnglish
- DTArticle
- ABThe pursuit of robust, long-range magnetic ordering in two-dimensional (2D) materials holds immense promise for driving technological advances. However, achieving this goal remains a grand challenge due to enhanced quantum and thermal fluctuations as well as chemical instability in the 2D limit. While magnetic ordering has been realized in atomically thin flakes of transition metal chalcogenides and metal halides, these materials often suffer from air instability. In contrast, 2D carbon-based materials are stable enough, yet the challenge lies in creating a high density of local magnetic moments and controlling their long-range magnetic ordering. Here, we report a novel wafer-scale synthesis of an air-stable metallo-carbon nitride monolayer (MCN, denoted as MN4/CNx), featuring ultradense single magnetic atoms and exhibiting robust room-temperature ferromagnetism. Under low-pressure chemical vapor deposition conditions, thermal dehydrogenation and polymerization of metal phthalocyanine (MPc) on copper foil at elevated temperature generate a substantial number of nitrogen coordination sites for anchoring magnetic single atoms in monolayer MN4/CNx (where M = Fe, Co, and Ni). The incorporation of densely populating MN4 sites into monolayer MCN networks leads to robust ferromagnetism up to room temperature, enabling the observation of anomalous Hall effects with excellent chemical stability. Detailed electronic structure calculations indicate that the presence of high-density metal sites results in the emergence of spin-split d-bands near the Fermi level, causing a favorable long-range ferromagnetic exchange coupling through direct exchange interactions. Our work demonstrates a novel synthesis approach for wafer-scale MCN monolayers with robust room-temperature ferromagnetism and may shed light on practical electronic and spintronic applications.
- C3National University of Singapore; Nanjing University of Aeronautics & Astronautics; Nanjing University of Aeronautics & Astronautics; National University of Singapore; National University of Singapore; National University of Singapore; Queensland University of Technology (QUT); Agency for Science Technology & Research (A*STAR); A*STAR - Institute of Sustainability for Chemicals, Energy & Environment (ISCE2); National University of Singapore; National University of Singapore; Institute for Functional Intelligent Materials (I-FIM); Beihang University; Peking University
- RPZhang, C (corresponding author), Natl Univ Singapore, Dept Chem, Singapore 117543, Singapore; Zhang, C (corresponding author), Natl Univ Singapore, Chongqing Res Inst, Chongqing 401123, Peoples R China; Zhang, C (corresponding author), Natl Univ Singapore, Dept Phys, Singapore 117551, Singapore; Zhang, C (corresponding author), Natl Univ Singapore, Ctr Adv Mat 2D, Singapore 117551, Singapore; Lu, J (corresponding author), Natl Univ Singapore, Inst Funct Intelligent Mat, Singapore 117544, Singapore; Li, J (corresponding author), Beihang Univ, Sch Chem, Key Lab Bioinspired Smart Interfacial Sci & Techn, Minist Educ, Beijing 100191, Peoples R China; Zhao, XX (corresponding author), Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China
- FXJ.L. acknowledges the support from MOE grants (MOE T2EP50121-0008, 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). C.Z. thanks the support from the NUS academic research grant (R-144-000-410-114). X.Z. and S.J.P. acknowledge support from the MOE grant (MOE2017-T2-2-139). D.Q. acknowledges the support of the Australian Research Council (Grant no. FT160100207). J.L. thanks the support from the National Natural Science Foundation of China (22272004) and the Fundamental Research Funds for the Central Universities (YWF-22-L-1256). X.Z. acknowledges the support from the Fundamental Research Funds for the Central Universities and the Beijing Natural Science Foundation (Grant no. Z220020). J.S. acknowledges the support from the Agency for Science, Technology and Research (A*STAR) Advanced Manufacturing & Engineering (AME) Young Individual Research Grant (YIRG) A2084c0171. Computations were done with the NUS High Performance Computing (HPC) facilities and the National Supercomputing Centre (NSCC) in Singapore. Part of this research was undertaken on the soft X-ray spectroscopy beamline at the Australian Synchrotron, part of ANSTO.
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- PDJUL 18
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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, 23 (8), 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 = {1},
issn = {1476-1122},
year = {2024},
date = {2024-06-03},
journal = {NATURE MATERIALS},
volume = {23},
number = {8},
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.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
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 - C3Institute for Functional Intelligent Materials (I-FIM); National University of Singapore; 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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- DI10.1038/s41563-024-01910-3
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