Two-dimensional inorganic molecular crystals

Han, Wei; Huang, Pu; Li, Liang; Wang, Fakun; Luo, Peng; Liu, Kailang; Zhou, Xing; Li, Huiqiao; Zhang, Xiuwen; Cui, Yi; Zhai, Tianyou

doi:10.1038/s41467-019-12569-9

Title: Two-dimensional inorganic molecular crystals

Journal Article · 17 October 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-12569-9 · OSTI ID:1575222

Han, Wei ^[1]; Huang, Pu ^[2]; Li, Liang ^[1]; Wang, Fakun ^[1]; Luo, Peng ^[1]; Liu, Kailang ^[1]; Zhou, Xing ^[1];

^[3]; Zhang, Xiuwen ^[2];

^[4];

^[1]

Huazhong Univ. of Science and Technology (HUST), Wuhan (China). State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering
Shenzhen Univ., Guangdong (China). Shenzhen Key Lab. of Flexible Memory Materials and Devices, College of Electronic Science and Technology
Huazhong Univ. of Science and Technology (HUST), Wuhan (China). State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering; Stanford Univ., Stanford, CA (United States). Dept. of Material Science and Engineering
Stanford Univ., Stanford, CA (United States). Dept. of Material Science and Engineering

Two-dimensional molecular crystals, consisting of zero-dimensional molecules, are very appealing due to their novel physical properties. However, they are mostly limited to organic molecules. The synthesis of inorganic version of two-dimensional molecular crystals is still a challenge due to the difficulties in controlling the crystal phase and growth plane. Here, we design a passivator-assisted vapor deposition method for the growth of two-dimensional Sb₂O₃ inorganic molecular crystals as thin as monolayer. The passivator can prevent the heterophase nucleation and suppress the growth of low-energy planes, and enable the molecule-by-molecule lateral growth along high-energy planes. Using Raman spectroscopy and in situ transmission electron microscopy, we show that the insulating α-phase of Sb₂O₃ flakes can be transformed into semiconducting β-phase under heat and electron-beam irradiation. Our findings can be extended to the controlled growth of other two-dimensional inorganic molecular crystals and open up opportunities for potential molecular electronic devices.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1575222

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (78)

From Bulk to Monolayer MoS2: Evolution of Raman Scattering Li, Hong; Zhang, Qing; Yap, Chin Chong Ray Advanced Functional Materials, Vol. 22, Issue 7 https://doi.org/10.1002/adfm.201102111	journal	January 2012
Preparation of Single-Crystalline Heterojunctions for Organic Electronics Wu, Jiake; Li, Qinfen; Xue, Guobiao Advanced Materials, Vol. 29, Issue 14 https://doi.org/10.1002/adma.201606101	journal	February 2017
Two-Dimensional Fullerene Assembly from an Exfoliated van der Waals Template Lee, Kihong; Choi, Bonnie; Plante, Ilan Jen-La Angewandte Chemie International Edition, Vol. 57, Issue 21 https://doi.org/10.1002/anie.201800953	journal	April 2018
Raman scattering, luminescence, and absorption edge under hydrostatic pressures of layered BiI3 and SbI3 Saitoh, A. Journal of Raman Spectroscopy, Vol. 38, Issue 5 https://doi.org/10.1002/jrs.1676	journal	January 2007
Vibrational spectroscopic and quantum chemical study of antimony(III) oxide Voit, E. I.; Panasenko, A. E.; Zemnukhova, L. A. Journal of Structural Chemistry, Vol. 50, Issue 1 https://doi.org/10.1007/s10947-009-0008-0	journal	February 2009
Strong In-Plane Anisotropies of Optical and Electrical Response in Layered Dimetal Chalcogenide Li, Liang; Gong, Penglai; Wang, Weike ACS Nano, Vol. 11, Issue 10 https://doi.org/10.1021/acsnano.7b04860	journal	September 2017
Halide-Induced Self-Limited Growth of Ultrathin Nonlayered Ge Flakes for High-Performance Phototransistors Hu, Xiaozong; Huang, Pu; Jin, Bao Journal of the American Chemical Society, Vol. 140, Issue 40 https://doi.org/10.1021/jacs.8b07383	journal	September 2018
Electronic Structures of Antimony Oxides Allen, Jeremy P.; Carey, John J.; Walsh, Aron The Journal of Physical Chemistry C, Vol. 117, Issue 28 https://doi.org/10.1021/jp4026249	journal	July 2013
Cluster-Assembled Materials Claridge, Shelley A.; Castleman, A. W.; Khanna, Shiv N. ACS Nano, Vol. 3, Issue 2 https://doi.org/10.1021/nn800820e	journal	January 2009
Bottom-up organic integrated circuits Smits, Edsger C. P.; Mathijssen, Simon G. J.; van Hal, Paul A. Nature, Vol. 455, Issue 7215 https://doi.org/10.1038/nature07320	journal	October 2008
One-pot growth of two-dimensional lateral heterostructures via sequential edge-epitaxy Sahoo, Prasana K.; Memaran, Shahriar; Xin, Yan Nature, Vol. 553, Issue 7686 https://doi.org/10.1038/nature25155	journal	January 2018
Two-dimensional quasi-freestanding molecular crystals for high-performance organic field-effect transistors He, Daowei; Zhang, Yuhan; Wu, Qisheng Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6162	journal	October 2014
Orientational order controls crystalline and amorphous thermal transport in superatomic crystals Ong, Wee-Liat; O’Brien, Evan S.; Dougherty, Patrick S. M. Nature Materials, Vol. 16, Issue 1 https://doi.org/10.1038/nmat4739	journal	September 2016
Activating the molecular spinterface Cinchetti, Mirko; Dediu, V. Alek; Hueso, Luis E. Nature Materials, Vol. 16, Issue 5 https://doi.org/10.1038/nmat4902	journal	April 2017
Sub-nanometre channels embedded in two-dimensional materials Han, Yimo; Li, Ming-Yang; Jung, Gang-Seob Nature Materials, Vol. 17, Issue 2 https://doi.org/10.1038/nmat5038	journal	December 2017
Transforming C60 molecules into graphene quantum dots Lu, Jiong; Yeo, Pei Shan Emmeline; Gan, Chee Kwan Nature Nanotechnology, Vol. 6, Issue 4 https://doi.org/10.1038/nnano.2011.30	journal	March 2011
Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2 Lin, Yung-Chang; Dumcenco, Dumitru O.; Huang, Ying-Sheng Nature Nanotechnology, Vol. 9, Issue 5 https://doi.org/10.1038/nnano.2014.64	journal	April 2014
Room-temperature current blockade in atomically defined single-cluster junctions Lovat, Giacomo; Choi, Bonnie; Paley, Daniel W. Nature Nanotechnology, Vol. 12, Issue 11 https://doi.org/10.1038/nnano.2017.156	journal	August 2017
Vapour–liquid–solid growth of monolayer MoS2 nanoribbons Li, Shisheng; Lin, Yung-Chang; Zhao, Wen Nature Materials, Vol. 17, Issue 6 https://doi.org/10.1038/s41563-018-0055-z	journal	April 2018
Humidity-controlled rectification switching in ruthenium-complex molecular junctions Atesci, Huseyin; Kaliginedi, Veerabhadrarao; Celis Gil, Jose A. Nature Nanotechnology, Vol. 13, Issue 2 https://doi.org/10.1038/s41565-017-0016-8	journal	December 2017
Peltier cooling in molecular junctions Cui, Longji; Miao, Ruijiao; Wang, Kun Nature Nanotechnology, Vol. 13, Issue 2 https://doi.org/10.1038/s41565-017-0020-z	journal	December 2017
A library of atomically thin metal chalcogenides Zhou, Jiadong; Lin, Junhao; Huang, Xiangwei Nature, Vol. 556, Issue 7701 https://doi.org/10.1038/s41586-018-0008-3	journal	April 2018
Definition of a Transcendental Order Parameter for Reconstructive Phase Transitions Dmitriev, V. P.; Rochal, S. B.; Gufan, Yu. M. Physical Review Letters, Vol. 60, Issue 19 https://doi.org/10.1103/physrevlett.60.1958	journal	May 1988
Molecular behavior of zero-dimensional perovskites Yin, Jun; Maity, Partha; De Bastiani, Michele Science Advances, Vol. 3, Issue 12 https://doi.org/10.1126/sciadv.1701793	journal	December 2017
A molecular spin-photovoltaic device Sun, Xiangnan; Vélez, Saül; Atxabal, Ainhoa Science, Vol. 357, Issue 6352 https://doi.org/10.1126/science.aan5348	journal	August 2017
Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices Zhang, Zhengwei; Chen, Peng; Duan, Xidong Science, Vol. 357, Issue 6353 https://doi.org/10.1126/science.aan6814	journal	August 2017
Theoretical analysis of doped graphene as cathode catalyst in Li-O2 and Na-O2 batteries -- the impact of the computational scheme Novčić, Katarina A.; Dobrota, Ana S.; Petković, Milena arXiv https://doi.org/10.48550/arxiv.2006.12912	preprint	January 2020
From Bulk to Monolayer MoS2: Evolution of Raman Scattering Li, Hong; Zhang, Qing; Yap, Chin Chong Ray Advanced Functional Materials, Vol. 22, Issue 7 https://doi.org/10.1002/adfm.201102111	journal	January 2012
Self-Limited Epitaxial Growth of Ultrathin Nonlayered CdS Flakes for High-Performance Photodetectors Jin, Bao; Huang, Pu; Zhang, Qi Advanced Functional Materials, Vol. 28, Issue 20 https://doi.org/10.1002/adfm.201800181	journal	March 2018
Preparation of Single-Crystalline Heterojunctions for Organic Electronics Wu, Jiake; Li, Qinfen; Xue, Guobiao Advanced Materials, Vol. 29, Issue 14 https://doi.org/10.1002/adma.201606101	journal	February 2017
Two‐Dimensional Fullerene Assembly from an Exfoliated van der Waals Template Lee, Kihong; Choi, Bonnie; Plante, Ilan Jen‐La Angewandte Chemie, Vol. 130, Issue 21 https://doi.org/10.1002/ange.201800953	journal	April 2018
Two-Dimensional Fullerene Assembly from an Exfoliated van der Waals Template Lee, Kihong; Choi, Bonnie; Plante, Ilan Jen-La Angewandte Chemie International Edition, Vol. 57, Issue 21 https://doi.org/10.1002/anie.201800953	journal	April 2018
Raman scattering, luminescence, and absorption edge under hydrostatic pressures of layered BiI3 and SbI3 Saitoh, A. Journal of Raman Spectroscopy, Vol. 38, Issue 5 https://doi.org/10.1002/jrs.1676	journal	January 2007
Vibrational spectroscopic and quantum chemical study of antimony(III) oxide Voit, E. I.; Panasenko, A. E.; Zemnukhova, L. A. Journal of Structural Chemistry, Vol. 50, Issue 1 https://doi.org/10.1007/s10947-009-0008-0	journal	February 2009
Synthesis and purple-blue emission of antimony trioxide single-crystalline nanobelts with elliptical cross section Deng, Zhengtao; Chen, Dong; Tang, Fangqiong Nano Research, Vol. 2, Issue 2 https://doi.org/10.1007/s12274-009-9014-y	journal	February 2009
Parallel Nanoimprint Forming of One-Dimensional Chiral Semiconductor for Strain-Engineered Optical Properties Wang, Yixiu; Jin, Shengyu; Wang, Qingxiao Nano-Micro Letters, Vol. 12, Issue 1 https://doi.org/10.1007/s40820-020-00493-3	journal	August 2020
Thermal behaviour of chlorine-antimony fire-retardant systems Costa, L.; Goberti, P.; Paganetto, G. Polymer Degradation and Stability, Vol. 30, Issue 1 https://doi.org/10.1016/0141-3910(90)90114-M	journal	January 1990
Thermal phase transitions in antimony (III) oxides Orman, R. G.; Holland, D. Journal of Solid State Chemistry, Vol. 180, Issue 9 https://doi.org/10.1016/j.jssc.2007.07.004	journal	September 2007
The electronic structure of the antimony chalcogenide series: Prospects for optoelectronic applications Carey, John J.; Allen, Jeremy P.; Scanlon, David O. Journal of Solid State Chemistry, Vol. 213 https://doi.org/10.1016/j.jssc.2014.02.014	journal	May 2014
Strong In-Plane Anisotropies of Optical and Electrical Response in Layered Dimetal Chalcogenide Li, Liang; Gong, Penglai; Wang, Weike ACS Nano, Vol. 11, Issue 10 https://doi.org/10.1021/acsnano.7b04860	journal	September 2017
Halide-Induced Self-Limited Growth of Ultrathin Nonlayered Ge Flakes for High-Performance Phototransistors Hu, Xiaozong; Huang, Pu; Jin, Bao Journal of the American Chemical Society, Vol. 140, Issue 40 https://doi.org/10.1021/jacs.8b07383	journal	September 2018
Electronic Structures of Antimony Oxides Allen, Jeremy P.; Carey, John J.; Walsh, Aron The Journal of Physical Chemistry C, Vol. 117, Issue 28 https://doi.org/10.1021/jp4026249	journal	July 2013
Cluster-Assembled Materials Claridge, Shelley A.; Castleman, A. W.; Khanna, Shiv N. ACS Nano, Vol. 3, Issue 2 https://doi.org/10.1021/nn800820e	journal	January 2009
Bottom-up organic integrated circuits Smits, Edsger C. P.; Mathijssen, Simon G. J.; van Hal, Paul A. Nature, Vol. 455, Issue 7215 https://doi.org/10.1038/nature07320	journal	October 2008
Structural phase transition in monolayer MoTe2 driven by electrostatic doping Wang, Ying; Xiao, Jun; Zhu, Hanyu Nature, Vol. 550, Issue 7677 https://doi.org/10.1038/nature24043	journal	October 2017
One-pot growth of two-dimensional lateral heterostructures via sequential edge-epitaxy Sahoo, Prasana K.; Memaran, Shahriar; Xin, Yan Nature, Vol. 553, Issue 7686 https://doi.org/10.1038/nature25155	journal	January 2018
Two-dimensional quasi-freestanding molecular crystals for high-performance organic field-effect transistors He, Daowei; Zhang, Yuhan; Wu, Qisheng Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6162	journal	October 2014
Orientational order controls crystalline and amorphous thermal transport in superatomic crystals Ong, Wee-Liat; O’Brien, Evan S.; Dougherty, Patrick S. M. Nature Materials, Vol. 16, Issue 1 https://doi.org/10.1038/nmat4739	journal	September 2016
Activating the molecular spinterface Cinchetti, Mirko; Dediu, V. Alek; Hueso, Luis E. Nature Materials, Vol. 16, Issue 5 https://doi.org/10.1038/nmat4902	journal	April 2017
Sub-nanometre channels embedded in two-dimensional materials Han, Yimo; Li, Ming-Yang; Jung, Gang-Seob Nature Materials, Vol. 17, Issue 2 https://doi.org/10.1038/nmat5038	journal	December 2017
Transforming C60 molecules into graphene quantum dots Lu, Jiong; Yeo, Pei Shan Emmeline; Gan, Chee Kwan Nature Nanotechnology, Vol. 6, Issue 4 https://doi.org/10.1038/nnano.2011.30	journal	March 2011
Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2 Lin, Yung-Chang; Dumcenco, Dumitru O.; Huang, Ying-Sheng Nature Nanotechnology, Vol. 9, Issue 5 https://doi.org/10.1038/nnano.2014.64	journal	April 2014
Molecular diodes with rectification ratios exceeding 105 driven by electrostatic interactions Chen, Xiaoping; Roemer, Max; Yuan, Li Nature Nanotechnology, Vol. 12, Issue 8 https://doi.org/10.1038/nnano.2017.110	journal	July 2017
Breaking the Landauer limit Clement, Nicolas; Fujiwara, Akira Nature Nanotechnology, Vol. 12, Issue 8 https://doi.org/10.1038/nnano.2017.123	journal	July 2017
Room-temperature current blockade in atomically defined single-cluster junctions Lovat, Giacomo; Choi, Bonnie; Paley, Daniel W. Nature Nanotechnology, Vol. 12, Issue 11 https://doi.org/10.1038/nnano.2017.156	journal	August 2017
Evolutionary selection growth of two-dimensional materials on polycrystalline substrates Vlassiouk, Ivan V.; Stehle, Yijing; Pudasaini, Pushpa Raj Nature Materials, Vol. 17, Issue 4 https://doi.org/10.1038/s41563-018-0019-3	journal	March 2018
Vapour–liquid–solid growth of monolayer MoS2 nanoribbons Li, Shisheng; Lin, Yung-Chang; Zhao, Wen Nature Materials, Vol. 17, Issue 6 https://doi.org/10.1038/s41563-018-0055-z	journal	April 2018
Phase-selective synthesis of 1T′ MoS2 monolayers and heterophase bilayers Liu, Lina; Wu, Juanxia; Wu, Liyuan Nature Materials, Vol. 17, Issue 12 https://doi.org/10.1038/s41563-018-0187-1	journal	October 2018
Humidity-controlled rectification switching in ruthenium-complex molecular junctions Atesci, Huseyin; Kaliginedi, Veerabhadrarao; Celis Gil, Jose A. Nature Nanotechnology, Vol. 13, Issue 2 https://doi.org/10.1038/s41565-017-0016-8	journal	December 2017
Peltier cooling in molecular junctions Cui, Longji; Miao, Ruijiao; Wang, Kun Nature Nanotechnology, Vol. 13, Issue 2 https://doi.org/10.1038/s41565-017-0020-z	journal	December 2017
A library of atomically thin metal chalcogenides Zhou, Jiadong; Lin, Junhao; Huang, Xiangwei Nature, Vol. 556, Issue 7701 https://doi.org/10.1038/s41586-018-0008-3	journal	April 2018
Lead palladium titanate: A room temperature nanoscale multiferroic thin film Mishra, K. K.; Instan, Alvaro A.; Kumari, Shalini Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-59961-w	journal	February 2020
Chemical accuracy for the van der Waals density functional Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Journal of Physics: Condensed Matter, Vol. 22, Issue 2 https://doi.org/10.1088/0953-8984/22/2/022201	journal	December 2009
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Van der Waals density functionals applied to solids Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Physical Review B, Vol. 83, Issue 19 https://doi.org/10.1103/PhysRevB.83.195131	journal	May 2011
Structural and vibrational study of cubic Sb 2 O 3 under high pressure Pereira, A. L. J.; Gracia, L.; Santamaría-Pérez, D. Physical Review B, Vol. 85, Issue 17 https://doi.org/10.1103/PhysRevB.85.174108	journal	May 2012
Definition of a Transcendental Order Parameter for Reconstructive Phase Transitions Dmitriev, V. P.; Rochal, S. B.; Gufan, Yu. M. Physical Review Letters, Vol. 60, Issue 19 https://doi.org/10.1103/PhysRevLett.60.1958	journal	May 1988
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Refinement of the crystal structure of cubic antimony trioxide, Sb ₂ O ₃ Svensson, C. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 31, Issue 8 https://doi.org/10.1107/S0567740875006759	journal	August 1975
Molecular behavior of zero-dimensional perovskites Yin, Jun; Maity, Partha; De Bastiani, Michele Science Advances, Vol. 3, Issue 12 https://doi.org/10.1126/sciadv.1701793	journal	December 2017
A molecular spin-photovoltaic device Sun, Xiangnan; Vélez, Saül; Atxabal, Ainhoa Science, Vol. 357, Issue 6352 https://doi.org/10.1126/science.aan5348	journal	August 2017
Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices Zhang, Zhengwei; Chen, Peng; Duan, Xidong Science, Vol. 357, Issue 6353 https://doi.org/10.1126/science.aan6814	journal	August 2017
Chemical accuracy for the van der Waals density functional Klimes, J.; Bowler, D. R.; Michaelides, A. arXiv https://doi.org/10.48550/arxiv.0910.0438	preprint	January 2009
Van der Waals density functionals applied to solids Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos arXiv https://doi.org/10.48550/arxiv.1102.1358	text	January 2011
Two-dimensional Quasi-Freestanding Molecular Crystals for High-Performance Organic Field-Effect Transistors He, Daowei; Zhang, Yuhan; Wu, Qisheng arXiv https://doi.org/10.48550/arxiv.1408.6612	text	January 2014
Sub-Nanometer Channels Embedded in Two-Dimensional Materials Han, Yimo; Li, Ming-Yang; Jung, Gang-Seob arXiv https://doi.org/10.48550/arxiv.1707.09880	text	January 2017

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