Two-dimensional inorganic molecular crystals
Abstract
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.
- Authors:
-
[3];
[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
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1575222
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Han, Wei, Huang, Pu, Li, Liang, Wang, Fakun, Luo, Peng, Liu, Kailang, Zhou, Xing, Li, Huiqiao, Zhang, Xiuwen, Cui, Yi, and Zhai, Tianyou. Two-dimensional inorganic molecular crystals. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-12569-9.
Han, Wei, Huang, Pu, Li, Liang, Wang, Fakun, Luo, Peng, Liu, Kailang, Zhou, Xing, Li, Huiqiao, Zhang, Xiuwen, Cui, Yi, & Zhai, Tianyou. Two-dimensional inorganic molecular crystals. United States. https://doi.org/10.1038/s41467-019-12569-9
Han, Wei, Huang, Pu, Li, Liang, Wang, Fakun, Luo, Peng, Liu, Kailang, Zhou, Xing, Li, Huiqiao, Zhang, Xiuwen, Cui, Yi, and Zhai, Tianyou. Thu .
"Two-dimensional inorganic molecular crystals". United States. https://doi.org/10.1038/s41467-019-12569-9. https://www.osti.gov/servlets/purl/1575222.
@article{osti_1575222,
title = {Two-dimensional inorganic molecular crystals},
author = {Han, Wei and Huang, Pu and Li, Liang and Wang, Fakun and Luo, Peng and Liu, Kailang and Zhou, Xing and Li, Huiqiao and Zhang, Xiuwen and Cui, Yi and Zhai, Tianyou},
abstractNote = {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.},
doi = {10.1038/s41467-019-12569-9},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Thu Oct 17 00:00:00 EDT 2019},
month = {Thu Oct 17 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 68 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Self-Limited Epitaxial Growth of Ultrathin Nonlayered CdS Flakes for High-Performance Photodetectors
journal, March 2018
- Jin, Bao; Huang, Pu; Zhang, Qi
- Advanced Functional Materials, Vol. 28, Issue 20
Structural phase transition in monolayer MoTe2 driven by electrostatic doping
journal, October 2017
- Wang, Ying; Xiao, Jun; Zhu, Hanyu
- Nature, Vol. 550, Issue 7677
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Molecular behavior of zero-dimensional perovskites
journal, December 2017
- Yin, Jun; Maity, Partha; De Bastiani, Michele
- Science Advances, Vol. 3, Issue 12
Thermal phase transitions in antimony (III) oxides
journal, September 2007
- Orman, R. G.; Holland, D.
- Journal of Solid State Chemistry, Vol. 180, Issue 9
One-pot growth of two-dimensional lateral heterostructures via sequential edge-epitaxy
journal, January 2018
- Sahoo, Prasana K.; Memaran, Shahriar; Xin, Yan
- Nature, Vol. 553, Issue 7686
Electronic Structures of Antimony Oxides
journal, July 2013
- Allen, Jeremy P.; Carey, John J.; Walsh, Aron
- The Journal of Physical Chemistry C, Vol. 117, Issue 28
Sub-nanometre channels embedded in two-dimensional materials
journal, December 2017
- Han, Yimo; Li, Ming-Yang; Jung, Gang-Seob
- Nature Materials, Vol. 17, Issue 2
Breaking the Landauer limit
journal, July 2017
- Clement, Nicolas; Fujiwara, Akira
- Nature Nanotechnology, Vol. 12, Issue 8
Halide-Induced Self-Limited Growth of Ultrathin Nonlayered Ge Flakes for High-Performance Phototransistors
journal, September 2018
- Hu, Xiaozong; Huang, Pu; Jin, Bao
- Journal of the American Chemical Society, Vol. 140, Issue 40
Activating the molecular spinterface
journal, April 2017
- Cinchetti, Mirko; Dediu, V. Alek; Hueso, Luis E.
- Nature Materials, Vol. 16, Issue 5
Raman scattering, luminescence, and absorption edge under hydrostatic pressures of layered BiI3 and SbI3
journal, January 2007
- Saitoh, A.
- Journal of Raman Spectroscopy, Vol. 38, Issue 5
Van der Waals density functionals applied to solids
journal, May 2011
- Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos
- Physical Review B, Vol. 83, Issue 19
Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices
journal, August 2017
- Zhang, Zhengwei; Chen, Peng; Duan, Xidong
- Science, Vol. 357, Issue 6353
Transforming C60 molecules into graphene quantum dots
journal, March 2011
- Lu, Jiong; Yeo, Pei Shan Emmeline; Gan, Chee Kwan
- Nature Nanotechnology, Vol. 6, Issue 4
Evolutionary selection growth of two-dimensional materials on polycrystalline substrates
journal, March 2018
- Vlassiouk, Ivan V.; Stehle, Yijing; Pudasaini, Pushpa Raj
- Nature Materials, Vol. 17, Issue 4
Thermal behaviour of chlorine-antimony fire-retardant systems
journal, January 1990
- Costa, L.; Goberti, P.; Paganetto, G.
- Polymer Degradation and Stability, Vol. 30, Issue 1
Vapour–liquid–solid growth of monolayer MoS2 nanoribbons
journal, April 2018
- Li, Shisheng; Lin, Yung-Chang; Zhao, Wen
- Nature Materials, Vol. 17, Issue 6
Peltier cooling in molecular junctions
journal, December 2017
- Cui, Longji; Miao, Ruijiao; Wang, Kun
- Nature Nanotechnology, Vol. 13, Issue 2
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Refinement of the crystal structure of cubic antimony trioxide, Sb 2 O 3
journal, August 1975
- Svensson, C.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 31, Issue 8
Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2
journal, April 2014
- Lin, Yung-Chang; Dumcenco, Dumitru O.; Huang, Ying-Sheng
- Nature Nanotechnology, Vol. 9, Issue 5
Chemical accuracy for the van der Waals density functional
journal, December 2009
- Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos
- Journal of Physics: Condensed Matter, Vol. 22, Issue 2
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011
- Momma, Koichi; Izumi, Fujio
- Journal of Applied Crystallography, Vol. 44, Issue 6
Two-dimensional quasi-freestanding molecular crystals for high-performance organic field-effect transistors
journal, October 2014
- He, Daowei; Zhang, Yuhan; Wu, Qisheng
- Nature Communications, Vol. 5, Issue 1
The electronic structure of the antimony chalcogenide series: Prospects for optoelectronic applications
journal, May 2014
- Carey, John J.; Allen, Jeremy P.; Scanlon, David O.
- Journal of Solid State Chemistry, Vol. 213
Structural and vibrational study of cubic Sb O under high pressure
journal, May 2012
- Pereira, A. L. J.; Gracia, L.; Santamaría-Pérez, D.
- Physical Review B, Vol. 85, Issue 17
Room-temperature current blockade in atomically defined single-cluster junctions
journal, August 2017
- Lovat, Giacomo; Choi, Bonnie; Paley, Daniel W.
- Nature Nanotechnology, Vol. 12, Issue 11
A library of atomically thin metal chalcogenides
journal, April 2018
- Zhou, Jiadong; Lin, Junhao; Huang, Xiangwei
- Nature, Vol. 556, Issue 7701
Strong In-Plane Anisotropies of Optical and Electrical Response in Layered Dimetal Chalcogenide
journal, September 2017
- Li, Liang; Gong, Penglai; Wang, Weike
- ACS Nano, Vol. 11, Issue 10
Molecular diodes with rectification ratios exceeding 105 driven by electrostatic interactions
journal, July 2017
- Chen, Xiaoping; Roemer, Max; Yuan, Li
- Nature Nanotechnology, Vol. 12, Issue 8
Preparation of Single-Crystalline Heterojunctions for Organic Electronics
journal, February 2017
- Wu, Jiake; Li, Qinfen; Xue, Guobiao
- Advanced Materials, Vol. 29, Issue 14
A molecular spin-photovoltaic device
journal, August 2017
- Sun, Xiangnan; Vélez, Saül; Atxabal, Ainhoa
- Science, Vol. 357, Issue 6352
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Orientational order controls crystalline and amorphous thermal transport in superatomic crystals
journal, September 2016
- Ong, Wee-Liat; O’Brien, Evan S.; Dougherty, Patrick S. M.
- Nature Materials, Vol. 16, Issue 1
Humidity-controlled rectification switching in ruthenium-complex molecular junctions
journal, December 2017
- Atesci, Huseyin; Kaliginedi, Veerabhadrarao; Celis Gil, Jose A.
- Nature Nanotechnology, Vol. 13, Issue 2
Cluster-Assembled Materials
journal, January 2009
- Claridge, Shelley A.; Castleman, A. W.; Khanna, Shiv N.
- ACS Nano, Vol. 3, Issue 2
Bottom-up organic integrated circuits
journal, October 2008
- Smits, Edsger C. P.; Mathijssen, Simon G. J.; van Hal, Paul A.
- Nature, Vol. 455, Issue 7215
Phase-selective synthesis of 1T′ MoS2 monolayers and heterophase bilayers
journal, October 2018
- Liu, Lina; Wu, Juanxia; Wu, Liyuan
- Nature Materials, Vol. 17, Issue 12
Synthesis and purple-blue emission of antimony trioxide single-crystalline nanobelts with elliptical cross section
journal, February 2009
- Deng, Zhengtao; Chen, Dong; Tang, Fangqiong
- Nano Research, Vol. 2, Issue 2
Vibrational spectroscopic and quantum chemical study of antimony(III) oxide
journal, February 2009
- Voit, E. I.; Panasenko, A. E.; Zemnukhova, L. A.
- Journal of Structural Chemistry, Vol. 50, Issue 1
From Bulk to Monolayer MoS2: Evolution of Raman Scattering
journal, January 2012
- Li, Hong; Zhang, Qing; Yap, Chin Chong Ray
- Advanced Functional Materials, Vol. 22, Issue 7
Two-Dimensional Fullerene Assembly from an Exfoliated van der Waals Template
journal, April 2018
- Lee, Kihong; Choi, Bonnie; Plante, Ilan Jen-La
- Angewandte Chemie International Edition, Vol. 57, Issue 21
Two‐Dimensional Fullerene Assembly from an Exfoliated van der Waals Template
journal, April 2018
- Lee, Kihong; Choi, Bonnie; Plante, Ilan Jen‐La
- Angewandte Chemie, Vol. 130, Issue 21
Parallel Nanoimprint Forming of One-Dimensional Chiral Semiconductor for Strain-Engineered Optical Properties
journal, August 2020
- Wang, Yixiu; Jin, Shengyu; Wang, Qingxiao
- Nano-Micro Letters, Vol. 12, Issue 1
Lead palladium titanate: A room temperature nanoscale multiferroic thin film
journal, February 2020
- Mishra, K. K.; Instan, Alvaro A.; Kumari, Shalini
- Scientific Reports, Vol. 10, Issue 1
Chemical accuracy for the van der Waals density functional
preprint, January 2009
- Klimes, J.; Bowler, D. R.; Michaelides, A.
- arXiv
Van der Waals density functionals applied to solids
text, January 2011
- Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos
- arXiv
Two-dimensional Quasi-Freestanding Molecular Crystals for High-Performance Organic Field-Effect Transistors
text, January 2014
- He, Daowei; Zhang, Yuhan; Wu, Qisheng
- arXiv
Sub-Nanometer Channels Embedded in Two-Dimensional Materials
text, January 2017
- Han, Yimo; Li, Ming-Yang; Jung, Gang-Seob
- arXiv
From Bulk to Monolayer MoS2: Evolution of Raman Scattering
journal, January 2012
- Li, Hong; Zhang, Qing; Yap, Chin Chong Ray
- Advanced Functional Materials, Vol. 22, Issue 7
Preparation of Single-Crystalline Heterojunctions for Organic Electronics
journal, February 2017
- Wu, Jiake; Li, Qinfen; Xue, Guobiao
- Advanced Materials, Vol. 29, Issue 14
Two-Dimensional Fullerene Assembly from an Exfoliated van der Waals Template
journal, April 2018
- Lee, Kihong; Choi, Bonnie; Plante, Ilan Jen-La
- Angewandte Chemie International Edition, Vol. 57, Issue 21
Raman scattering, luminescence, and absorption edge under hydrostatic pressures of layered BiI3 and SbI3
journal, January 2007
- Saitoh, A.
- Journal of Raman Spectroscopy, Vol. 38, Issue 5
Vibrational spectroscopic and quantum chemical study of antimony(III) oxide
journal, February 2009
- Voit, E. I.; Panasenko, A. E.; Zemnukhova, L. A.
- Journal of Structural Chemistry, Vol. 50, Issue 1
Strong In-Plane Anisotropies of Optical and Electrical Response in Layered Dimetal Chalcogenide
journal, September 2017
- Li, Liang; Gong, Penglai; Wang, Weike
- ACS Nano, Vol. 11, Issue 10
Halide-Induced Self-Limited Growth of Ultrathin Nonlayered Ge Flakes for High-Performance Phototransistors
journal, September 2018
- Hu, Xiaozong; Huang, Pu; Jin, Bao
- Journal of the American Chemical Society, Vol. 140, Issue 40
Electronic Structures of Antimony Oxides
journal, July 2013
- Allen, Jeremy P.; Carey, John J.; Walsh, Aron
- The Journal of Physical Chemistry C, Vol. 117, Issue 28
Cluster-Assembled Materials
journal, January 2009
- Claridge, Shelley A.; Castleman, A. W.; Khanna, Shiv N.
- ACS Nano, Vol. 3, Issue 2
Bottom-up organic integrated circuits
journal, October 2008
- Smits, Edsger C. P.; Mathijssen, Simon G. J.; van Hal, Paul A.
- Nature, Vol. 455, Issue 7215
One-pot growth of two-dimensional lateral heterostructures via sequential edge-epitaxy
journal, January 2018
- Sahoo, Prasana K.; Memaran, Shahriar; Xin, Yan
- Nature, Vol. 553, Issue 7686
Two-dimensional quasi-freestanding molecular crystals for high-performance organic field-effect transistors
journal, October 2014
- He, Daowei; Zhang, Yuhan; Wu, Qisheng
- Nature Communications, Vol. 5, Issue 1
Orientational order controls crystalline and amorphous thermal transport in superatomic crystals
journal, September 2016
- Ong, Wee-Liat; O’Brien, Evan S.; Dougherty, Patrick S. M.
- Nature Materials, Vol. 16, Issue 1
Activating the molecular spinterface
journal, April 2017
- Cinchetti, Mirko; Dediu, V. Alek; Hueso, Luis E.
- Nature Materials, Vol. 16, Issue 5
Sub-nanometre channels embedded in two-dimensional materials
journal, December 2017
- Han, Yimo; Li, Ming-Yang; Jung, Gang-Seob
- Nature Materials, Vol. 17, Issue 2
Transforming C60 molecules into graphene quantum dots
journal, March 2011
- Lu, Jiong; Yeo, Pei Shan Emmeline; Gan, Chee Kwan
- Nature Nanotechnology, Vol. 6, Issue 4
Atomic mechanism of the semiconducting-to-metallic phase transition in single-layered MoS2
journal, April 2014
- Lin, Yung-Chang; Dumcenco, Dumitru O.; Huang, Ying-Sheng
- Nature Nanotechnology, Vol. 9, Issue 5
Room-temperature current blockade in atomically defined single-cluster junctions
journal, August 2017
- Lovat, Giacomo; Choi, Bonnie; Paley, Daniel W.
- Nature Nanotechnology, Vol. 12, Issue 11
Vapour–liquid–solid growth of monolayer MoS2 nanoribbons
journal, April 2018
- Li, Shisheng; Lin, Yung-Chang; Zhao, Wen
- Nature Materials, Vol. 17, Issue 6
Humidity-controlled rectification switching in ruthenium-complex molecular junctions
journal, December 2017
- Atesci, Huseyin; Kaliginedi, Veerabhadrarao; Celis Gil, Jose A.
- Nature Nanotechnology, Vol. 13, Issue 2
Peltier cooling in molecular junctions
journal, December 2017
- Cui, Longji; Miao, Ruijiao; Wang, Kun
- Nature Nanotechnology, Vol. 13, Issue 2
A library of atomically thin metal chalcogenides
journal, April 2018
- Zhou, Jiadong; Lin, Junhao; Huang, Xiangwei
- Nature, Vol. 556, Issue 7701
Definition of a Transcendental Order Parameter for Reconstructive Phase Transitions
journal, May 1988
- Dmitriev, V. P.; Rochal, S. B.; Gufan, Yu. M.
- Physical Review Letters, Vol. 60, Issue 19
Molecular behavior of zero-dimensional perovskites
journal, December 2017
- Yin, Jun; Maity, Partha; De Bastiani, Michele
- Science Advances, Vol. 3, Issue 12
A molecular spin-photovoltaic device
journal, August 2017
- Sun, Xiangnan; Vélez, Saül; Atxabal, Ainhoa
- Science, Vol. 357, Issue 6352
Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices
journal, August 2017
- Zhang, Zhengwei; Chen, Peng; Duan, Xidong
- Science, Vol. 357, Issue 6353
Theoretical analysis of doped graphene as cathode catalyst in Li-O2 and Na-O2 batteries -- the impact of the computational scheme
preprint, January 2020
- Novčić, Katarina A.; Dobrota, Ana S.; Petković, Milena
- arXiv