Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy
Abstract
Defects in materials give rise to fluctuations in electrostatic fields that reflect the local charge density, but imaging this with single atom sensitivity is challenging. However, if possible, this provides information about the energetics of adatom binding, localized conduction channels, molecular functionality and their relationship to individual bonds. Here, ultrastable electron-optics are combined with a high-speed 2D electron detector to map electrostatic fields around individual atoms in 2D monolayers using 4D scanning transmission electron microscopy. Simultaneous imaging of the electric field, phase, annular dark field and the total charge in 2D MoS2 and WS2 is demonstrated for pristine areas and regions with 1D wires. The in-gap states in sulphur line vacancies cause 1D electron-rich channels that are mapped experimentally and confirmed using density functional theory calculations. We show how electrostatic fields are sensitive in defective areas to changes of atomic bonding and structural determination beyond conventional imaging.
- Authors:
-
[3];
[3];
- Harvard Univ., Cambridge, MA (United States)
- Univ. of Oxford (United Kingdom)
- Univ. of Oxford (United Kingdom); Diamond Light Source Ltd., Didcot, Oxfordshire (United Kingdom)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Brandeis Univ., Waltham, MA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1559192
- Grant/Contract Number:
- AC02-05CH11231
- 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
Fang, Shiang, Wen, Yi, Allen, Christopher S., Ophus, Colin, Han, Grace G. D., Kirkland, Angus I., Kaxiras, Efthimios, and Warner, Jamie H. Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-08904-9.
Fang, Shiang, Wen, Yi, Allen, Christopher S., Ophus, Colin, Han, Grace G. D., Kirkland, Angus I., Kaxiras, Efthimios, & Warner, Jamie H. Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy. United States. https://doi.org/10.1038/s41467-019-08904-9
Fang, Shiang, Wen, Yi, Allen, Christopher S., Ophus, Colin, Han, Grace G. D., Kirkland, Angus I., Kaxiras, Efthimios, and Warner, Jamie H. Fri .
"Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy". United States. https://doi.org/10.1038/s41467-019-08904-9. https://www.osti.gov/servlets/purl/1559192.
@article{osti_1559192,
title = {Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy},
author = {Fang, Shiang and Wen, Yi and Allen, Christopher S. and Ophus, Colin and Han, Grace G. D. and Kirkland, Angus I. and Kaxiras, Efthimios and Warner, Jamie H.},
abstractNote = {Defects in materials give rise to fluctuations in electrostatic fields that reflect the local charge density, but imaging this with single atom sensitivity is challenging. However, if possible, this provides information about the energetics of adatom binding, localized conduction channels, molecular functionality and their relationship to individual bonds. Here, ultrastable electron-optics are combined with a high-speed 2D electron detector to map electrostatic fields around individual atoms in 2D monolayers using 4D scanning transmission electron microscopy. Simultaneous imaging of the electric field, phase, annular dark field and the total charge in 2D MoS2 and WS2 is demonstrated for pristine areas and regions with 1D wires. The in-gap states in sulphur line vacancies cause 1D electron-rich channels that are mapped experimentally and confirmed using density functional theory calculations. We show how electrostatic fields are sensitive in defective areas to changes of atomic bonding and structural determination beyond conventional imaging.},
doi = {10.1038/s41467-019-08904-9},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Fri Mar 08 00:00:00 EST 2019},
month = {Fri Mar 08 00:00:00 EST 2019}
}
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Works referenced in this record:
Experimental analysis of charge redistribution due to chemical bonding by high-resolution transmission electron microscopy
journal, January 2011
- Meyer, Jannik C.; Kurasch, Simon; Park, Hye Jin
- Nature Materials, Vol. 10, Issue 3
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
Sub-Ångstrom electric field measurements on a universal detector in a scanning transmission electron microscope
journal, August 2018
- Hachtel, Jordan A.; Idrobo, Juan Carlos; Chi, Miaofang
- Advanced Structural and Chemical Imaging, Vol. 4, Issue 1
Atomic-scale quantification of charge densities in two-dimensional materials
journal, September 2018
- Müller-Caspary, Knut; Duchamp, Martial; Rösner, Malte
- Physical Review B, Vol. 98, Issue 12
An improved ptychographical phase retrieval algorithm for diffractive imaging
journal, September 2009
- Maiden, Andrew M.; Rodenburg, John M.
- Ultramicroscopy, Vol. 109, Issue 10
Characterisation of the Medipix3 detector for 60 and 80 keV electrons
journal, November 2017
- Mir, J. A.; Clough, R.; MacInnes, R.
- Ultramicroscopy, Vol. 182
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Strain Mapping of Two-Dimensional Heterostructures with Subpicometer Precision
journal, May 2018
- Han, Yimo; Nguyen, Kayla; Cao, Michael
- Nano Letters, Vol. 18, Issue 6
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Determining the Optimized Interlayer Separation Distance in Vertical Stacked 2D WS 2 :hBN:MoS 2 Heterostructures for Exciton Energy Transfer
journal, February 2018
- Xu, Wenshuo; Kozawa, Daichi; Liu, Yu
- Small, Vol. 14, Issue 13
Direct Visualization of Local Electromagnetic Field Structures by Scanning Transmission Electron Microscopy
journal, July 2017
- Shibata, Naoya; Findlay, Scott D.; Matsumoto, Takao
- Accounts of Chemical Research, Vol. 50, Issue 7
Measuring nanometre-scale electric fields in scanning transmission electron microscopy using segmented detectors
journal, November 2017
- Brown, H. G.; Shibata, N.; Sasaki, H.
- Ultramicroscopy, Vol. 182
Ptychographic electron microscopy using high-angle dark-field scattering for sub-nanometre resolution imaging
journal, January 2012
- Humphry, M. J.; Kraus, B.; Hurst, A. C.
- Nature Communications, Vol. 3, Issue 1
Ultralong 1D Vacancy Channels for Rapid Atomic Migration during 2D Void Formation in Monolayer MoS 2
journal, July 2018
- Chen, Qu; Li, Huashan; Zhou, Si
- ACS Nano, Vol. 12, Issue 8
Probing the Internal Atomic Charge Density Distributions in Real Space
journal, August 2018
- Sánchez-Santolino, Gabriel; Lugg, Nathan R.; Seki, Takehito
- ACS Nano, Vol. 12, Issue 9
Simultaneous atomic-resolution electron ptychography and Z-contrast imaging of light and heavy elements in complex nanostructures
journal, August 2016
- Yang, H.; Rutte, R. N.; Jones, L.
- Nature Communications, Vol. 7, Issue 1
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
Phase contrast STEM for thin samples: Integrated differential phase contrast
journal, January 2016
- Lazić, Ivan; Bosch, Eric G. T.; Lazar, Sorin
- Ultramicroscopy, Vol. 160
Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992
- Perdew, John P.; Wang, Yue
- Physical Review B, Vol. 45, Issue 23, p. 13244-13249
Practical aspects of diffractive imaging using an atomic-scale coherent electron probe
journal, October 2016
- Chen, Z.; Weyland, M.; Ercius, P.
- Ultramicroscopy, Vol. 169
Direct electric field imaging of graphene defects
journal, September 2018
- Ishikawa, Ryo; Findlay, Scott D.; Seki, Takehito
- Nature Communications, Vol. 9, Issue 1
Atomic Level Distributed Strain within Graphene Divacancies from Bond Rotations
journal, July 2015
- Chen, Qu; Robertson, Alex W.; He, Kuang
- ACS Nano, Vol. 9, Issue 8
Electric field imaging of single atoms
journal, May 2017
- Shibata, Naoya; Seki, Takehito; Sánchez-Santolino, Gabriel
- Nature Communications, Vol. 8, Issue 1
Electron ptychography of 2D materials to deep sub-ångström resolution
journal, July 2018
- Jiang, Yi; Chen, Zhen; Han, Yimo
- Nature, Vol. 559, Issue 7714
Differential phase-contrast microscopy at atomic resolution
journal, June 2012
- Shibata, Naoya; Findlay, Scott D.; Kohno, Yuji
- Nature Physics, Vol. 8, Issue 8
Detailed Atomic Reconstruction of Extended Line Defects in Monolayer MoS 2
journal, May 2016
- Wang, Shanshan; Lee, Gun-Do; Lee, Sungwoo
- ACS Nano, Vol. 10, Issue 5
Towards quantitative, atomic-resolution reconstruction of the electrostatic potential via differential phase contrast using electrons
journal, December 2015
- Close, R.; Chen, Z.; Shibata, N.
- Ultramicroscopy, Vol. 159
Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction
journal, December 2014
- Müller, Knut; Krause, Florian F.; Béché, Armand
- Nature Communications, Vol. 5, Issue 1
Development of Cs and Cc correctors for transmission electron microscopy
journal, February 2013
- Hosokawa, Fumio; Sawada, Hidetaka; Kondo, Yukihito
- Microscopy, Vol. 62, Issue 1
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020
- Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna
- Scientific Reports, Vol. 10, Issue 1
Strain Mapping of Two-Dimensional Heterostructures with Sub-Picometer Precision
text, January 2018
- Han, Yimo; Nguyen, Kayla; Cao, Michael
- arXiv
Determining the Optimized Interlayer Separation Distance in Vertical Stacked 2D WS 2 :hBN:MoS 2 Heterostructures for Exciton Energy Transfer
journal, February 2018
- Xu, Wenshuo; Kozawa, Daichi; Liu, Yu
- Small, Vol. 14, Issue 13
An improved ptychographical phase retrieval algorithm for diffractive imaging
journal, September 2009
- Maiden, Andrew M.; Rodenburg, John M.
- Ultramicroscopy, Vol. 109, Issue 10
Towards quantitative, atomic-resolution reconstruction of the electrostatic potential via differential phase contrast using electrons
journal, December 2015
- Close, R.; Chen, Z.; Shibata, N.
- Ultramicroscopy, Vol. 159
Phase contrast STEM for thin samples: Integrated differential phase contrast
journal, January 2016
- Lazić, Ivan; Bosch, Eric G. T.; Lazar, Sorin
- Ultramicroscopy, Vol. 160
Measuring nanometre-scale electric fields in scanning transmission electron microscopy using segmented detectors
journal, November 2017
- Brown, H. G.; Shibata, N.; Sasaki, H.
- Ultramicroscopy, Vol. 182
Atomic Level Distributed Strain within Graphene Divacancies from Bond Rotations
journal, July 2015
- Chen, Qu; Robertson, Alex W.; He, Kuang
- ACS Nano, Vol. 9, Issue 8
Ultralong 1D Vacancy Channels for Rapid Atomic Migration during 2D Void Formation in Monolayer MoS 2
journal, July 2018
- Chen, Qu; Li, Huashan; Zhou, Si
- ACS Nano, Vol. 12, Issue 8
Probing the Internal Atomic Charge Density Distributions in Real Space
journal, August 2018
- Sánchez-Santolino, Gabriel; Lugg, Nathan R.; Seki, Takehito
- ACS Nano, Vol. 12, Issue 9
Electric field imaging of single atoms
journal, May 2017
- Shibata, Naoya; Seki, Takehito; Sánchez-Santolino, Gabriel
- Nature Communications, Vol. 8, Issue 1
Ptychographic electron microscopy using high-angle dark-field scattering for sub-nanometre resolution imaging
journal, January 2012
- Humphry, M. J.; Kraus, B.; Hurst, A. C.
- Nature Communications, Vol. 3, Issue 1
Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction
journal, December 2014
- Müller, Knut; Krause, Florian F.; Béché, Armand
- Nature Communications, Vol. 5, Issue 1
Experimental analysis of charge redistribution due to chemical bonding by high-resolution transmission electron microscopy
journal, January 2011
- Meyer, Jannik C.; Kurasch, Simon; Park, Hye Jin
- Nature Materials, Vol. 10, Issue 3
Differential phase-contrast microscopy at atomic resolution
journal, June 2012
- Shibata, Naoya; Findlay, Scott D.; Kohno, Yuji
- Nature Physics, Vol. 8, Issue 8
Direct electric field imaging of graphene defects
journal, September 2018
- Ishikawa, Ryo; Findlay, Scott D.; Seki, Takehito
- Nature Communications, Vol. 9, Issue 1
Development of Cs and Cc correctors for transmission electron microscopy
journal, February 2013
- Hosokawa, Fumio; Sawada, Hidetaka; Kondo, Yukihito
- Microscopy, Vol. 62, Issue 1
Sub-Ångstrom electric field measurements on a universal detector in a scanning transmission electron microscope
journal, August 2018
- Hachtel, Jordan A.; Idrobo, Juan Carlos; Chi, Miaofang
- Advanced Structural and Chemical Imaging, Vol. 4, Issue 1
Strain Mapping of Two-Dimensional Heterostructures with Sub-Picometer Precision
text, January 2018
- Han, Yimo; Nguyen, Kayla; Cao, Michael
- arXiv
Works referencing / citing this record:
In situ electron microscopy observation of the redox process in plasmonic heterogeneous-photo-sensitive nanoparticles
journal, January 2019
- Muraca, Diego; Scaffardi, Lucia B.; Santillán, Jesica M. J.
- Nanoscale Advances, Vol. 1, Issue 10
Sub-100 nanosecond temporally resolved imaging with the Medipix3 direct electron detector
journal, March 2020
- Paterson, Gary W.; Lamb, Raymond J.; Ballabriga, Rafael
- Ultramicroscopy, Vol. 210
Fast Pixelated Detectors in Scanning Transmission Electron Microscopy. Part I: Data Acquisition, Live Processing, and Storage
journal, July 2020
- Nord, Magnus; Webster, Robert W. H.; Paton, Kirsty A.
- Microscopy and Microanalysis, Vol. 26, Issue 4
Robust Sample Preparation of Large-Area In- and Out-of-Plane Cross Sections of Layered Materials with Ultramicrotomy
journal, March 2020
- Cichocka, Magdalena O.; Bolhuis, Maarten; van Heijst, Sabrya E.
- ACS Applied Materials & Interfaces, Vol. 12, Issue 13
Fast Grain Mapping with Sub-Nanometer Resolution Using 4D-STEM with Grain Classification by Principal Component Analysis and Non-Negative Matrix Factorization
text, January 2021
- Allen, Frances I.; Pekin, Thomas C.; Persaud, Arun
- arXiv