3D Imaging and Manipulation of Subsurface Selenium Vacancies in
Abstract
Two-dimensional materials such as layered transition-metal dichalcogenides (TMDs) are ideal platforms for studying defect behaviors, an essential step towards defect engineering for novel material functions. Here, we image the 3D lattice locations of selenium-vacancy VSe defects and manipulate them using a scanning tunneling microscope (STM) near the surface of PdSe2, a recently discovered pentagonal layered TMD. The VSe show a characterisitc charging ring in a spatially resolved conductance map, based on which we can determine its subsurface lattice location precisely. Using the STM tip, not only can we reversibly switch the defect states between charge neutral and charge negative, but also trigger migrations of VSe defects. This allows a demonstration of direct “writing” and “erasing” of atomic defects and tracing the diffusion pathways. First-principles calculations reveal a small diffusion barrier of VSe in PdSe2, which is much lower than S vacancy in MoS2 or an O vacancy in TiO2. As a result, this finding opens an opportunity of defect engineering in PdSe2 for such as controlled phase transformations and resistive-switching memory device application.
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[1];
[1]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Nanyang Technological Univ. (Singapore)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1484990
- Alternate Identifier(s):
- OSTI ID: 1465233
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 8; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Nguyen, Giang D., Liang, Liangbo, Zou, Qiang, Fu, Mingming, Oyedele, Akinola D., Sumpter, Bobby G., Liu, Zheng, Gai, Zheng, Xiao, Kai, and Li, An -Ping. 3D Imaging and Manipulation of Subsurface Selenium Vacancies in PdSe2. United States: N. p., 2018.
Web. doi:10.1103/PhysRevLett.121.086101.
Nguyen, Giang D., Liang, Liangbo, Zou, Qiang, Fu, Mingming, Oyedele, Akinola D., Sumpter, Bobby G., Liu, Zheng, Gai, Zheng, Xiao, Kai, & Li, An -Ping. 3D Imaging and Manipulation of Subsurface Selenium Vacancies in PdSe2. United States. https://doi.org/10.1103/PhysRevLett.121.086101
Nguyen, Giang D., Liang, Liangbo, Zou, Qiang, Fu, Mingming, Oyedele, Akinola D., Sumpter, Bobby G., Liu, Zheng, Gai, Zheng, Xiao, Kai, and Li, An -Ping. Mon .
"3D Imaging and Manipulation of Subsurface Selenium Vacancies in PdSe2". United States. https://doi.org/10.1103/PhysRevLett.121.086101. https://www.osti.gov/servlets/purl/1484990.
@article{osti_1484990,
title = {3D Imaging and Manipulation of Subsurface Selenium Vacancies in PdSe2},
author = {Nguyen, Giang D. and Liang, Liangbo and Zou, Qiang and Fu, Mingming and Oyedele, Akinola D. and Sumpter, Bobby G. and Liu, Zheng and Gai, Zheng and Xiao, Kai and Li, An -Ping},
abstractNote = {Two-dimensional materials such as layered transition-metal dichalcogenides (TMDs) are ideal platforms for studying defect behaviors, an essential step towards defect engineering for novel material functions. Here, we image the 3D lattice locations of selenium-vacancy VSe defects and manipulate them using a scanning tunneling microscope (STM) near the surface of PdSe2, a recently discovered pentagonal layered TMD. The VSe show a characterisitc charging ring in a spatially resolved conductance map, based on which we can determine its subsurface lattice location precisely. Using the STM tip, not only can we reversibly switch the defect states between charge neutral and charge negative, but also trigger migrations of VSe defects. This allows a demonstration of direct “writing” and “erasing” of atomic defects and tracing the diffusion pathways. First-principles calculations reveal a small diffusion barrier of VSe in PdSe2, which is much lower than S vacancy in MoS2 or an O vacancy in TiO2. As a result, this finding opens an opportunity of defect engineering in PdSe2 for such as controlled phase transformations and resistive-switching memory device application.},
doi = {10.1103/PhysRevLett.121.086101},
journal = {Physical Review Letters},
number = 8,
volume = 121,
place = {United States},
year = {Mon Aug 20 00:00:00 EDT 2018},
month = {Mon Aug 20 00:00:00 EDT 2018}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 60 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:
Thermodynamic assessment of the palladium–selenium (Pd–Se) system
journal, August 2014
- Bordier, S.; Chocard, A.; Gossé, S.
- Journal of Nuclear Materials, Vol. 451, Issue 1-3
Atomristor: Nonvolatile Resistance Switching in Atomic Sheets of Transition Metal Dichalcogenides
journal, December 2017
- Ge, Ruijing; Wu, Xiaohan; Kim, Myungsoo
- Nano Letters, Vol. 18, Issue 1
Spatially-resolved studies on the role of defects and boundaries in electronic behavior of 2D materials
journal, August 2017
- Hus, Saban M.; Li, An-Ping
- Progress in Surface Science, Vol. 92, Issue 3
Band structure related wave-function symmetry of amphoteric Si dopants in GaAs
journal, March 2008
- Loth, S.; Wenderoth, M.; Teichmann, K.
- Solid State Communications, Vol. 145, Issue 11-12
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
From point to extended defects in two-dimensional MoS : Evolution of atomic structure under electron irradiation
journal, July 2013
- Komsa, Hannu-Pekka; Kurasch, Simon; Lehtinen, Ossi
- Physical Review B, Vol. 88, Issue 3
Tunable Control over the Ionization State of Single Mn Acceptors in GaAs with Defect-Induced Band Bending
journal, May 2011
- Lee, Dong-Hun; Gupta, Jay A.
- Nano Letters, Vol. 11, Issue 5
Line and Point Defects in MoSe 2 Bilayer Studied by Scanning Tunneling Microscopy and Spectroscopy
journal, May 2015
- Liu, Hongjun; Zheng, Hao; Yang, Fang
- ACS Nano, Vol. 9, Issue 6
Influence of external electric fields on oxygen vacancies at the anatase (101) surface
journal, August 2014
- Selçuk, Sencer; Selloni, Annabella
- The Journal of Chemical Physics, Vol. 141, Issue 8
Resolving the Spatial Structures of Bound Hole States in Black Phosphorus
journal, October 2017
- Qiu, Zhizhan; Fang, Hanyan; Carvalho, Alexandra
- Nano Letters, Vol. 17, Issue 11
Gate-controlled ionization and screening of cobalt adatoms on a graphene surface
journal, October 2010
- Brar, Victor; Decker, Régis; Solowan, Hans-Michael
- Nature Physics, Vol. 7, Issue 1, p. 43-47
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
Local Electronic Structure near Mn Acceptors in InAs: Surface-Induced Symmetry Breaking and Coupling to Host States
journal, October 2007
- Marczinowski, F.; Wiebe, J.; Tang, J. -M.
- Physical Review Letters, Vol. 99, Issue 15
An updated version of wannier90: A tool for obtaining maximally-localised Wannier functions
journal, August 2014
- Mostofi, Arash A.; Yates, Jonathan R.; Pizzi, Giovanni
- Computer Physics Communications, Vol. 185, Issue 8
Gating the charge state of single Fe dopants in the topological insulator Bi Se with a scanning tunneling microscope
journal, July 2012
- Song, Can-Li; Jiang, Ye-Ping; Wang, Yi-Lin
- Physical Review B, Vol. 86, Issue 4
Atomic-scale properties of the amphoteric dopant Si in GaAs(110) surfaces
journal, October 1998
- Domke, C.; Ebert, Ph.; Urban, K.
- Surface Science, Vol. 415, Issue 3
Controlled Charge Switching on a Single Donor with a Scanning Tunneling Microscope
journal, August 2008
- Teichmann, K.; Wenderoth, M.; Loth, S.
- Physical Review Letters, Vol. 101, Issue 7
Manipulation of Subsurface Donors in ZnO
journal, May 2013
- Zheng, Hao; Weismann, Alexander; Berndt, Richard
- Physical Review Letters, Vol. 110, Issue 22
Tunneling spectroscopy of the GaAs(110) surface
journal, July 1987
- Feenstra, R. M.
- Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 5, Issue 4
Novel Two-Dimensional Phase Driven by Interlayer Fusion in Layered
journal, July 2017
- Lin, Junhao; Zuluaga, Sebastian; Yu, Peng
- Physical Review Letters, Vol. 119, Issue 1
Effect of charge manipulation on scanning tunneling spectra of single Mn acceptors in InAs
journal, March 2008
- Marczinowski, Felix; Wiebe, Jens; Meier, Focko
- Physical Review B, Vol. 77, Issue 11
Impact of vacancies on electronic properties of black phosphorus probed by STM
journal, January 2018
- Riffle, J. V.; Flynn, C.; St. Laurent, B.
- Journal of Applied Physics, Vol. 123, Issue 4
Gate-tunable memristive phenomena mediated by grain boundaries in single-layer MoS2
journal, April 2015
- Sangwan, Vinod K.; Jariwala, Deep; Kim, In Soo
- Nature Nanotechnology, Vol. 10, Issue 5
Pressure-induced superconductivity up to 13.1 K in the pyrite phase of palladium diselenide
journal, August 2017
- ElGhazali, Moaz A.; Naumov, Pavel G.; Mirhosseini, Hossein
- Physical Review B, Vol. 96, Issue 6
Experimental and Theoretical Investigation on the Relative Stability of the PdS 2 - and Pyrite-Type Structures of PdSe 2
journal, March 2004
- Soulard, C.; Rocquefelte, X.; Petit, P. -E.
- Inorganic Chemistry, Vol. 43, Issue 6
Coherent Dynamics of Coupled Electron and Nuclear Spin Qubits in Diamond
journal, October 2006
- Childress, L.; Gurudev Dutt, M. V.; Taylor, J. M.
- Science, Vol. 314, Issue 5797
Resistive switching in transition metal oxides
journal, June 2008
- Sawa, Akihito
- Materials Today, Vol. 11, Issue 6
Atomic Scale Conductance Induced by Single Impurity Charging
journal, February 2005
- Pradhan, N. A.; Liu, N.; Silien, C.
- Physical Review Letters, Vol. 94, Issue 7
Metal–Oxide RRAM
journal, June 2012
- Wong, H.-S. Philip; Lee, Heng-Yuan; Yu, Shimeng
- Proceedings of the IEEE, Vol. 100, Issue 6, p. 1951-1970
Electronic, transport, and optical properties of bulk and mono-layer PdSe 2
journal, October 2015
- Sun, Jifeng; Shi, Hongliang; Siegrist, Theo
- Applied Physics Letters, Vol. 107, Issue 15
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
PdSe 2 : Pentagonal Two-Dimensional Layers with High Air Stability for Electronics
journal, September 2017
- Oyedele, Akinola D.; Yang, Shize; Liang, Liangbo
- Journal of the American Chemical Society, Vol. 139, Issue 40
Enhanced Donor Binding Energy Close to a Semiconductor Surface
journal, April 2009
- Wijnheijmer, A. P.; Garleff, J. K.; Teichmann, K.
- Physical Review Letters, Vol. 102, Issue 16
Reaction of O2 with Subsurface Oxygen Vacancies on TiO2 Anatase (101)
journal, August 2013
- Setvin, M.; Aschauer, U.; Scheiber, P.
- Science, Vol. 341, Issue 6149
Single-Layer MoS 2 with Sulfur Vacancies: Structure and Catalytic Application
journal, March 2014
- Le, Duy; Rawal, Takat B.; Rahman, Talat S.
- The Journal of Physical Chemistry C, Vol. 118, Issue 10
Defect Structure of Localized Excitons in a Monolayer
journal, July 2017
- Zhang, Shuai; Wang, Chen-Guang; Li, Ming-Yang
- Physical Review Letters, Vol. 119, Issue 4
van der Waals Bonding in Layered Compounds from Advanced Density-Functional First-Principles Calculations
journal, June 2012
- Björkman, T.; Gulans, A.; Krasheninnikov, A. V.
- Physical Review Letters, Vol. 108, Issue 23
Systematic study of structural, electronic, and optical properties of atomic-scale defects in the two-dimensional transition metal dichalcogenides ( , W; , Se, Te)
journal, December 2015
- Haldar, Soumyajyoti; Vovusha, Hakkim; Yadav, Manoj Kumar
- Physical Review B, Vol. 92, Issue 23
High Mobility 2D Palladium Diselenide Field-Effect Transistors with Tunable Ambipolar Characteristics
journal, April 2017
- Chow, Wai Leong; Yu, Peng; Liu, Fucai
- Advanced Materials, Vol. 29, Issue 21
Memristive switching mechanism for metal/oxide/metal nanodevices
journal, June 2008
- Yang, J. Joshua; Pickett, Matthew D.; Li, Xuema
- Nature Nanotechnology, Vol. 3, Issue 7
Tailoring Vacancies Far Beyond Intrinsic Levels Changes the Carrier Type and Optical Response in Monolayer MoSe 2− x Crystals
journal, July 2016
- Mahjouri-Samani, Masoud; Liang, Liangbo; Oyedele, Akinola
- Nano Letters, Vol. 16, Issue 8
Surface-sensitive measurement of dielectric screening via atom and electron manipulations
journal, November 2016
- Eom, Daejin; Seo, Eonmi; Koo, Ja-Yong
- Physical Review B, Vol. 94, Issue 19
Experimental and Theoretical Investigation on the Relative Stability of the PdS2- and Pyrite-Type Structures of PdSe2.
journal, June 2004
- Soulard, C.; Rocquefelte, X.; Petit, P. -E.
- ChemInform, Vol. 35, Issue 25
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Reaction of O₂ with Subsurface Oxygen Vacancies on TiO₂ Anatase (101)
text, January 2013
- Hou, W.; Setvin, M.; Schmid, M.
- American Association for the Advancement of Science
Gate-tunable Memristive Phenonmena Mediated by Grain Boundaries in Single Layer MoS2
text, January 2015
- Sangwan, V. K.; Jariwala, D.; Kim, I. S.
- arXiv
Line and Point Defects in MoSe2 Bilayer Studied by Scanning Tunneling Microscopy and Spectroscopy
text, January 2015
- Liu, Hongjun; Zheng, Hao; Yang, Fang
- arXiv
Reaction of O2 with Subsurface Oxygen Vacancies on TiO2 Anatase (101)
text, January 2018
- Setvin, Martin; Aschauer, Ulrich; Scheiber, Philipp
- arXiv
Works referencing / citing this record:
Pressure‐Tunable Ambipolar Conduction and Hysteresis in Thin Palladium Diselenide Field Effect Transistors
journal, May 2019
- Di Bartolomeo, Antonio; Pelella, Aniello; Liu, Xiaowei
- Advanced Functional Materials, Vol. 29, Issue 29
Atomic‐Scale Manipulation and In Situ Characterization with Scanning Tunneling Microscopy
journal, October 2019
- Ko, Wonhee; Ma, Chuanxu; Nguyen, Giang D.
- Advanced Functional Materials, Vol. 29, Issue 52
Recent Progress on 2D Noble‐Transition‐Metal Dichalcogenides
journal, October 2019
- Pi, Lejing; Li, Liang; Liu, Kailang
- Advanced Functional Materials, Vol. 29, Issue 51
Anisotropic Growth and Scanning Tunneling Microscopy Identification of Ultrathin Even‐Layered PdSe 2 Ribbons
journal, September 2019
- Jiang, Shaolong; Xie, Chunyu; Gu, Yue
- Small, Vol. 15, Issue 45
Electronic transport in planar atomic-scale structures measured by two-probe scanning tunneling spectroscopy
journal, April 2019
- Kolmer, Marek; Brandimarte, Pedro; Lis, Jakub
- Nature Communications, Vol. 10, Issue 1
Exploring the air stability of PdSe2 via electrical transport measurements and defect calculations
journal, December 2019
- Hoffman, Anna N.; Gu, Yiyi; Liang, Liangbo
- npj 2D Materials and Applications, Vol. 3, Issue 1
Ferroelastic lattice rotation and band-gap engineering in quasi 2D layered-structure PdSe 2 under uniaxial stress
journal, January 2019
- Lei, Wen; Cai, Bo; Zhou, Huanfu
- Nanoscale, Vol. 11, Issue 25
Spin Polarization Properties of Pentagonal PdSe2 Induced by 3D Transition-Metal Doping: First-Principles Calculations
journal, November 2018
- Zhao, Xiuwen; Qiu, Bin; Hu, Guichao
- Materials, Vol. 11, Issue 11