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Title: 3D Imaging and Manipulation of Subsurface Selenium Vacancies in PdSe 2

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 V Se defects and manipulate them using a scanning tunneling microscope (STM) near the surface of PdSe 2, a recently discovered pentagonal layered TMD. The V Se 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 V Se 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 V Se in PdSe 2, which is much lower than S vacancy in MoS 2 or an O vacancy in TiO 2. As a result, this finding opens an opportunity of defect engineering in PdSe 2 for such as controlled phase transformations and resistive-switching memory device application.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [1];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  3. Nanyang Technological Univ. (Singapore)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1484990
DOE Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article
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. 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, and Li, An -Ping. Mon . "3D Imaging and Manipulation of Subsurface Selenium Vacancies in PdSe2". United States. doi:10.1103/PhysRevLett.121.086101.
@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},
issn = {0031-9007},
number = 8,
volume = 121,
place = {United States},
year = {2018},
month = {8}
}

Works referenced in this record:

Thermodynamic assessment of the palladium–selenium (Pd–Se) system
journal, August 2014


Atomristor: Nonvolatile Resistance Switching in Atomic Sheets of Transition Metal Dichalcogenides
journal, December 2017


Spatially-resolved studies on the role of defects and boundaries in electronic behavior of 2D materials
journal, August 2017


Band structure related wave-function symmetry of amphoteric Si dopants in GaAs
journal, March 2008


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
  • DOI: 10.1103/PhysRevLett.77.3865

From point to extended defects in two-dimensional MoS 2 : Evolution of atomic structure under electron irradiation
journal, July 2013


Tunable Control over the Ionization State of Single Mn Acceptors in GaAs with Defect-Induced Band Bending
journal, May 2011


Line and Point Defects in MoSe 2 Bilayer Studied by Scanning Tunneling Microscopy and Spectroscopy
journal, May 2015


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
  • DOI: 10.1063/1.4893559

Resolving the Spatial Structures of Bound Hole States in Black Phosphorus
journal, October 2017


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
  • DOI: 10.1038/nphys1807

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Local Electronic Structure near Mn Acceptors in InAs: Surface-Induced Symmetry Breaking and Coupling to Host States
journal, October 2007


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
  • DOI: 10.1016/j.cpc.2014.05.003

Gating the charge state of single Fe dopants in the topological insulator Bi 2 Se 3 with a scanning tunneling microscope
journal, July 2012


Atomic-scale properties of the amphoteric dopant Si in GaAs(110) surfaces
journal, October 1998


Controlled Charge Switching on a Single Donor with a Scanning Tunneling Microscope
journal, August 2008


Manipulation of Subsurface Donors in ZnO
journal, May 2013


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
  • DOI: 10.1116/1.583691

Novel Pd 2 Se 3 Two-Dimensional Phase Driven by Interlayer Fusion in Layered PdSe 2
journal, July 2017


Effect of charge manipulation on scanning tunneling spectra of single Mn acceptors in InAs
journal, March 2008


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
  • DOI: 10.1063/1.5016988

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
  • DOI: 10.1038/nnano.2015.56

Pressure-induced superconductivity up to 13.1 K in the pyrite phase of palladium diselenide PdS e 2
journal, August 2017


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
  • DOI: 10.1021/ic0352396

Coherent Dynamics of Coupled Electron and Nuclear Spin Qubits in Diamond
journal, October 2006


Resistive switching in transition metal oxides
journal, June 2008


Atomic Scale Conductance Induced by Single Impurity Charging
journal, February 2005


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
  • DOI: 10.1109/JPROC.2012.2190369

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
  • DOI: 10.1063/1.4933302

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
  • DOI: 10.1063/1.1329672

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
  • DOI: 10.1021/jacs.7b04865

Enhanced Donor Binding Energy Close to a Semiconductor Surface
journal, April 2009


Reaction of O2 with Subsurface Oxygen Vacancies on TiO2 Anatase (101)
journal, August 2013


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
  • DOI: 10.1021/jp411256g

Defect Structure of Localized Excitons in a WSe 2 Monolayer
journal, July 2017


van der Waals Bonding in Layered Compounds from Advanced Density-Functional First-Principles Calculations
journal, June 2012


High Mobility 2D Palladium Diselenide Field-Effect Transistors with Tunable Ambipolar Characteristics
journal, April 2017


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
  • DOI: 10.1038/nnano.2008.160

Tailoring Vacancies Far Beyond Intrinsic Levels Changes the Carrier Type and Optical Response in Monolayer MoSe 2− x Crystals
journal, July 2016


Surface-sensitive measurement of dielectric screening via atom and electron manipulations
journal, November 2016