skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electronic and optical properties of oxygen vacancies in amorphous Ta 2 O 5 from first principles

Abstract

Oxygen vacancies are important defects considered to play a central role in the electronic and optical properties of tantalum pentoxide (Ta2O5) films and devices. Despite extensive experimental studies on oxygen vacancies in Ta2O5, the reported defect states are ambiguously identified due to the absence of accurate and conclusive theoretical evidence. Here we investigate the thermodynamic, electronic, and optical properties of oxygen vacancies in amorphous Ta2O5 by first-principles calculations based on hybrid-functional density functional theory (DFT). The calculated thermodynamic and optical transition levels are in good agreement with a broad range of diverse measured properties with various experimental methods, providing conclusive evidence for the identification of the defect states observed in experiments as originating from oxygen vacancies. Our calculations also predict the formation of spin-polarized polarons. Our results elucidate the fundamental atomistic properties of oxygen vacancies in various oxidation states as a function of growth conditions and provide guidance to control the properties of Ta2O5 films/devices.

Authors:
 [1];  [2];  [3]
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering and Dept. of Electrical Engineering and Computer Science
  2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Electrical Engineering and Computer Science
  3. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1492042
DOE Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 9; Journal Issue: 3; Journal ID: ISSN 2040-3364
Country of Publication:
United States
Language:
English

Citation Formats

Lee, Jihang, Lu, Wei D., and Kioupakis, Emmanouil. Electronic and optical properties of oxygen vacancies in amorphous Ta 2 O 5 from first principles. United States: N. p., 2017. Web. doi:10.1039/c6nr07892c.
Lee, Jihang, Lu, Wei D., & Kioupakis, Emmanouil. Electronic and optical properties of oxygen vacancies in amorphous Ta 2 O 5 from first principles. United States. doi:10.1039/c6nr07892c.
Lee, Jihang, Lu, Wei D., and Kioupakis, Emmanouil. Sun . "Electronic and optical properties of oxygen vacancies in amorphous Ta 2 O 5 from first principles". United States. doi:10.1039/c6nr07892c.
@article{osti_1492042,
title = {Electronic and optical properties of oxygen vacancies in amorphous Ta 2 O 5 from first principles},
author = {Lee, Jihang and Lu, Wei D. and Kioupakis, Emmanouil},
abstractNote = {Oxygen vacancies are important defects considered to play a central role in the electronic and optical properties of tantalum pentoxide (Ta2O5) films and devices. Despite extensive experimental studies on oxygen vacancies in Ta2O5, the reported defect states are ambiguously identified due to the absence of accurate and conclusive theoretical evidence. Here we investigate the thermodynamic, electronic, and optical properties of oxygen vacancies in amorphous Ta2O5 by first-principles calculations based on hybrid-functional density functional theory (DFT). The calculated thermodynamic and optical transition levels are in good agreement with a broad range of diverse measured properties with various experimental methods, providing conclusive evidence for the identification of the defect states observed in experiments as originating from oxygen vacancies. Our calculations also predict the formation of spin-polarized polarons. Our results elucidate the fundamental atomistic properties of oxygen vacancies in various oxidation states as a function of growth conditions and provide guidance to control the properties of Ta2O5 films/devices.},
doi = {10.1039/c6nr07892c},
journal = {Nanoscale},
issn = {2040-3364},
number = 3,
volume = 9,
place = {United States},
year = {2017},
month = {1}
}

Works referenced in this record:

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

Defect dominated charge transport in amorphous Ta2O5 thin films
journal, July 2000

  • Fleming, R. M.; Lang, D. V.; Jones, C. D. W.
  • Journal of Applied Physics, Vol. 88, Issue 2
  • DOI: 10.1063/1.373747

Projector augmented-wave method
journal, December 1994


Anatomy of a Nanoscale Conduction Channel Reveals the Mechanism of a High-Performance Memristor
journal, November 2011

  • Miao, Feng; Strachan, John Paul; Yang, J. Joshua
  • Advanced Materials, Vol. 23, Issue 47, p. 5633-5640
  • DOI: 10.1002/adma.201103379

Electronic structure of oxygen vacancy in Ta2O5
journal, July 1999

  • Sawada, H.; Kawakami, K.
  • Journal of Applied Physics, Vol. 86, Issue 2
  • DOI: 10.1063/1.370831

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Oxygen vacancy effects on an amorphous-TaO x -based resistance switch: a first principles study
journal, January 2014


Synergistic Resistive Switching Mechanism of Oxygen Vacancies and Metal Interstitials in Ta 2 O 5
journal, January 2016

  • Zhu, Linggang; Zhou, Jian; Guo, Zhonglu
  • The Journal of Physical Chemistry C, Vol. 120, Issue 4
  • DOI: 10.1021/acs.jpcc.5b11080

Fundamentals of zinc oxide as a semiconductor
journal, October 2009


Predicting and Designing Optical Properties of Inorganic Materials
journal, July 2015


Dual behavior of excess electrons in rutile TiO 2
journal, January 2013

  • Janotti, A.; Franchini, C.; Varley, J. B.
  • physica status solidi (RRL) - Rapid Research Letters, Vol. 7, Issue 3
  • DOI: 10.1002/pssr.201206464

Alternative dielectrics to silicon dioxide for memory and logic devices
journal, August 2000

  • Kingon, Angus I.; Maria, Jon-Paul; Streiffer, S. K.
  • Nature, Vol. 406, Issue 6799
  • DOI: 10.1038/35023243

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Nitrogen plasma annealing for low temperature Ta2O5 films
journal, March 1998

  • Alers, G. B.; Fleming, R. M.; Wong, Y. H.
  • Applied Physics Letters, Vol. 72, Issue 11
  • DOI: 10.1063/1.120569

Detection of oxygen vacancy defect states in capacitors with ultrathin Ta2O5 films by zero-bias thermally stimulated current spectroscopy
journal, October 2003

  • Lau, W. S.; Leong, L. L.; Han, Taejoon
  • Applied Physics Letters, Vol. 83, Issue 14
  • DOI: 10.1063/1.1616990

Tantalum pentoxide (Ta2O5) thin films for advanced dielectric applications
journal, May 1998

  • Chaneliere, C.; Autran, J. L.; Devine, R. A. B.
  • Materials Science and Engineering: R: Reports, Vol. 22, Issue 6
  • DOI: 10.1016/S0927-796X(97)00023-5

Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994


First-principles calculations for point defects in solids
journal, March 2014

  • Freysoldt, Christoph; Grabowski, Blazej; Hickel, Tilmann
  • Reviews of Modern Physics, Vol. 86, Issue 1
  • DOI: 10.1103/RevModPhys.86.253

Electrical characteristics of metal-dielectric-metal and metal-dielectric-semiconductor structures based on electron beam evaporated Y2O3, Ta2O5 and Al2O3 thin film
journal, December 1998

  • Mikhaelashvili, V.; Betzer, Y.; Prudnikov, I.
  • Journal of Applied Physics, Vol. 84, Issue 12
  • DOI: 10.1063/1.369002

Enhanced oxygen vacancy diffusion in Ta 2 O 5 resistive memory devices due to infinitely adaptive crystal structure
journal, April 2016

  • Jiang, Hao; Stewart, Derek A.
  • Journal of Applied Physics, Vol. 119, Issue 13
  • DOI: 10.1063/1.4945579

Electronic structure of δ -Ta 2 O 5 with oxygen vacancy: ab initio calculations and comparison with experiment
journal, July 2011

  • Ivanov, Maxim V.; Perevalov, Timofey V.; Aliev, Vladimir S.
  • Journal of Applied Physics, Vol. 110, Issue 2
  • DOI: 10.1063/1.3606416

Nonlinear Current—Voltage Characteristics of Ta2O5 and Nb2O5 Amorphous Oxides
journal, October 1990

  • Bryksin, V. V.; Goltsev, A. V.; Khanin, S. D.
  • physica status solidi (b), Vol. 161, Issue 2
  • DOI: 10.1002/pssb.2221610232

Defect photoconductivity of anodic Ta 2 O 5 films
journal, April 1973


Direct View at Excess Electrons in TiO 2 Rutile and Anatase
journal, August 2014


Ab initiomolecular dynamics for liquid metals
journal, January 1993


Electronic properties of tantalum pentoxide polymorphs from first-principles calculations
journal, November 2014

  • Lee, J.; Lu, W.; Kioupakis, E.
  • Applied Physics Letters, Vol. 105, Issue 20
  • DOI: 10.1063/1.4901939

A fast, high-endurance and scalable non-volatile memory device made from asymmetric Ta2O5−x/TaO2−x bilayer structures
journal, July 2011

  • Lee, Myoung-Jae; Lee, Chang Bum; Lee, Dongsoo
  • Nature Materials, Vol. 10, Issue 8, p. 625-630
  • DOI: 10.1038/nmat3070

Tuning Ionic Transport in Memristive Devices by Graphene with Engineered Nanopores
journal, February 2016


Study of spontaneous and induced absorption in amorphous Ta 2 O 5 and SiO 2 dielectric thin films
journal, April 2013

  • Markosyan, A. S.; Route, R.; Fejer, M. M.
  • Journal of Applied Physics, Vol. 113, Issue 13
  • DOI: 10.1063/1.4799415

Experimental Demonstration of a Second-Order Memristor and Its Ability to Biorealistically Implement Synaptic Plasticity
journal, February 2015


First-Principles Optical Spectra for F Centers in MgO
journal, March 2012


Thermal noise in interferometric gravitational wave detectors due to dielectric optical coatings
journal, February 2002

  • Harry, Gregory M.; Gretarsson, Andri M.; Saulson, Peter R.
  • Classical and Quantum Gravity, Vol. 19, Issue 5
  • DOI: 10.1088/0264-9381/19/5/305