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Title: Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study

Abstract

Here, we apply density-functional theory calculations to predict dopant modulation of electrical conductivity (σo) for seven dopants (C, Si, Ge, H, F, N, and B) sampled at 18 quantum molecular dynamics configurations of five independent insertion sites into two (high/low) baseline references of σo in amorphous Ta2O5, where each reference contains a single, neutral O vacancy center (VO0). From this statistical population (n = 1260), we analyze defect levels, physical structure, and valence charge distributions to characterize nanoscale modification of the atomistic structure in local dopant neighborhoods. C is the most effective dopant at lowering Ta2Ox σo, while also exhibiting an amphoteric doping behavior by either donating or accepting charge depending on the host oxide matrix. Both B and F robustly increase Ta2Ox σo, although F does so through elimination of Ta high charge outliers, while B insertion conversely creates high charge O outliers through favorable BO3 group formation, especially in the low σo reference. While N applications to dope and passivate oxides are prevalent, we also found that N exacerbates the stochasticity of σo we sought to mitigate; sensitivity to the N insertion site and some propensity to form N-O bond chemistries appear responsible. Finally, we use direct first-principlesmore » predictions of σo to explore feasible Ta2O5 dopants to engineer improved oxides with lower variance and greater repeatability to advance the manufacturability of resistive memory technologies.« less

Authors:
 [1];  [1];  [1]
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  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1361046
Alternate Identifier(s):
OSTI ID: 1366554
Report Number(s):
SAND2017-3842J
Journal ID: ISSN 0021-8979; 652423
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 121; Journal Issue: 21; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Bondi, Robert J., Fox, Brian P., and Marinella, Matthew J. Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study. United States: N. p., 2017. Web. doi:10.1063/1.4983850.
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Bondi, Robert J., Fox, Brian P., & Marinella, Matthew J. Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study. United States. https://doi.org/10.1063/1.4983850
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Bondi, Robert J., Fox, Brian P., and Marinella, Matthew J. Thu . "Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study". United States. https://doi.org/10.1063/1.4983850. https://www.osti.gov/servlets/purl/1361046.
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@article{osti_1361046,
title = {Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study},
author = {Bondi, Robert J. and Fox, Brian P. and Marinella, Matthew J.},
abstractNote = {Here, we apply density-functional theory calculations to predict dopant modulation of electrical conductivity (σo) for seven dopants (C, Si, Ge, H, F, N, and B) sampled at 18 quantum molecular dynamics configurations of five independent insertion sites into two (high/low) baseline references of σo in amorphous Ta2O5, where each reference contains a single, neutral O vacancy center (VO0). From this statistical population (n = 1260), we analyze defect levels, physical structure, and valence charge distributions to characterize nanoscale modification of the atomistic structure in local dopant neighborhoods. C is the most effective dopant at lowering Ta2Ox σo, while also exhibiting an amphoteric doping behavior by either donating or accepting charge depending on the host oxide matrix. Both B and F robustly increase Ta2Ox σo, although F does so through elimination of Ta high charge outliers, while B insertion conversely creates high charge O outliers through favorable BO3 group formation, especially in the low σo reference. While N applications to dope and passivate oxides are prevalent, we also found that N exacerbates the stochasticity of σo we sought to mitigate; sensitivity to the N insertion site and some propensity to form N-O bond chemistries appear responsible. Finally, we use direct first-principles predictions of σo to explore feasible Ta2O5 dopants to engineer improved oxides with lower variance and greater repeatability to advance the manufacturability of resistive memory technologies.},
doi = {10.1063/1.4983850},
journal = {Journal of Applied Physics},
number = 21,
volume = 121,
place = {United States},
year = {Thu Jun 01 00:00:00 EDT 2017},
month = {Thu Jun 01 00:00:00 EDT 2017}
}
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Works referenced in this record:

Doping effects in amorphous oxides
journal, January 2012

  • Funabiki, Fuji; Kamiya, Toshio; Hosono, Hideo
  • Journal of the Ceramic Society of Japan, Vol. 120, Issue 1407
  • DOI: 10.2109/jcersj2.120.447

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

Efficient hybrid density functional calculations in solids: Assessment of the Heyd–Scuseria–Ernzerhof screened Coulomb hybrid functional
journal, July 2004

  • Heyd, Jochen; Scuseria, Gustavo E.
  • The Journal of Chemical Physics, Vol. 121, Issue 3, p. 1187-1192
  • DOI: 10.1063/1.1760074

Dopant selection rules for desired electronic structure and vacancy formation characteristics of TiO 2 resistive memory
journal, February 2013

  • Zhao, Liang; Park, Seong-Geon; Magyari-Köpe, Blanka
  • Applied Physics Letters, Vol. 102, Issue 8
  • DOI: 10.1063/1.4794083

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

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

Computer graphics and graphical user interfaces as tools in simulations of matter at the atomic scale
journal, October 2003

Tuning Resistive Switching Characteristics of Tantalum Oxide Memristors through Si Doping
journal, September 2014

  • Kim, Sungho; Choi, ShinHyun; Lee, Jihang
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn503464q

Electrical conductivity in oxygen-deficient phases of tantalum pentoxide from first-principles calculations
journal, November 2013

  • Bondi, Robert J.; Desjarlais, Michael P.; Thompson, Aidan P.
  • Journal of Applied Physics, Vol. 114, Issue 20
  • DOI: 10.1063/1.4829900

Electrical conductivity for warm, dense aluminum plasmas and liquids
journal, August 2002

H-treatment impact on conductive-filament formation and stability in Ta2O5-based resistive-switching memory cells
journal, March 2015

  • Goux, L.; Kim, J. Y.; Magyari-Kope, B.
  • Journal of Applied Physics, Vol. 117, Issue 12
  • DOI: 10.1063/1.4915946

On the Switching Parameter Variation of Metal Oxide RRAM—Part II: Model Corroboration and Device Design Strategy
journal, April 2012

  • Yu, Shimeng; Guan, Ximeng; Wong, H. -S. Philip
  • IEEE Transactions on Electron Devices, Vol. 59, Issue 4
  • DOI: 10.1109/TED.2012.2184544

Nitrogen- and fluorine-doped ZrO 2 : a promising p–n junction for an ultraviolet light-emitting diode
journal, July 2012

First principles study of oxygen vacancy defects in tantalum pentoxide
journal, November 2003

A fast and robust algorithm for Bader decomposition of charge density
journal, June 2006

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

First principles study of oxygen vacancy migration in tantalum pentoxide
journal, February 2004

Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 124, Issue 21
  • DOI: 10.1063/1.2204597

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Direct Observation of Nitrogen Location in Molecular Beam Epitaxy Grown Nitrogen-Doped ZnO
journal, February 2006

Ab initio study of the optical properties of shocked LiF
journal, October 2005

Role of Nitrogen Atoms in Reduction of Electron Charge Traps in Hf-Based High- $\kappa$ Dielectrics
journal, May 2007

  • Umezawa, N.; Shiraishi, K.; Torii, K.
  • IEEE Electron Device Letters, Vol. 28, Issue 5
  • DOI: 10.1109/LED.2007.894655

Defect passivation in HfO2 gate oxide by fluorine
journal, October 2006

  • Tse, K.; Robertson, J.
  • Applied Physics Letters, Vol. 89, Issue 14
  • DOI: 10.1063/1.2360190

Defect energy levels in Ta2O5 and nitrogen-doped Ta2O5
journal, December 2008

  • Shin, Hyunho; Park, Sang Yeup; Bae, Shin-Tae
  • Journal of Applied Physics, Vol. 104, Issue 11
  • DOI: 10.1063/1.2937197

Reliable resistive switching memory based on oxygen-vacancy-controlled bilayer structures
journal, January 2016

Improved resistive switching properties by nitrogen doping in tungsten oxide thin films
journal, May 2015

Probing the atomic structure of amorphous Ta2O5 coatings
journal, January 2011

  • Bassiri, R.; Borisenko, K. B.; Cockayne, D. J. H.
  • Applied Physics Letters, Vol. 98, Issue 3
  • DOI: 10.1063/1.3535982

Phase Diagram and Electrical Conductivity of High Energy-Density Water from Density Functional Theory
journal, July 2006

Low power switching of Si-doped Ta 2 O 5 resistive random access memory for high density memory application
journal, March 2016

  • Kim, Beom Yong; Lee, Kee Jeung; Chung, Su Ock
  • Japanese Journal of Applied Physics, Vol. 55, Issue 4S
  • DOI: 10.7567/JJAP.55.04EE09

The Boltzmann Equation in the Theory of Electrical Conduction in Metals
journal, April 1958

How We Found The Missing Memristor
journal, December 2008

Classification of chemical bonds based on topological analysis of electron localization functions
journal, October 1994

The missing memristor found
journal, May 2008

  • Strukov, Dmitri B.; Snider, Gregory S.; Stewart, Duncan R.
  • Nature, Vol. 453, Issue 7191
  • DOI: 10.1038/nature06932

Role of atomistic structure in the stochastic nature of conductivity in substoichiometric tantalum pentoxide
journal, March 2016

  • Bondi, Robert J.; Fox, Brian P.; Marinella, Matthew J.
  • Journal of Applied Physics, Vol. 119, Issue 12
  • DOI: 10.1063/1.4943163

First-principles study of carbon impurity effects in the pseudo-hexagonal Ta2O5
journal, June 2016

  • Kim, Ja-Yong; Magyari-Köpe, Blanka; Nishi, Yoshio
  • Current Applied Physics, Vol. 16, Issue 6
  • DOI: 10.1016/j.cap.2016.03.014

Effects of Mg-Doping on ${\rm HfO}_{2}$-Based ReRAM Device Switching Characteristics
journal, October 2013

  • Long, Branden Michael; Mandal, Saptarshi; Livecchi, Joseph
  • IEEE Electron Device Letters, Vol. 34, Issue 10
  • DOI: 10.1109/LED.2013.2276482

Why nitrogen cannot lead to p-type conductivity in ZnO
journal, December 2009

  • Lyons, J. L.; Janotti, A.; Van de Walle, C. G.
  • Applied Physics Letters, Vol. 95, Issue 25
  • DOI: 10.1063/1.3274043

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

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

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

Atomistic structural description of the Si(001)/ a -SiO 2 interface: The influence of different Keating-like potential parameters
journal, June 2011

  • Lee, Sangheon; Bondi, Robert J.; Hwang, Gyeong S.
  • Journal of Applied Physics, Vol. 109, Issue 11
  • DOI: 10.1063/1.3581110

Structural systematics in the binary system Ta2O5–WO3. V. The structure of the low-temperature form of tantalum oxide L-Ta2O5
journal, May 1971

  • Stephenson, N. C.; Roth, R. S.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 27, Issue 5
  • DOI: 10.1107/S056774087100342X

Ab initio simulations of the electrical and optical properties of shock-compressed SiO 2
journal, October 2004

Electrically inactive nitrogen complex in Si oxynitride
journal, December 2002

Well controlled multiple resistive switching states in the Al local doped HfO 2 resistive random access memory device
journal, April 2013

  • Chen, Y. S.; Chen, B.; Gao, B.
  • Journal of Applied Physics, Vol. 113, Issue 16
  • DOI: 10.1063/1.4803076

Role of Hydrogen Ions in TiO 2 -Based Memory Devices
journal, January 2011

Correlations between the mechanical loss and atomic structure of amorphous TiO2-doped Ta2O5 coatings
journal, February 2013

Ring Configurations in a Random Network Model of Vitreous Silica
journal, March 1967

Infra-red absorption of the orthoborate ion
journal, January 1966

Memristor and selector devices fabricated from HfO 2−x N x
journal, April 2016

  • Murdoch, B. J.; McCulloch, D. G.; Ganesan, R.
  • Applied Physics Letters, Vol. 108, Issue 14
  • DOI: 10.1063/1.4945727

Hidden Structural Order in Orthorhombic Ta 2 O 5
journal, June 2013

Ion conducting properties of hydrogen-containing Ta2O5 thin films prepared by reactive sputtering
journal, October 2008

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