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Title: Role of atomistic structure in the stochastic nature of conductivity in substoichiometric tantalum pentoxide

In this study, first-principles calculations of electrical conductivity (σ o) are revisited to determine the atomistic origin of its stochasticity in a distribution generated from sampling 14 ab-initio molecular dynamics configurations from 10 independently quenched models (n = 140) of substoichiometric amorphous Ta 2O 5, where each structure contains a neutral O monovacancy (V O 0). Structural analysis revealed a distinct minimum Ta-Ta separation (dimer/trimer) corresponding to each V O 0 location. Bader charge decomposition using a commonality analysis approach based on the σ o distribution extremes revealed nanostructural signatures indicating that both the magnitude and distribution of cationic charge on the Ta subnetwork have a profound influence on σ o. Furthermore, visualization of local defect structures and their electron densities reinforces these conclusions and suggests σ o in the amorphous oxide is best suppressed by a highly charged, compact Ta cation shell that effectively screens and minimizes localized V O 0 interaction with the a-Ta 2O 5 network; conversely, delocalization of V O 0 corresponds to metallic character and high σ o. The random network of a-Ta 2O 5 provides countless variations of an ionic configuration scaffold in which small perturbations affect the electronic charge distribution and result inmore » a fixed-stoichiometry distribution of σ o; consequently, precisely controlled and highly repeatable oxide fabrication processes are likely paramount for advancement of resistive memory technologies.« less
Authors:
 [1] ;  [1] ;  [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
OSTI Identifier:
1248534
Report Number(s):
SAND-2016-0408J
Journal ID: ISSN 0021-8979; JAPIAU; 618608
Grant/Contract Number:
AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 119; Journal Issue: 12; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; tantalum; crystal structure; amorphous metals; electrical resistivity; carrier density