Oxidation state and interfacial effects on oxygen vacancies in tantalum pentoxide

Bondi, Robert J.; Marinella, Matthew J.

doi:10.1063/1.4913206

Title: Oxidation state and interfacial effects on oxygen vacancies in tantalum pentoxide

Journal Article · Sat Feb 28 00:00:00 EST 2015 · Journal of Applied Physics

DOI:https://doi.org/10.1063/1.4913206· OSTI ID:1184499

Bondi, Robert J. ^[1]; Marinella, Matthew J. ^[1]

Sandia National Laboratories (SNL), Albuquerque, NM (United States)

First-principles density-functional theory (DFT) calculations are used to study the atomistic structure, structural energetics, and electron density near the O monovacancy (V_Oⁿ; n=0,1+,2+) in both bulk, amorphous tantalum pentoxide (a-Ta₂O₅) and also at vacuum and metallic Ta interfaces. We calculate multivariate vacancy formation energies to evaluate stability as a function of oxidation state, distance from interface plane, and Fermi energy. V_Oⁿ of all oxidation states preferentially segregate at both Ta and vacuum interfaces, where the metallic interface exhibits global formation energy minima. In a-Ta₂O₅, V_O⁰ are characterized by structural contraction and electron density localization, while V_O²⁺ promote structural expansion and are depleted of electron density. In contrast, interfacial V_O⁰ and V_O²⁺ show nearly indistinguishable ionic and electronic signatures indicative of a reduced V_O center. Interfacial V_O²⁺ extract electron density from metallic Ta indicating V_O²⁺ is spontaneously reduced at the expense of the metal. This oxidation/reduction behavior suggests careful selection and processing of both oxide layer and metal electrodes for engineering memristor device operation.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1184499

Alternate ID(s):: OSTI ID: 1228560

Report Number(s):: SAND-2014-18988J; JAPIAU; 540613

Journal Information:: Journal of Applied Physics, Vol. 117, Issue 8; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 7 works

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