First principles calculations of optical properties for oxygen vacancies in binary metal oxides

Strand, Jack and Chulkov, Sergey and Watkins, Matthew and Shluger, Alexander (2019) First principles calculations of optical properties for oxygen vacancies in binary metal oxides. Journal of Chemical Physics, 150 (4). ISSN 0021-9606

Full content URL: https://doi.org/10.1063/1.5078682

Documents
First principles calculations of optical properties for oxygen vacancies in binary metal oxides
Accepted Manuscript
[img]
[Download]
[img] PDF
First_principles_calculations_of_optical_properties_for_oxygen_vacancies_in_binary_metal_oxides.pdf - Whole Document

1MB
Item Type:Article
Item Status:Live Archive

Abstract

Using an advanced computational methodology implemented in CP2K, a non-local PBE0-TC-LRC density functional and the recently implemented linear response formulation of the Time-dependent Density Functional Theory equations, we test the interpretation of the optical absorption and photoluminescence signatures attributed by previous experimental and theoretical studies to O-vacancies in two widely used oxides—cubic MgO and monoclinic (m)-HfO2. The results obtained in large periodic cells including up to 1000 atoms emphasize the importance of accurate predictions of defect-induced lattice distortions. They confirm that optical transitions of O-vacancies in 0, +1, and +2 charge states in MgO all have energies close to 5 eV. We test the models of photoluminescence of O-vacancies proposed in the literature. The photoluminescence of V+2O centers in m-HfO2 is predicted to peak at 3.7 eV and originate from radiative tunneling transition between a V+1O center and a self-trapped hole created by the 5.2 eV excitation.

Keywords:Photoluminescence Transition radiation Crystallographic defects Computational methods Optical properties Density functional theory Optical absorption
Subjects:F Physical Sciences > F343 Computational Physics
F Physical Sciences > F170 Physical Chemistry
Divisions:College of Science > School of Mathematics and Physics
ID Code:35236
Deposited On:08 Apr 2019 13:36

Repository Staff Only: item control page