Non-radiative luminescence decay with self-trapped hole migration in strontium titanate: Interplay between optical and transport properties

Crespillo, Miguel L.; Graham, Joseph T.; Agulló-López, F.; Zhang, Yanwen; Weber, William J.

doi:10.1016/j.apmt.2021.101041

Non-radiative luminescence decay with self-trapped hole migration in strontium titanate: Interplay between optical and transport properties

Journal Article · Fri Apr 23 00:00:00 EDT 2021 · Applied Materials Today

DOI:https://doi.org/10.1016/j.apmt.2021.101041· OSTI ID:1807226

Crespillo, Miguel L. ^[1]; Graham, Joseph T. ^[2]; Agulló-López, F. ^[3]; ^[4]; ^[5]

Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Missouri Univ. of Science and Technology, Rolla, MO (United States). Dept. of Nuclear Engineering and Radiation Science; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Autonomous Univ. of Madrid (Spain). Centro de Microanálisis de Materiales
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division

A novel model for the non-radiative decay of self-trapped excitons (STEs) in the advanced functional oxide SrTiO3 is proposed and supported by experimental observations. The study is based on the initial ionoluminescence stage for STE emission at 2.5 eV, and its dependence on temperature and electronic excitation rate under energetic heavy-ion irradiation. For all temperatures, this initial stage reaches rapidly a quasi-steady level, and then decreases as induced-structural damage increases. The quasi-steady luminescence exhibits a linear dependence on the excitation rate, suggesting a constant efficiency for STEs formation. An activation energy of 55 meV, essentially independent of the incident ion mass and energy of projectile-ion, is deduced from an Arrhenius-type relationship with irradiation temperature. This energy is in good agreement with experimental values, measured for non-radiative STE decay under ns-laser pulse excitation, and reasonably consistent with density functional theory calculations for migration of self-trapped holes (STHs) described by a small-polaron adiabatic hopping model. A new mechanism dealing with a non-radiative contribution to the STE transition is discussed, consisting of STH migration through thermally-activated hopping and annihilation with the STE-electron. Luminescence kinetics from the chromium intrinsic impurity strongly supports this model, being consistent with the annihilation of Cr³⁺ centers through recombination with migrating STHs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1807226

Journal Information:: Applied Materials Today, Journal Name: Applied Materials Today Journal Issue: NA Vol. 23; ISSN 2352-9407

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
activation energy
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Non-radiative luminescence decay with self-trapped hole migration in strontium titanate: Interplay between optical and transport properties

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