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Title: Ab initio calculations of the rate of carrier trapping and release at dopant sites in NaI: Tl beyond the harmonic approximation

Abstract

We present ab initio calculations of electron capture and release coefficients as a function of temperature for Tl dopants in the widely used scintillator NaI, which is a soft ionic crystal. The modelled capture and release events occur by transitions mediated by multiple phonon absorption and emission between states with significantly different local geometries around the trapping site. We demonstrate that such transitions are not well-described by the normal harmonic approximation to the nuclear dynamics. We avoid the harmonic approximation by numerically solving the vibrational Schrödinger equation for the motion along/of a single effective phonon coordinate. The localized trapped state is not correctly described by semilocal density functionals, so we employ a hybrid functional tuned to reproduce the band gap and lattice constant of the host material. Our calculations, which combine plane-wave and cluster electronic structure methods in a novel way, are in reasonable agreement with available experimental data for detrapping and predict an unusual temperature dependence for trapping rates.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]
  1. BATTELLE (PACIFIC NW LAB)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1597649
Report Number(s):
PNNL-SA-145002
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 101; Journal Issue: 2
Country of Publication:
United States
Language:
English

Citation Formats

Prange, Micah P., Govind, Niranjan, and Kerisit, Sebastien N. Ab initio calculations of the rate of carrier trapping and release at dopant sites in NaI: Tl beyond the harmonic approximation. United States: N. p., 2020. Web. doi:10.1103/PhysRevB.101.024304.
Prange, Micah P., Govind, Niranjan, & Kerisit, Sebastien N. Ab initio calculations of the rate of carrier trapping and release at dopant sites in NaI: Tl beyond the harmonic approximation. United States. doi:10.1103/PhysRevB.101.024304.
Prange, Micah P., Govind, Niranjan, and Kerisit, Sebastien N. Wed . "Ab initio calculations of the rate of carrier trapping and release at dopant sites in NaI: Tl beyond the harmonic approximation". United States. doi:10.1103/PhysRevB.101.024304.
@article{osti_1597649,
title = {Ab initio calculations of the rate of carrier trapping and release at dopant sites in NaI: Tl beyond the harmonic approximation},
author = {Prange, Micah P. and Govind, Niranjan and Kerisit, Sebastien N.},
abstractNote = {We present ab initio calculations of electron capture and release coefficients as a function of temperature for Tl dopants in the widely used scintillator NaI, which is a soft ionic crystal. The modelled capture and release events occur by transitions mediated by multiple phonon absorption and emission between states with significantly different local geometries around the trapping site. We demonstrate that such transitions are not well-described by the normal harmonic approximation to the nuclear dynamics. We avoid the harmonic approximation by numerically solving the vibrational Schrödinger equation for the motion along/of a single effective phonon coordinate. The localized trapped state is not correctly described by semilocal density functionals, so we employ a hybrid functional tuned to reproduce the band gap and lattice constant of the host material. Our calculations, which combine plane-wave and cluster electronic structure methods in a novel way, are in reasonable agreement with available experimental data for detrapping and predict an unusual temperature dependence for trapping rates.},
doi = {10.1103/PhysRevB.101.024304},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 2,
volume = 101,
place = {United States},
year = {2020},
month = {1}
}

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