First-principles simulations of vibrational decay and lifetimes in a-Si:H and a-Si:D

Raymond Atta-Fynn, David A. Drabold, Stephen R. Elliott, and Parthapratim Biswas
Phys. Rev. B 95, 104205 – Published 21 March 2017

Abstract

Phonon lifetime in materials is an important observable that conveys basic information about structure, dynamics, and anharmonicity. Recent vibrational transient-grating measurements, using picosecond infrared pulses from free-electron lasers, have demonstrated that the vibrational-population decay rates of localized high-frequency stretching modes (HSMs) in hydrogenated and deuterated amorphous silicon (a-Si:H/D) increase with temperature and the vibrational energy redistributes among the bending modes of Si in a-Si:H/D. Motivated by this observation, we address the problem from first-principles density-functional calculations and study the time evolution of the vibrational-population decay in a-Si:H/D, the average decay times, and the possible decay channels for the redistribution of vibrational energy. The average lifetimes of the localized HSMs in a-Si:H and a-Si:D are found to be approximately 51–92 ps and 50–78 ps, respectively, in the temperature range of 25–200 K, which are consistent with experimental data. A weak temperature dependence of the vibrational-population decay rates has been observed via a slight increase of the decay rates with temperature, which can be attributed to stimulated emission and increased anharmonic coupling between the normal modes at high temperature.

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  • Received 11 January 2017
  • Revised 21 February 2017

DOI:https://doi.org/10.1103/PhysRevB.95.104205

©2017 American Physical Society

Physics Subject Headings (PhySH)

  1. Research Areas
  1. Physical Systems
Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Raymond Atta-Fynn1,*, David A. Drabold2,†, Stephen R. Elliott3,‡, and Parthapratim Biswas4,§

  • 1Department of Physics, University of Texas, Arlington, Texas 76019, USA
  • 2Department of Physics and Astronomy, Ohio University, Athens, Ohio 45701, USA
  • 3Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, United Kingdom
  • 4Department of Physics and Astronomy, The University of Southern Mississippi, Hattiesburg, Mississippi 39406, USA

  • *attafynn@uta.edu
  • drabold@ohio.edu
  • sre1@cam.ac.uk
  • §Corresponding author: partha.biswas@usm.edu

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Issue

Vol. 95, Iss. 10 — 1 March 2017

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