Barriers to carriers: faults and recombination in non-stoichiometric perovskite scintillators

Talapatra, Anjana; Ghosh, Dibyajyoti; Uberuaga, Blas P.; Pilania, Ghanshyam

doi:10.1007/s10853-021-06294-2

Barriers to carriers: faults and recombination in non-stoichiometric perovskite scintillators

Journal Article · Fri Jul 16 00:00:00 UTC 2021 · Journal of Materials Science

DOI:https://doi.org/10.1007/s10853-021-06294-2· OSTI ID:1808353

Talapatra, Anjana; Ghosh, Dibyajyoti; ; Pilania, Ghanshyam

Abstract

Tuning the efficiency and speed of charge carrier recombination in inorganic scintillators can potentially improve their performance in diverse applications. Recent work suggests that this maybe be achieved via a two-phase scintillator AB that naturally phase separates into A -rich and B -rich domains. In addition, a favorable electronic structure and band-edge alignment such that the charge carriers are confined or are thermodynamically driven to preferentially accumulate in one of the two domains, might lead to an improved radiative recombination rate. Here, we use density functional theory computations and ab initio molecular dynamics (AIMD), including non-adiabatic molecular dynamics (NAMD) simulations, to examine an alternative phase structure and its potential impact on recombination. Using a model perovskite SrTiO $$$$_3$$$$ $_{3}$ system with one-, two- and three-dimensional Ruddlesden–Popper (RP) phases, we demonstrate that RP faults induce band structure changes in the material that can act as barriers to carrier transport. Our AIMD/NAMD simulations indicate competing effects of a lower mean free path (potentially enhancing the desired radiative recombination and overall scintillating efficiency) and faster non-radiative recombination (undesired) due to enhanced electron–phonon coupling in the faulted system. Full exploitation of such a rational design approach would require tuning of the effective scintillation efficiency by varying the perovskite chemistry using appropriate arrangements of RP faults in the bulk material. Finally, other effects, such as the tendency of point defects to segregate at the interface, that might affect the overall performance, are briefly discussed. We expect the basic results found here to apply to other nanostructured scintillators.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1808353

Alternate ID(s):: OSTI ID: 1811891

Report Number(s):: LA-UR--21-23719; PII: 6294

Journal Information:: Journal of Materials Science, Journal Name: Journal of Materials Science Journal Issue: 28 Vol. 56; ISSN 0022-2461

Publisher:: Springer Science + Business MediaCopyright Statement

Country of Publication:: United States

Language:: English

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