Phonon lifetimes and mode softening in cubic Cs2AgBiBr6

<h2>Summary</h2> Metal halide perovskites (MHPs) have emerged as noteworthy candidates for photovoltaic applications in recent years. Their high power-conversion efficiency is largely attributed to the structure-function relationship, which is not well understood. In this study, we examine the low-frequency phonons of the double perovskite <mml:math><mml:mrow><mml:mrow>Cs</mml:mrow><mml:mn>2</mml:mn>AgBiBr<mml:mn>6</mml:mn></mml:mrow></mml:math> using neutron inelastic scattering. We find that the acoustic phonon lifetimes decrease from 16 to 3 ps along <mml:math><mml:mrow><mml:mi>Γ</mml:mi></mml:mrow></mml:math> to <mml:math><mml:mrow><mml:mi>X</mml:mi></mml:mrow></mml:math>, which is indicative of significant anharmonicity that contributes to the ultralow thermal conductivity. Additionally, we observe a linear temperature dependence of the square of the zone-center soft optical phonon energy, which is consistent with a weakly first-order displacive cubic-tetragonal structural phase transition. These results provide a deeper understanding of the lattice dynamics and phase transitions in MHPs as well as the effects of anharmonicity by comparison with prototypical hybrid organic-inorganic MHPs, (<mml:math><mml:mrow>CH<mml:mn>3</mml:mn>NH<mml:mn>3</mml:mn></mml:mrow></mml:math>) <mml:math><mml:mrow><mml:mrow>PbX</mml:mrow><mml:mn>3</mml:mn></mml:mrow></mml:math> (X = Br, I).

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Publication Details

Journal
Newton
Published
2025-05-09
DOI
https://doi.org/10.1016/j.newton.2025.100097
Citations
2
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
1.46

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article

Phonon lifetimes and mode softening in cubic Cs2AgBiBr6

Johan Klarbring, J. A. Rodriguez‐Rivera, P. M. Gehring, Michael F. Toney et al.
2 citations
Newton
Perovskite Materials and Applications
1.46
article

Phonon lifetimes and mode softening in cubic Cs2AgBiBr6

Johan Klarbring, J. A. Rodriguez‐Rivera, P. M. Gehring, Michael F. Toney, Julian A. Vigil, Tao Hong, Nicholas J. Weadock, Adam H. Slavney, Hemamala I. Karunadasa, Zihan Zhang
article en
2 citations

Abstract

<h2>Summary</h2> Metal halide perovskites (MHPs) have emerged as noteworthy candidates for photovoltaic applications in recent years. Their high power-conversion efficiency is largely attributed to the structure-function relationship, which is not well understood. In this study, we examine the low-frequency phonons of the double perovskite <mml:math><mml:mrow><mml:mrow>Cs</mml:mrow><mml:mn>2</mml:mn>AgBiBr<mml:mn>6</mml:mn></mml:mrow></mml:math> using neutron inelastic scattering. We find that the acoustic phonon lifetimes decrease from 16 to 3 ps along <mml:math><mml:mrow><mml:mi>Γ</mml:mi></mml:mrow></mml:math> to <mml:math><mml:mrow><mml:mi>X</mml:mi></mml:mrow></mml:math>, which is indicative of significant anharmonicity that contributes to the ultralow thermal conductivity. Additionally, we observe a linear temperature dependence of the square of the zone-center soft optical phonon energy, which is consistent with a weakly first-order displacive cubic-tetragonal structural phase transition. These results provide a deeper understanding of the lattice dynamics and phase transitions in MHPs as well as the effects of anharmonicity by comparison with prototypical hybrid organic-inorganic MHPs, (<mml:math><mml:mrow>CH<mml:mn>3</mml:mn>NH<mml:mn>3</mml:mn></mml:mrow></mml:math>) <mml:math><mml:mrow><mml:mrow>PbX</mml:mrow><mml:mn>3</mml:mn></mml:mrow></mml:math> (X = Br, I).

NewtonVol. 1(4)
Linköping University (SE), Oak Ridge National Laboratory (US), National Institute of Standards and Technology (US), University of Colorado Boulder (US), SLAC National Accelerator Laboratory (US), NIST Center for Neutron Research (US), University of Maryland, College Park (US), Stanford University (US)
National Science Foundation, U.S. Department of Energy, Center for Hybrid Organic Inorganic Semiconductors for Energy, National Institute of Standards and Technology, Office of Science, Division of Materials Research, Basic Energy Sciences, Oak Ridge National Laboratory, Division of Materials Sciences and Engineering
Openalex Percentile: Top 18%
Perovskite Materials and Applications
1.46
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