Temporally decoherent and spatially coherent vibrations in metal halide perovskites

Zhang, Depei; Hu, Xiao; Chen, Tianran; Abernathy, Douglas L.; Kajimoto, Ryoichi; Nakamura, Mitsutaka; Kofu, Maiko; Foley, Benjamin J.; Yoon, Mina; Choi, Joshua J.; Lee, Seung-Hun

doi:10.1103/physrevb.102.224310

Title: Temporally decoherent and spatially coherent vibrations in metal halide perovskites

Journal Article · Thu Dec 31 00:00:00 EST 2020 · Physical Review B

DOI:https://doi.org/10.1103/physrevb.102.224310· OSTI ID:1783011

Zhang, Depei ^[1]; Hu, Xiao ^[1]; Chen, Tianran ^[1];

^[2];

^[3]; Nakamura, Mitsutaka ^[3]; Kofu, Maiko ^[3]; Foley, Benjamin J. ^[1];

^[4]; Choi, Joshua J. ^[1]; Lee, Seung-Hun ^[1]

Univ. of Virginia, Charlottesville, VA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
J-PARC Center, Tokai (Japan). Materials and Life Science Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

The long carrier lifetime and defect tolerance in metal halide perovskites (MHPs) are major contributors to the superb performance of MHP optoelectronic devices. Large polarons were reported to be responsible for the long carrier lifetime. Yet microscopic mechanisms of the large polaron formation, including the so-called phonon melting, are still under debate. In this study, time-of-flight inelastic neutron scattering experiments and first-principles density-functional theory calculations were employed to investigate the lattice vibrations (or phonon dynamics) in methylammonium lead iodide, a prototypical example of MHPs. Our findings are that optical phonons lose temporal coherence gradually with increasing temperature which vanishes at the orthorhombic-to-tetragonal structural phase transition. Surprisingly, however, we found that the spatial coherence is still retained throughout the decoherence process. We argue that the temporally decoherent and spatially coherent vibrations contribute to the formation of large polarons in this metal halide perovskite.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0016144; AC02-05CH11231

OSTI ID:: 1783011

Journal Information:: Physical Review B, Vol. 102, Issue 22; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
optical phonons
phonons
polarons
perovskite
density functional calculations
inelastic neutron scattering

Title: Temporally decoherent and spatially coherent vibrations in metal halide perovskites

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