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Title: Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation

Abstract

Lead halide perovskites have been demonstrated as high performance materials in solar cells and light-emitting devices. These materials are characterized by coherent band transport expected from crystalline semiconductors, but dielectric responses and phonon dynamics typical of liquids. This “crystal-liquid” duality implies that lead halide perovskites belong to phonon glass electron crystals, a class of materials believed to make the most efficient thermoelectrics. We show that the crystal-liquid duality and the resulting dielectric response are responsible for large polaron formation and screening of charge carriers, leading to defect tolerance, moderate charge carrier mobility, and radiative recombination properties. Large polaron formation, along with the phonon glass character, may also explain the marked reduction in hot carrier cooling rates in these materials.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Columbia Univ., New York, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1499930
Grant/Contract Number:  
[SC0010692]
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
[ Journal Volume: 3; Journal Issue: 10]; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY

Citation Formats

Miyata, Kiyoshi, Atallah, Timothy L., and Zhu, X. -Y. Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation. United States: N. p., 2017. Web. doi:10.1126/sciadv.1701469.
Miyata, Kiyoshi, Atallah, Timothy L., & Zhu, X. -Y. Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation. United States. doi:10.1126/sciadv.1701469.
Miyata, Kiyoshi, Atallah, Timothy L., and Zhu, X. -Y. Fri . "Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation". United States. doi:10.1126/sciadv.1701469. https://www.osti.gov/servlets/purl/1499930.
@article{osti_1499930,
title = {Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation},
author = {Miyata, Kiyoshi and Atallah, Timothy L. and Zhu, X. -Y.},
abstractNote = {Lead halide perovskites have been demonstrated as high performance materials in solar cells and light-emitting devices. These materials are characterized by coherent band transport expected from crystalline semiconductors, but dielectric responses and phonon dynamics typical of liquids. This “crystal-liquid” duality implies that lead halide perovskites belong to phonon glass electron crystals, a class of materials believed to make the most efficient thermoelectrics. We show that the crystal-liquid duality and the resulting dielectric response are responsible for large polaron formation and screening of charge carriers, leading to defect tolerance, moderate charge carrier mobility, and radiative recombination properties. Large polaron formation, along with the phonon glass character, may also explain the marked reduction in hot carrier cooling rates in these materials.},
doi = {10.1126/sciadv.1701469},
journal = {Science Advances},
number = [10],
volume = [3],
place = {United States},
year = {2017},
month = {10}
}

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Cited by: 68 works
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Figures / Tables:

Fig. 1 Fig. 1: Structure of CH3NH3PbX3 perovskite. It consists of a framework of corner-sharing lead (gray) halide (purple) octahedrals and the CH3NH3⁺ cation (black, blue, and white) in the nanocage.

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Appealing Perspectives of Hybrid Lead–Iodide Perovskites as Thermoelectric Materials
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Organic Cations Might Not Be Essential to the Remarkable Properties of Band Edge Carriers in Lead Halide Perovskites
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A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells
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Observation of a hot-phonon bottleneck in lead-iodide perovskites
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Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells
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Calculating polaron mobility in halide perovskites
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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.