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Title: Experimental Phonon Dispersion and Lifetimes of Tetragonal CH 3NH 3PbI 3 Perovskite Crystals

Abstract

Hybrid organic–inorganic perovskites were reported to have ultralow thermal conductivity in recent studies. In this Letter, we report the first experimental phonon dispersion and lifetimes of tetragonal CH 3NH 3PbI 3 single crystals at both 200 and 300 K by high-energy resolution inelastic X-ray scattering, which enables a thorough understanding of the underlying mechanisms for the ultralow thermal conductivity. Notably, we observed unusual and significant phonon dips along the [100] and [110] directions at both temperatures. The ultralow thermal conductivity can be attributed to small group velocities due to ultrasoft acoustic modes and short phonon lifetimes originating from the strong acoustic-optical coupling. We further provided the structural origins for these peculiar phonon features. Moreover, our results and interpretation are consistent with the reported temperature-dependent trend for thermal conductivity of CH 3NH 3PbI 3. Lastly, our work offers critical guidelines for accelerating the design and discovery of novel hybrid materials for energy applications including photovoltaics and thermoelectrics.

Authors:
ORCiD logo [1];  [2];  [3];  [2];  [4]; ORCiD logo [5];  [1]
  1. Cornell Univ., Ithaca, NY (United States)
  2. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Illinois Inst. of Technology, Chicago, IL (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1491239
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ma, Hao, Ma, Yunwei, Wang, Heng, Slebodnick, Carla, Alatas, Ahmet, Urban, Jeffrey J., and Tian, Zhiting. Experimental Phonon Dispersion and Lifetimes of Tetragonal CH3NH3PbI3 Perovskite Crystals. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b03419.
Ma, Hao, Ma, Yunwei, Wang, Heng, Slebodnick, Carla, Alatas, Ahmet, Urban, Jeffrey J., & Tian, Zhiting. Experimental Phonon Dispersion and Lifetimes of Tetragonal CH3NH3PbI3 Perovskite Crystals. United States. doi:10.1021/acs.jpclett.8b03419.
Ma, Hao, Ma, Yunwei, Wang, Heng, Slebodnick, Carla, Alatas, Ahmet, Urban, Jeffrey J., and Tian, Zhiting. Sun . "Experimental Phonon Dispersion and Lifetimes of Tetragonal CH3NH3PbI3 Perovskite Crystals". United States. doi:10.1021/acs.jpclett.8b03419. https://www.osti.gov/servlets/purl/1491239.
@article{osti_1491239,
title = {Experimental Phonon Dispersion and Lifetimes of Tetragonal CH3NH3PbI3 Perovskite Crystals},
author = {Ma, Hao and Ma, Yunwei and Wang, Heng and Slebodnick, Carla and Alatas, Ahmet and Urban, Jeffrey J. and Tian, Zhiting},
abstractNote = {Hybrid organic–inorganic perovskites were reported to have ultralow thermal conductivity in recent studies. In this Letter, we report the first experimental phonon dispersion and lifetimes of tetragonal CH3NH3PbI3 single crystals at both 200 and 300 K by high-energy resolution inelastic X-ray scattering, which enables a thorough understanding of the underlying mechanisms for the ultralow thermal conductivity. Notably, we observed unusual and significant phonon dips along the [100] and [110] directions at both temperatures. The ultralow thermal conductivity can be attributed to small group velocities due to ultrasoft acoustic modes and short phonon lifetimes originating from the strong acoustic-optical coupling. We further provided the structural origins for these peculiar phonon features. Moreover, our results and interpretation are consistent with the reported temperature-dependent trend for thermal conductivity of CH3NH3PbI3. Lastly, our work offers critical guidelines for accelerating the design and discovery of novel hybrid materials for energy applications including photovoltaics and thermoelectrics.},
doi = {10.1021/acs.jpclett.8b03419},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 1,
volume = 10,
place = {United States},
year = {2018},
month = {12}
}

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Cited by: 3 works
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