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Title: Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach

Abstract

Here, we study the temperature-dependent phonon modes of the organometallic lead iodide perovskite CH 3NH 3PbI 3 thin film across the terahertz (0.5–3 THz) and temperature (20–300 K) ranges. These modes are related to the vibration of the Pb–I bonds. We found that two phonon modes in the tetragonal phase at room temperature split into four modes in the low-temperature orthorhombic phase. By use of the Lorentz model fitting, we also analyze the critical behavior of this phase transition. The carrier mobility values calculated from the low-temperature phonon mode frequencies, via two theoretical approaches, are found to agree reasonably with the experimental value (~2000 cm 2 V –1 s –1) from a previous time-resolved THz spectroscopy work. Thus, we have established a possible link between terahertz phonon modes and the transport properties of perovskite-based solar cells.

Authors:
 [1];  [2];  [3];  [4];  [2];  [5];  [4]; ORCiD logo [6];  [7];  [2];  [2]
  1. King Mongkut's Univ. of Technology, Bangkok (Thailand). Theoretical and Computational Science Center (TaCS)
  2. Nanyang Technological Univ. (Singapore). School of Physics and Mathematics Sciences
  3. Nanyang Technological Univ. (Singapore). School of Physics and Mathematics Sciences; Federal Inst. of Technology in Lausanne (Switzlerland). Lab. of Photomolecular Sciences
  4. Nanyang Technological Univ. (Singapore). School of Materials Science and Engineering
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
  7. Nanyang Technological Univ. (Singapore). School of Physics and Mathematics Sciences; California Inst. of Technology (CalTech), Pasadena, CA (United States). Noyes Lab.
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1402594
Report Number(s):
LA-UR-15-27800
Journal ID: ISSN 1948-7185; TRN: US1703115
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; perovskite; phonon; solar cells; structural phase transition; terahertz time-domain spectroscopy; vibrational spectroscopy

Citation Formats

La-o-vorakiat, Chan, Xia, Huanxin, Kadro, Jeannette, Salim, Teddy, Zhao, Daming, Ahmed, Towfiq, Lam, Yeng Ming, Zhu, Jian-Xin, Marcus, Rudolph A., Michel-Beyerle, Maria-Elisabeth, and Chia, Elbert E. M. Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach. United States: N. p., 2015. Web. doi:10.1021/acs.jpclett.5b02223.
La-o-vorakiat, Chan, Xia, Huanxin, Kadro, Jeannette, Salim, Teddy, Zhao, Daming, Ahmed, Towfiq, Lam, Yeng Ming, Zhu, Jian-Xin, Marcus, Rudolph A., Michel-Beyerle, Maria-Elisabeth, & Chia, Elbert E. M. Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach. United States. doi:10.1021/acs.jpclett.5b02223.
La-o-vorakiat, Chan, Xia, Huanxin, Kadro, Jeannette, Salim, Teddy, Zhao, Daming, Ahmed, Towfiq, Lam, Yeng Ming, Zhu, Jian-Xin, Marcus, Rudolph A., Michel-Beyerle, Maria-Elisabeth, and Chia, Elbert E. M. Thu . "Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach". United States. doi:10.1021/acs.jpclett.5b02223. https://www.osti.gov/servlets/purl/1402594.
@article{osti_1402594,
title = {Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach},
author = {La-o-vorakiat, Chan and Xia, Huanxin and Kadro, Jeannette and Salim, Teddy and Zhao, Daming and Ahmed, Towfiq and Lam, Yeng Ming and Zhu, Jian-Xin and Marcus, Rudolph A. and Michel-Beyerle, Maria-Elisabeth and Chia, Elbert E. M.},
abstractNote = {Here, we study the temperature-dependent phonon modes of the organometallic lead iodide perovskite CH3NH3PbI3 thin film across the terahertz (0.5–3 THz) and temperature (20–300 K) ranges. These modes are related to the vibration of the Pb–I bonds. We found that two phonon modes in the tetragonal phase at room temperature split into four modes in the low-temperature orthorhombic phase. By use of the Lorentz model fitting, we also analyze the critical behavior of this phase transition. The carrier mobility values calculated from the low-temperature phonon mode frequencies, via two theoretical approaches, are found to agree reasonably with the experimental value (~2000 cm2 V–1 s–1) from a previous time-resolved THz spectroscopy work. Thus, we have established a possible link between terahertz phonon modes and the transport properties of perovskite-based solar cells.},
doi = {10.1021/acs.jpclett.5b02223},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 1,
volume = 7,
place = {United States},
year = {2015},
month = {12}
}

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