Phonon Mode Transformation Across the Orthohombic-Tetragonal Phase Transition in a Lead Iodide Perovskite CH3NH3PbI3: A Terahertz Time-Domain Spectroscopy Approach

Chan La-o-Vorakiat; Huanxin Xia; Jeannette Kadro; Teddy Salim; Daming Zhao; Towfiq Ahmed; Yeng Ming Lam; Jian-Xin Zhu; Rudolph A Marcus; Maria-Elisabeth Michel-Beyerle; Elbert E M Chia

doi:10.1021/acs.jpclett.5b02223

Phonon Mode Transformation Across the Orthohombic-Tetragonal Phase Transition in a Lead Iodide Perovskite CH3NH3PbI3: A Terahertz Time-Domain Spectroscopy Approach

J Phys Chem Lett. 2016 Jan 7;7(1):1-6. doi: 10.1021/acs.jpclett.5b02223. Epub 2015 Dec 10.

Authors

Chan La-o-Vorakiat^{1

2

3}, Huanxin Xia⁴, Jeannette Kadro^{4

5}, Teddy Salim⁶, Daming Zhao⁴, Towfiq Ahmed⁷, Yeng Ming Lam⁶, Jian-Xin Zhu^{7

8}, Rudolph A Marcus^{4

9}, Maria-Elisabeth Michel-Beyerle⁴, Elbert E M Chia⁴

Affiliations

¹ Nanoscience and Nanotechnology Graduate Program, King Mongkut's University of Technology Thonburi , Bangkok 10140 Thailand.
² Theoretical and Computational Science Center (TaCS), Faculty of Science, King Mongkut's University of Technology Thonburi , Bangkok 10140 Thailand.
³ Faculty of Science, King Mongkut's University of Technology Thonburi , Bangkok 10140 Thailand.
⁴ Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University , 637371 Singapore.
⁵ Laboratoire des Sciences Photomoléculaires, Ecole Polytechnique Fédérale de Lausanne , Switzerland.
⁶ School of Materials Science and Engineering, Nanyang Technological University , 639798 Singapore.
⁷ Theoretical Division, Los Alamos National Laboratory , Los Alamos, New Mexico 87545, United States.
⁸ Center for Integrated Nanotechnologies, Los Alamos National Laboratories , Los Alamos, New Mexico 87545, United States.
⁹ Noyes Laboratory, California Institute of Technology , Pasadena, California 91125, United States.

PMID: 26633131
DOI: 10.1021/acs.jpclett.5b02223

Abstract

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 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.

Keywords: perovskite; phonon; solar cells; structural phase transition; terahertz time-domain spectroscopy; vibrational spectroscopy.

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.