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Title: Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence

Abstract

Carrier dynamics in methylammonium lead halide (CH3NH3PbI3-xClx) perovskite thin films, of differing crystal morphology, are examined as functions of temperature and excitation wavelength. At room temperature, long-lived (> nanosecond) transient absorption signals indicate negligible carrier trapping. However, in measurements of ultrafast photoluminescence excited at 400 nm, a heretofore unexplained, large amplitude (50%-60%), 45 ps decay process is observed. This feature persists for temperatures down to the orthorhombic phase transition. Varying pump photon energy reveals that the fast, band-edge photoluminescence (PL) decay only appears for excitation ≥ 2.38 eV (520 nm), with larger amplitudes for higher pump energies. Lower photon-energy excitation yields slow dynamics consistent with negligible carrier trapping. Further, sub-bandgap two-photon pumping yields identical PL dynamics as direct absorption, signifying sensitivity to the total deposited energy and insensitivity to interfacial effects. Together with first principles electronic structure and ab initio molecular dynamics calculations, the results suggest the fast PL decay stems from excitation of high energy phonon modes associated with the organic sub-lattice that temporarily enhance wavefunction overlap within the inorganic component owing to atomic displacement, thereby transiently changing the PL radiative rate during thermalization. Furthermore, the fast PL decay relates a characteristic organic-to-inorganic sub-lattice equilibration timescale at optoelectronic-relevant excitationmore » energies.« less

Authors:
 [1];  [2];  [2];  [2];  [3];  [3];  [1];  [3];  [2];  [4]
+ Show Author Affiliations
  1. Northwestern Univ., Evanston, IL (United States)
  2. National Tsing-Hua Univ., Hsin Chu (Taiwan)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1367171
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 15; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; density functional theory; hybrid perovskite; transient absorption; transient photoluminescence

Citation Formats

Chang, Angela Y., Cho, Yi -Ju, Chen, Kuan -Chen, Chen, Chang -Wen, Kinaci, Alper, Diroll, Benjamin T., Wagner, Michael J., Chan, Maria K. Y., Lin, Hao -Wu, and Schaller, Richard D. Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence. United States: N. p., 2016. Web. doi:10.1002/aenm.201600422.
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Chang, Angela Y., Cho, Yi -Ju, Chen, Kuan -Chen, Chen, Chang -Wen, Kinaci, Alper, Diroll, Benjamin T., Wagner, Michael J., Chan, Maria K. Y., Lin, Hao -Wu, & Schaller, Richard D. Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence. United States. https://doi.org/10.1002/aenm.201600422
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Chang, Angela Y., Cho, Yi -Ju, Chen, Kuan -Chen, Chen, Chang -Wen, Kinaci, Alper, Diroll, Benjamin T., Wagner, Michael J., Chan, Maria K. Y., Lin, Hao -Wu, and Schaller, Richard D. Tue . "Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence". United States. https://doi.org/10.1002/aenm.201600422. https://www.osti.gov/servlets/purl/1367171.
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@article{osti_1367171,
title = {Slow Organic-to-Inorganic Sub-Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence},
author = {Chang, Angela Y. and Cho, Yi -Ju and Chen, Kuan -Chen and Chen, Chang -Wen and Kinaci, Alper and Diroll, Benjamin T. and Wagner, Michael J. and Chan, Maria K. Y. and Lin, Hao -Wu and Schaller, Richard D.},
abstractNote = {Carrier dynamics in methylammonium lead halide (CH3NH3PbI3-xClx) perovskite thin films, of differing crystal morphology, are examined as functions of temperature and excitation wavelength. At room temperature, long-lived (> nanosecond) transient absorption signals indicate negligible carrier trapping. However, in measurements of ultrafast photoluminescence excited at 400 nm, a heretofore unexplained, large amplitude (50%-60%), 45 ps decay process is observed. This feature persists for temperatures down to the orthorhombic phase transition. Varying pump photon energy reveals that the fast, band-edge photoluminescence (PL) decay only appears for excitation ≥ 2.38 eV (520 nm), with larger amplitudes for higher pump energies. Lower photon-energy excitation yields slow dynamics consistent with negligible carrier trapping. Further, sub-bandgap two-photon pumping yields identical PL dynamics as direct absorption, signifying sensitivity to the total deposited energy and insensitivity to interfacial effects. Together with first principles electronic structure and ab initio molecular dynamics calculations, the results suggest the fast PL decay stems from excitation of high energy phonon modes associated with the organic sub-lattice that temporarily enhance wavefunction overlap within the inorganic component owing to atomic displacement, thereby transiently changing the PL radiative rate during thermalization. Furthermore, the fast PL decay relates a characteristic organic-to-inorganic sub-lattice equilibration timescale at optoelectronic-relevant excitation energies.},
doi = {10.1002/aenm.201600422},
journal = {Advanced Energy Materials},
number = 15,
volume = 6,
place = {United States},
year = {Tue May 31 00:00:00 EDT 2016},
month = {Tue May 31 00:00:00 EDT 2016}
}
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https://doi.org/10.1002/aenm.201600422
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