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

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.

doi:10.1002/aenm.201600422

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

Journal Article · Tue May 31 00:00:00 EDT 2016 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201600422· OSTI ID:1367171

Chang, Angela Y. ^[1]; Cho, Yi -Ju ^[2]; Chen, Kuan -Chen ^[2]; Chen, Chang -Wen ^[2]; Kinaci, Alper ^[3]; Diroll, Benjamin T. ^[3]; Wagner, Michael J. ^[1]; Chan, Maria K. Y. ^[3]; Lin, Hao -Wu ^[2]; Schaller, Richard D. ^[4]

Northwestern Univ., Evanston, IL (United States)
National Tsing-Hua Univ., Hsin Chu (Taiwan)
Argonne National Lab. (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Carrier dynamics in methylammonium lead halide (CH₃NH₃PbI_3-xCl_x) 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1367171

Journal Information:: Advanced Energy Materials, Vol. 6, Issue 15; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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