Coherent charge-phonon correlations and exciton dynamics in orthorhombic CH3NH3PbI3 measured by ultrafast multi-THz spectroscopy

Lan, Yang; Tao, Xixi; Kong, Xianghua; He, Yihui; Zheng, Xiaohong; Sutton, Mark; Kanatzidis, Mercouri G.; Guo, Hong; Cooke, David G.

doi:10.1063/1.5127992

Coherent charge-phonon correlations and exciton dynamics in orthorhombic CH₃NH₃PbI₃ measured by ultrafast multi-THz spectroscopy

Journal Article · Wed Dec 04 00:00:00 EST 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5127992· OSTI ID:1802377

^[1]; Tao, Xixi ^[2]; Kong, Xianghua ^[3]; He, Yihui ^[4]; ^[5]; Sutton, Mark ^[3]; Kanatzidis, Mercouri G. ^[4]; Guo, Hong ^[3]; ^[3]

McGill Univ., Montreal, QC (Canada); OSTI
McGill Univ., Montreal, QC (Canada); Chinese Academy of Sciences (CAS), Hefei (China); Univ. of Science and Technology of China, Hefei (China)
McGill Univ., Montreal, QC (Canada)
Northwestern Univ., Evanston, IL (United States)
Chinese Academy of Sciences (CAS), Hefei (China); Univ. of Science and Technology of China, Hefei (China)

We use time-resolved multi-terahertz spectroscopy for the range 4–40 meV to probe coherent and incoherent ultrafast charge carrier and exciton dynamics in the low temperature orthorhombic phase of the hybrid metal halide perovskite CH₃NH₃PbI₃. Time- and energy-resolved terahertz reflectivity maps reveal strongly damped but coherent oscillations in the 2–4 THz reststrahlen band, indicating charge coupling to a distribution of low energy phonon modes centered at 0.9 THz (3.7 meV or 30 cm^-1). First-principles calculations reveal that these modes are entirely of mixed organic/inorganic sublattice character, with the power spectrum of the coherent oscillations showing a high frequency cutoff just at the onset of organic cation-only vibrations. Two anomalous reflectivity signatures are observed which are not phonon related, which we assign to a free exciton at 12 meV appearing on a 0.5 ps time scale and a defect bound exciton at 29–32 meV appearing on slower 1 ps time scale. Our measurements reveal the coherent coupling of charges to low energy vibrations of mixed sublattice character and the presence of two distinct populations of free and bound excitons at low temperatures.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0012541

OSTI ID:: 1802377

Alternate ID(s):: OSTI ID: 1577015

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 151; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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