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Straus DB, Hurtado Parra S, Iotov N, et al. Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites. J Am Chem Soc. 2016;138(42):13798-13801doi: 10.1021/jacs.6b08175.
Straus, D. B., Hurtado Parra, S., Iotov, N., Gebhardt, J., Rappe, A. M., Subotnik, J. E., Kikkawa, J. M., & Kagan, C. R. (2016). Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites. Journal of the American Chemical Society, 138(42), 13798-13801. https://doi.org/10.1021/jacs.6b08175
Straus, Daniel B, et al. "Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites." Journal of the American Chemical Society vol. 138,42 (2016): 13798-13801. doi: https://doi.org/10.1021/jacs.6b08175
Straus DB, Hurtado Parra S, Iotov N, Gebhardt J, Rappe AM, Subotnik JE, Kikkawa JM, Kagan CR. Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites. J Am Chem Soc. 2016 Oct 26;138(42):13798-13801. doi: 10.1021/jacs.6b08175. Epub 2016 Oct 11. PMID: 27706940.
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J Am Chem Soc. 2016 Oct 26;138(42):13798-13801. doi: 10.1021/jacs.6b08175. Epub 2016 Oct 11.

Direct Observation of Electron-Phonon Coupling and Slow Vibrational Relaxation in Organic-Inorganic Hybrid Perovskites.

Journal of the American Chemical Society

Daniel B Straus, Sebastian Hurtado Parra, Natasha Iotov, Julian Gebhardt, Andrew M Rappe, Joseph E Subotnik, James M Kikkawa, Cherie R Kagan

Affiliations

  1. Departments of †Chemistry, ‡Physics and Astronomy, §Materials Science and Engineering, and ?Electrical and Systems Engineering, University of Pennsylvania , Philadelphia, Pennsylvania 19104, United States.

PMID: 27706940 DOI: 10.1021/jacs.6b08175

Abstract

Quantum and dielectric confinement effects in Ruddlesden-Popper 2D hybrid perovskites create excitons with a binding energy exceeding 150 meV. We exploit the large exciton binding energy to study exciton and carrier dynamics as well as electron-phonon coupling (EPC) in hybrid perovskites using absorption and photoluminescence (PL) spectroscopies. At temperatures <75 K, we resolve splitting of the excitonic absorption and PL into multiple regularly spaced resonances every 40-46 meV, consistent with EPC to phonons located on the organic cation. We also resolve resonances with a 14 meV spacing, in accord with coupling to phonons with mixed organic and inorganic character. These assignments are supported by density-functional theory calculations. Hot exciton PL and time-resolved PL measurements show that vibrational relaxation occurs on a picosecond time scale competitive with that for PL. At temperatures >75 K, excitonic absorption and PL exhibit homogeneous broadening. While absorption remains homogeneous, PL becomes inhomogeneous at temperatures <75K, which we speculate is caused by the formation and subsequent dynamics of a polaronic exciton.

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