期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 42, 页码 13798-13801出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b08175
关键词
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资金
- CRK's Stephen J. Angello Professorship
- National Science Foundation [DGE-1321851]
- Frances Velay fellowship
- German Research Foundation [GE 2827/1-1]
- U.S. Office of Naval Research [N00014-14-1-0761]
- U.S. Air Force Office of Scientific Research PECASE award [FA9950-13-1-0157]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0002158]
- U.S. Department of Energy (DOE) [DE-SC0002158] Funding Source: U.S. Department of Energy (DOE)
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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