Screening in crystalline liquids protects energetic carriers in hybrid perovskites

Hybrid lead halide perovskites exhibit carrier properties that resemble those of pristine nonpolar semiconductors despite static and dynamic disorder, but how carriers are protected from efficient scattering with charged defects and optical phonons is unknown. Here, we reveal the carrier protection...

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Bibliographic Details
Published in:Science (American Association for the Advancement of Science) 2016-09, Vol.353 (6306), p.1409-1413
Main Authors: Zhu, Haiming, Miyata, Kiyoshi, Fu, Yongping, Wang, Jue, Joshi, Prakriti P., Niesner, Daniel, Williams, Kristopher W., Jin, Song, Zhu, X.-Y.
Format: Article
Language:English
Subjects:
Carriers
Cooling
Crystallization
Dynamics
Energy
Fluorescence
Hybridization
Liquids
Perovskite
Perovskites
Screening
Semiconductors
Solvation
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Summary:Hybrid lead halide perovskites exhibit carrier properties that resemble those of pristine nonpolar semiconductors despite static and dynamic disorder, but how carriers are protected from efficient scattering with charged defects and optical phonons is unknown. Here, we reveal the carrier protection mechanism by comparing three single-crystal lead bromide perovskites: CH₃NH₃PbBr₃, CH(NH₂)₂PbBr₃, and CsPbBr₃. We observed hot fluorescence emission from energetic carriers with ~10²-picosecond lifetimes in CH₃NH₃PbBr₃ or CH(NH₂)₂PbBr₃, but not in CsPbBr₃. The hot fluorescence is correlated with liquid-like molecular reorientational motions, suggesting that dynamic screening protects energetic carriers via solvation or large polaron formation on time scales competitive with that of ultrafast cooling. Similar protections likely exist for band-edge carriers. The long-lived energetic carriers may enable hot-carrier solar cells with efficiencies exceeding the Shockley-Queisser limit.
ISSN:0036-8075
1095-9203
DOI:10.1126/science.aaf9570