Screening in crystalline liquids protects energetic carriers in hybrid perovskites

Haiming Zhu; Kiyoshi Miyata; Yongping Fu; Jue Wang; Prakriti P Joshi; Daniel Niesner; Kristopher W Williams; Song Jin; X-Y Zhu

doi:10.1126/science.aaf9570

Screening in crystalline liquids protects energetic carriers in hybrid perovskites

Science. 2016 Sep 23;353(6306):1409-1413. doi: 10.1126/science.aaf9570.

Authors

Haiming Zhu¹, Kiyoshi Miyata¹, Yongping Fu², Jue Wang¹, Prakriti P Joshi¹, Daniel Niesner¹, Kristopher W Williams¹, Song Jin², X-Y Zhu³

Affiliations

¹ Department of Chemistry, Columbia University, New York, NY 10027, USA.
² Department of Chemistry, University of Wisconsin-Madison, Madison, WI 53706, USA.
³ Department of Chemistry, Columbia University, New York, NY 10027, USA. xyzhu@columbia.edu.

PMID: 27708033
DOI: 10.1126/science.aaf9570

Abstract

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.

Publication types

Research Support, U.S. Gov't, Non-P.H.S.