Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

被引：169

作者：

Wu, Xiaoxi ^{[1
]}

Tan, Liang Z. ^{[2
]}

Shen, Xiaozhe ^{[3
]}

Hu, Te ^{[4
]}

Miyata, Kiyoshi ^{[5
]}

Trinh, M. Tuan ^{[5
]}

Li, Renkai ^{[3
]}

Coffee, Ryan ^{[3
]}

Liu, Shi ^{[6
]}

Egger, David A. ^{[7
]}

Makasyuk, Igor ^{[3
]}

Zheng, Qiang ^{[3
]}

Fry, Alan ^{[3
]}

Robinson, Joseph S. ^{[3
]}

Smith, Matthew D. ^{[8
]}

Guzelturk, Burak ^{[1
]}

Karunadasa, Hemamala I. ^{[8
]}

Wang, Xijie ^{[3
]}

Zhu, Xiaoyang ^{[5
]}

Kronik, Leeor ^{[7
]}

Rappe, Andrew M. ^{[2
]}

Lindenberg, Aaron M. ^{[1
,4
,9
]}

机构：

[1] Stanford Inst Mat & Energy Sci, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[2] Univ Penn, Dept Chem, Makineni Theoret Labs, Philadelphia, PA 19104 USA

[3] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[4] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA

[5] Columbia Univ, Dept Chem, New York, NY 10027 USA

[6] Carnegie Inst Sci, Geophys Lab, Extreme Mat Initiat, Washington, DC 20015 USA

[7] Weizmann Inst Sci, Dept Mat & Interfaces, IL-76100 Rehovot, Israel

[8] Stanford Univ, Dept Chem, Stanford, CA 94305 USA

[9] PULSE Inst, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

来源：

SCIENCE ADVANCES | 2017年 / 3卷 / 07期

基金：

奥地利科学基金会;

关键词：

METHYLAMMONIUM LEAD IODIDE; PHASE-TRANSITIONS; HIGH-PERFORMANCE; ORGANIC CATIONS; SOLAR-CELLS; ELECTRON; TRANSPORT; DEGRADATION; MOBILITIES;

D O I：

10.1126/sciadv.1602388

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.

引用

页数：7

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