Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite

Liang Luo, Long Men, Zhaoyu Liu, Yaroslav Mudryk, Xin Zhao, Yongxin Yao, Joong M. Park, Ruth Shinar, Joseph Shinar, Kai-Ming Ho, Ilias E. Perakis, Javier Vela and Jigang Wang ()
Additional contact information
Liang Luo: Ames Laboratory, Iowa State University
Long Men: Iowa State University
Zhaoyu Liu: Ames Laboratory, Iowa State University
Yaroslav Mudryk: Ames Laboratory, Iowa State University
Xin Zhao: Ames Laboratory, Iowa State University
Yongxin Yao: Ames Laboratory, Iowa State University
Joong M. Park: Ames Laboratory, Iowa State University
Ruth Shinar: Ames Laboratory, Iowa State University
Joseph Shinar: Ames Laboratory, Iowa State University
Kai-Ming Ho: Ames Laboratory, Iowa State University
Ilias E. Perakis: University of Alabama at Birmingham
Javier Vela: Iowa State University
Jigang Wang: Ames Laboratory, Iowa State University

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract How photoexcitations evolve into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaics and optoelectronics. Until now, the initial quantum dynamics following photoexcitation remains elusive in the hybrid perovskite system. Here we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant, internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes. The nearly ∼1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of ∼13.5 meV in perovskites are distinct from conventional photovoltaic semiconductors. In addition to providing implications for coherent energy conversion, these are potentially relevant to the development of light-harvesting and electron-transport devices.

Date: 2017
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DOI: 10.1038/ncomms15565

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