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

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. Furthermore 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.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ; ORCiD logo [1] ;  [1]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States)
  2. Univ. of Alabama, Birmingham, AL (United States)
Publication Date:
Report Number(s):
IS-J-9302
Journal ID: ISSN 2041-1723; ncomms15565
Grant/Contract Number:
AC02-07CH11358
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY; semiconductors; solar cells; terahertz optics; ultrafast photonics
OSTI Identifier:
1363630

Luo, Liang, Men, Long, Liu, Zhaoyu, Mudryk, Yaroslav, Zhao, Xin, Yao, Yongxin, Park, Joong M., Shinar, Ruth, Shinar, Joseph, Ho, Kai -Ming, Perakis, Ilias E., Vela, Javier, and Wang, Jigang. Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite. United States: N. p., Web. doi:10.1038/ncomms15565.
Luo, Liang, Men, Long, Liu, Zhaoyu, Mudryk, Yaroslav, Zhao, Xin, Yao, Yongxin, Park, Joong M., Shinar, Ruth, Shinar, Joseph, Ho, Kai -Ming, Perakis, Ilias E., Vela, Javier, & Wang, Jigang. Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite. United States. doi:10.1038/ncomms15565.
Luo, Liang, Men, Long, Liu, Zhaoyu, Mudryk, Yaroslav, Zhao, Xin, Yao, Yongxin, Park, Joong M., Shinar, Ruth, Shinar, Joseph, Ho, Kai -Ming, Perakis, Ilias E., Vela, Javier, and Wang, Jigang. 2017. "Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite". United States. doi:10.1038/ncomms15565. https://www.osti.gov/servlets/purl/1363630.
@article{osti_1363630,
title = {Ultrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite},
author = {Luo, Liang and Men, Long and Liu, Zhaoyu and Mudryk, Yaroslav and Zhao, Xin and Yao, Yongxin and Park, Joong M. and Shinar, Ruth and Shinar, Joseph and Ho, Kai -Ming and Perakis, Ilias E. and Vela, Javier and Wang, Jigang},
abstractNote = {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. Furthermore 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.},
doi = {10.1038/ncomms15565},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {6}
}