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

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

doi:10.1038/ncomms15565

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

Journal Article · Thu Jun 01 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/ncomms15565· OSTI ID:1363630

Luo, Liang ^[1]; Men, Long ^[1]; Liu, Zhaoyu ^[1]; Mudryk, Yaroslav ^[1]; ^[1]; Yao, Yongxin ^[1]; Park, Joong M. ^[1]; Shinar, Ruth ^[1]; Shinar, Joseph ^[1]; Ho, Kai -Ming ^[1]; Perakis, Ilias E. ^[2]; ^[1]; Wang, Jigang ^[1]

Ames Lab. and Iowa State Univ., Ames, IA (United States)
Univ. of Alabama, Birmingham, AL (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1363630

Report Number(s):: IS-J--9302; ncomms15565

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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