You are here

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

TitleUltrafast terahertz snapshots of excitonic Rydberg states and electronic coherence in an organometal halide perovskite
Publication TypeJournal Article
Year of Publication2017
AuthorsLuo, L, Men, L, Liu, ZY, Mudryk, Y, Zhao, X, Yao, YX, Park, JM, Shinar, R, Shinar, J, Ho, KM, Perakis, IE, Vela, J, Wang, JG
JournalNature Communications
Volume8
Pagination15565
Date Published06
Type of ArticleArticle
ISBN Number2041-1723
Accession NumberWOS:000402513300001
Keywordsabsorption, carrier dynamics, ch3nh3pbi3, energy, lengths, phase-transition, single-crystal, Spectroscopy, Technology - Other Topics
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 onand off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes. The nearly similar to 1 ps dephasing time, efficient electron scattering with discrete terahertz phonons and intermediate binding energy of similar to 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.

DOI10.1038/ncomms15565
Custom 1

Photonics

Custom 2

Nanodomains