Ultrafast Control of Excitonic Rashba Fine Structure by Phonon Coherence in the Metal Halide Perovskite CH3NH3PbI3

Autor: Jigang Wang, Yongxin Yao, Zhaoyu Liu, Xu Yang, Yanfa Yan, Zhaoning Song, Richard H. J. Kim, Jin Zhao, Liang Luo, Chuankun Huang, Yuejiang Shi, Chirag Vaswani, Dinusha Herath Mudiyanselage, Di Cheng, Joong-Mok Park, Xin Zhao, Kai-Ming Ho
Rok vydání: 2020
Předmět:
Zdroj: Physical Review Letters. 124
ISSN: 1079-7114
0031-9007
DOI: 10.1103/physrevlett.124.157401
Popis: We discover hidden Rashba fine structure in ${\mathrm{CH}}_{3}{\mathrm{NH}}_{3}{\mathrm{PbI}}_{3}$ and demonstrate its quantum control by vibrational coherence through symmetry-selective vibronic (electron-phonon) coupling. Above a critical threshold of a single-cycle terahertz pump field, a Raman phonon mode distinctly modulates the middle excitonic states with persistent coherence for more than ten times longer than the ones on two sides that predominately couple to infrared phonons. These vibronic quantum beats, together with first-principles modeling of phonon periodically modulated Rashba parameters, identify a threefold excitonic fine structure splitting, i.e., optically forbidden, degenerate dark states in between two bright ones with a narrow, $\ensuremath{\sim}3\text{ }\text{ }\text{nm}$ splitting. Harnessing of vibronic quantum coherence and symmetry inspires light-perovskite quantum control and sub-THz-cycle ``Rashba engineering'' of spin-split bands for ultimate multifunction device.
Databáze: OpenAIRE