期刊
PHYSICAL REVIEW LETTERS
卷 124, 期 15, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.124.157401
关键词
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资金
- Ames Laboratory, the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division [DE-AC02-07CH11358]
- National Science Foundation [1611454, DMR-1807818]
- National Natural Science Foundation of China [11620101003]
- National Key R&D Program of China [2016YFA0200604, 2017YFA0204904]
- Directorate For Engineering
- Div Of Electrical, Commun & Cyber Sys [1611454] Funding Source: National Science Foundation
We discover hidden Rashba fine structure in CH3NH3PbI3 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, similar to 3 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.
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