Publication Date
4-17-2020
Department
Ames Laboratory; Physics and Astronomy
Campus Units
Ames Laboratory, Physics and Astronomy
OSTI ID+
1615115
Report Number
IS-J 10209
DOI
10.1103/PhysRevLett.124.157401
Journal Title
Physical Review Letters
Volume Number
124
Issue Number
15
First Page
157401
Abstract
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.
DOE Contract Number(s)
AC02-07CH11358
Language
en
Publisher
Iowa State University Digital Repository, Ames IA (United States)
