Single-Cycle Terahertz Driven Quantum Beats Reveal Symmetry-Selective Control of Excitonic Fine Structure in Perovskite.

Coherent time-frequency visualization reveals symmetry-selective vibronic (mixed exciton/lattice) quantum beats at cryogenic temperature after a single-cycle terahertz (THz) pumping in MAPbI$_3$ perovskite. Above a critical threshold, a Raman phonon mode distinctly modulates the very {\em narrow}, middle region with {\em persistent} coherence for more than ten times longer than the two sides that predominately couple to infrared (IR) modes. Such spectral-temporal asymmetry and selectivity are inconsistent with a single exciton model, but in excellent agreement with a simulation of the Rashba-type, {\em three-fold} fine structure splitting of middle optically-forbidden, dark excitonic states and two bright ones, lying above and below. These hint ``Rashba engineering", i.e., periodic brightening and modulation of the spin-split excitons and Rashba parameters, by phonon symmetry and coherence.