Ultrafast Control of Excitonic Rashba Fine Structure by Phonon Coherences in a Metal Halide Perovskite CH${}_3$NH${}_3$PbI${}_3$

Abstract

We discover hidden Rashba fine structure in CH${}_3$NH${}_3$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 {\em 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 {\em three-fold} excitonic fine structure splitting, i.e., optically-forbidden, degenerate dark states in between two bright ones. Harnessing of vibronic quantum coherence and symmetry inspires light-perovskite quantum control and sub-THz-cycle "Rashba engineering" of spin-split bands for ultimate multi-function device.

arXiv commentPhys. Rev. Lett, in press (2020)

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Cited by in corpus (10)

• Discovery of Terahertz Second Harmonic Generation from Lightwave Acceleration of Symmetry--Breaking Nonlinear Supercurrents
• Light Quantum Control of Persisting Higgs Modes in Iron-Based Superconductors
• Dynamic Rashba-Dresselhaus Effect
• Chirality manipulation of ultrafast phase switchings in a correlated CDW-Weyl semimetal
• Visualizing heterogeneous dipole fields by terahertz light coupling in individual nano-junctions used in transmon qubits
• Photon echo polarimetry of excitons and biexcitons in a CH${}_3$NH${}_3$PbI${}_3$ perovskite single crystal
• Geometric pumping and dephasing at topological phase transition
• Ab-initio Simulations of Coherent Phonon-Induced Pumping of Carriers in Zirconium Pentatelluride
• Coherent Transfer of Lattice Entropy via Extreme Nonlinear Phononics in Metal Halide Perovskites
• Strongly Anharmonic Organic Cation Vibrations in Hybrid Lead Halide Perovskite CH3NH3PbI3 on Electronic Ground State