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The coherence of collective modes, such as phonons, and their modulation ofthe electronic states are long sought in complex systems, which is across-cutting issue in photovoltaics and quantum electronics. In photovoltaiccells and lasers based on metal halide perovskites, the presence of polaroniccoupling, i.e., photocarriers dressed by the macroscopic motion of chargedlattice, assisted by terahertz (THz) longitudinal optical (LO) phonons, hasbeen intensely studied yet still debated. This may be key for explaining theremarkable properties of the perovskite materials, e.g., defect tolerance, longcharge lifetimes and diffusion length. Here we use the intense single-cycle THzpulse with the peak electric field up to $E_{THz}=$1000\,kV/cm to drivecoherent band-edge oscillations at room temperature in CH$_3$NH$_3$PbI$_3$. Wereveal the oscillatory behavior dominantly to a specific quantized latticevibration mode at $\omega_{\mathrm{LO}}\sim$4 THz, being both dipole andmomentum forbidden. THz-driven coherent dynamics exhibits distinguishingfeatures: the room temperature coherent oscillations at $\omega_{\mathrm{LO}}$longer than 1 ps in both single crystals and thin films; the {\emmode-selective} modulation of different band edge states assisted byelectron-phonon ($e$-$ph$) interaction; {\em dynamic mode splitting} controlledby temperature due to entropy and anharmonicity of organic cations. Our resultsdemonstrate intense THz-driven coherent band-edge modulation as a powerfulprobe of electron-lattice coupling phenomena and provide compellingimplications for polaron correlations in perovskites.

Coherent Band-Edge Oscillations and Dynamic LO Phonon Mode Splitting as Evidence for Polaronic Coupling in Perovskites