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The interaction of a single-cycle THz electric field with the topological insulator triggers strongly anharmonic lattice dynamics, promoting fully coherent energy transfer between the otherwise non-interacting Raman-active and infrared (IR)-active phononic modes. Two-dimensional (2D) THz spectroscopy combined with modeling based on the classical equations of motion and symmetry analysis reveals the multi-stage process underlying the excitation of the Raman-active phonon. In this process, the THz electric field first prepares a coherent IR-active phononic state and subsequently interacts with this state to efficiently excite the phonon.

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