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The interplay between crystal symmetry and its optical responses is at theheart of tremendous recent advances in light-matter interactions andapplications. Nonlinear optical processes that produce electric currents, forexample bulk photovoltaic (BPV) effect, require inversion symmetry brokenmaterials, such as ferroelectrics. In the current work, we demonstrate thatsuch BPV current could be generated in centrosymmetric materials withexcitation of out-of-equilibrium coherent phonons. This is much different fromthe generally studied static or thermally excited states. We show thatdepending on the oscillating phase factor of the coherent phonon,uni-directional static electric current can be observed, in addition to someterahertz alternating currents. We also generalize the conventional injectioncharge current into angular momentum (spin and orbital) degrees of freedom, anddemonstrate spin and orbital BPV photocurrents under coherent phonons. Ourfindings open the pathway to exploring the exotic phonon-photon-electroncoherent interactions in quantum materials.

Coherence Control of Directional Nonlinear Photocurrent in Spatially Symmetric Systems