Light-Driven Extremely Nonlinear Bulk Photogalvanic Currents

We predict the generation of bulk photocurrents in materials driven by bichromatic fields that are circularly polarized and corotating. The nonlinear photocurrents have a fully controllable directionality and amplitude without requiring carrier-envelope-phase stabilization or few-cycle pulses, and can be generated with photon energies much smaller than the band gap (reducing heating in the photoconversion process). We demonstrate with ab initio calculations that the photocurrent generation mechanism is universal and arises in gaped materials (Si, diamond, MgO, hBN), in semimetals (graphene), and in two- and three-dimensional systems. Photocurrents are shown to rely on sub-laser-cycle asymmetries in the nonlinear response that build-up coherently from cycle to cycle as the conduction band is populated. Importantly, the photocurrents are always transverse to the major axis of the co-circular lasers regardless of the material’s structure and orientation (analogously to a Hall current), which we find originates from a generalized time-reversal symmetry in the driven system. At high laser powers (∼1013 W/cm2) this symmetry can be spontaneously broken by vast electronic excitations, which is accompanied by an onset of carrier-envelope-phase sensitivity and ultrafast many-body effects. Our results are directly applicable for efficient light-driven control of electronics, and for enhancing sub-band-gap bulk photogalvanic effects