Bulk photogalvanic current control and gap spectroscopy in 2D hexagonal materials

Two-dimensional (2D) hexagonal materials have been intensively explored for multiple optoelectronic applications such as spin current generation, all-optical valleytronics, and topological electronics. In the realm of strong-field and ultrafast light-driven phenomena, it was shown that tailored laser driving such as polychromatic or few-cycle pulses can drive robust bulk photogalvanic (BPG) currents originating from the <i>K</i>/<i>K</i>' valleys. We here explore the BPG effect in 2D systems in the strong-field regime and show that monochromatic elliptical pulses also generically generate such photocurrents. The resultant photocurrents exhibit both parallel and transverse (Hall-like) components, both highly sensitive to the laser parameters, providing photocurrent control knobs. Interestingly, we show that the photocurrent amplitude has a distinct behavior <i>vs.</i> the driving ellipticity that can be indicative of material properties such as the gap size at <i>K</i>/<i>K</i>', which should prove useful for novel forms of BPG-based spectroscopies. We demonstrate these effects also in benchmark <i>ab initio</i> simulations in monolayer hexagonal boron-nitride. Our work establishes new paths for controlling photocurrent responses in 2D systems that can also be used for multi-dimensional spectroscopy of ultrafast material properties through photocurrent measurements.