Instantaneous Optical Selection Rule for Independent Control of Valley Currents

We reveal an instantaneous optical valley selection rule that illuminates the coupling between the instantaneous optical chirality of the driving laser field and the chirality of valley systems. Building on this principle, we propose and demonstrate that a single chirality-separated optical field, in which oppositely signed instantaneous optical chiralities are separated within an optical cycle, enables independent manipulation of currents from K and K^{'} valleys. Based on this scheme, we highlight two key example applications: (1) complete separation of currents from different valleys, yielding 100%-purity valley-polarized currents, and (2) generation of pure valley current with zero net charge flow. Our Letter offers a robust and highly controllable all-optical strategy for ultrafast engineering valley currents in the optical cycle timescale, paving a new avenue for valleytronics and quantum information technologies.