Direct spatiotemporal imaging of carriers reveals a long-lived bulk photovoltaic mechanism

Abstract

The bulk photovoltaic effect (BPVE), a manifestation of broken centrosymmetry, has attracted interest as a probe of the symmetry and quantum geometry of materials, and for use in photovoltaic and optoelectronic devices. However, so far the effect has not been captured directly in space and time. Here, we use contactless pump-probe microscopy to visualize the spatiotemporal evolution of photoexcited carriers in single-crystal, mono-domain $BiFeO_{3}$, a prototypical ferroelectric material. We observe asymmetric carrier transport along the polar axis, which confirms the intrinsic bulk- and symmetry-driven nature of the BPVE. Remarkably, this asymmetric transport persists for several nanoseconds after photoexcitation, which cannot be explained by conventional short-lived shift or phonon ballistic current BPVE mechanisms. Our Monte Carlo simulations show that asymmetric momentum scattering by defects, such as oxygen vacancies, leads to long-lived asymmetric carrier transport, as observed experimentally. Beyond fundamental insights, this paves the way towards controlling symmetry- and defect-driven photoresponses.