Direct spatiotemporal imaging of a long-lived bulk photovoltaic effect in $BiFeO_{3}$

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 novel optoelectronic devices. Despite its bulk nature, the BPVE is typically measured with interfaces and metal contacts, raising concerns as to whether the observed signals are genuinely of bulk origin. Here, we use a contactless pump-probe microscopy method to observe the space- and time-resolved dynamics of photoexcited carriers in single-crystal, monodomain $BiFeO_{3}$. We observe asymmetric transport of carriers along the polar axis, confirming the intrinsic bulk and symmetry-driven nature of BPVE. This asymmetric transport persists for several nanoseconds after photoexcitation, which cannot be explained by the shift or phonon ballistic current BPVE mechanisms. Monte Carlo simulations show that asymmetric momentum scattering by defects under non-equilibrium conditions explains the long-lived carrier drift, while first principles calculations confirm that oxygen vacancies have an asymmetric electronic state that can cause such asymmetric scattering. Our findings highlight the critical role of defects in long-lived photoresponses.