Lawrence Berkeley National Laboratory

Solid systems with strong correlations and interactions under light illumination have the potential for exhibiting interesting bulk photovoltaic behavior in the nonperturbative regime, which has remained largely unexplored in past theoretical studies. We investigate the bulk photovoltaic response of a perovskite manganite with strongly coupled electron-spin-lattice dynamics using real-time simulations performed with a tight-binding model. The transient changes in the band structure and the photoinduced phase transitions, emerging from spin and phonon dynamics, result in a nonlinear current versus intensity behavior beyond the perturbative limit. The current rises sharply across a photoinduced magnetic phase transition, which later saturates at higher light intensities due to excited phonon and spin modes. The predicted peak photoresponsivity is an order of magnitude higher than another known transition metal ferroelectric oxide BiFeO3. We disentangle phonon-and spin-assisted components to the ballistic photocurrent, showing that they are comparable in magnitude. Our results illustrate a promising alternative way for controlling and optimizing the bulk photovoltaic response through the photoinduced phase transitions in strongly correlated systems.