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The bulk photovoltaic effect exhibited by the non-centrosymmetric systemgains research interest due to the observed large open-circuit voltage. Theferroelectric systems exhibiting anomalous photovoltaic effect are mostlycrystallized with multiphase coexistence. Hence, the computational difficultyin building a multi-phase system restricts the detailed photovoltaic studiesthrough phenomenological and shift current theory. In this work, ferroelectricBa$_{1- x}$(Bi$_{0.5}$K$_{0.5}$)$_x$TiO$_3$ (BBKT) oxide is designed tocrystallize in single-phase tetragonal symmetry with improved polarizationcharacteristics, and it is found to exhibits large PV response. Bothexperimental and theoretical studies on BBKT samples reveal ~18% reduction inbandgap compared to the parent BaTiO$_3$. Short-circuit current measured as afunction of light intensity and light polarization angle reveal linear andsinusoidal response, respectively. The observed features are in accordance withphenomenological theory. Remarkably, x = 0.125 sample displays ~8 times higheropen-circuit voltage (7.39 V) than the parent compound. The enhanced PV effectis attributed to the large shift current along z-direction as evidenced fromthe additional charge-center shift of valence band occupied by O-2p orbital andconduction band occupied by Bi-6p orbital. Notably, the degenerate Bi-p$_z$state at conduction band minimum in BBKT favours the large shift currentresponse in the z-direction.

Bulk photovoltaic effect in BaTiO$_3$-based ferroelectric oxides: An experimental and theoretical study