The bulk photovoltaic effect is a long-known but poorly understood phenomenon. Recently, however, the multiferroic bismuth ferrite has been observed to produce strong photovoltaic response to visible light, suggesting that the effect has been underexploited as well. Here we present three polar oxides in the LiNbO3 structure that we predict to have band gaps in the 1-2 eV range and very high bulk photovoltaic response: PbNiO3, Mg 1/2 Zn 1/2 PbO3, and LiBiO3. All three have band gaps determined by cations with d 10 s 0 electronic configurations, leading to conduction bands composed of cation s-orbitals and O p-orbitals. This both dramatically lowers the band gap and increases the bulk photovoltaic response by as much as an order of magnitude over previous materials, demonstrating the potential for high-performing bulk photovoltaics.Photovoltaic effects have long been observed in bulk polar materials, especially ferroelectrics [1][2][3][4]. Known as the bulk photovoltaic effect (BPVE), it appeared to derive from inversion symmetry breaking. Despite intense initial interest, early explorations revealed low energy conversion efficiency, in part due to the high band gaps of most known ferroelectrics. Additionally, despite several proposed mechanisms, the physical origin of the BPVE was unclear [2,[5][6][7][8].However, recent emphasis on alternative energy technologies and the observation of the effect in novel semiconducting ferroelectrics (with band-gaps in the visible range) has renewed interest [9][10][11][12][13][14]. Several studies have attempted to elucidate the various contributions to the photovoltaic response -bulk or otherwise -in ferroelectrics [15][16][17][18][19][20][21][22][23]. In particular, bismuth ferrite (BFO) has been found to generate significant bulk photocurrents; combined with its unusually low band gap of 2.7 eV, it has attracted a great deal of attention for its potential in photovoltaic applications [21,[23][24][25][26][27][28][29][30][31]. The understanding of the fundamental physics behind the effect has advanced as well; recently we demonstrated that the BPVE can be attributed to "shift currents", and that the bulk photocurrents may be calculated from first-principles. The ab initio calculation of the shift current and subsequent analysis yielded several chemical and structural criteria for optimizing the response. These criteria have been used previously to modify or identify existing materials with enhanced response [14,[32][33][34]. In this work, we use these insights to propose several candidate bulk photovoltaics with calculated response as much as an order of magnitude higher than well-known ferroelectrics, while having band gaps in or slightly below the visible spectrum. Our results demonstrate that bulk photovoltaic response can be much stronger than previously observed, supporting the possibility of materials suitable for application.There are two figures of merit for evaluating the BPVE in a material: the current density response to a spatially uniform electric field, and the G...