Understanding the nonlinear response of light and materials is crucial for fundamental physics and next-generation electronic devices. In this work, we have investigated the second-order nonlinear bulk photovoltaic (BPV) and bulk spin photovoltaic (BSPV) effects in the piezoelectric binary materials T-IV-VI and T-V-V (IV = Ge, Sn; VI = S, Se; and V = P, As, Sb, Bi). The independent nonzero conductivity tensors of charge current are derived for these binaries through the symmetry analysis, along with the mechanism for generating pure spin current. These binaries, with their unique folded structure, exhibit significant charge and spin currents under illumination. Furthermore, we find that strain engineering can effectively modulate charge/spin currents by influencing charge density distribution and built-in electric field due to the piezoelectric effect. Our research suggests that the piezoelectric binary materials possess enormous and tunable charge/spin currents, underscoring their potential for applications in nonlinear flexible optoelectronics and spintronics.
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