With the booming development of two-dimensional (2D) flexible devices, flexure has attracted much attention as an emerging means to modulate device performances. Here, the magnetic-optical-electrical multifield coupling mechanism of spin photocurrent in bent CrSBr monolayer is investigated through first-principles calculations. The studies show that simple mechanical bending of monolayer CrSBr can successfully achieve the spatial separation of electrons and holes. The nonequilibrium process of photogenerated carriers in bent CrSBr modulates both the shift current density and the ballistic current density, thereby enabling the photovoltaic effect. Meanwhile, the built-in electric field generated by flexure drives the device toward more efficient self-powered behavior. Moreover, this self-powered polarization devices have excellent spin photovoltaic properties and high polarization sensitivity. The present Letter creates novel opportunities for 2D spintronics and opens new avenues for realizing self-powered polarization devices.

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• Photocurrent
• Photovoltaic effect
• Spin optoelectronics
• 2-dimensional systems
• First-principles calculations