Spin-Chirality-Driven Bulk Photovoltaic Effect in van der Waals Magnet CrSBr

Abstract The bulk photovoltaic effect (BPVE) manifests with remarkable diversity in magnetic materials. Here, we establish vector spin chirality as a tunable knob for generating an unconventional time-reversal-even magnetic BPVE, comprising the chiral shift current (CSC) and chiral injection current (CIC). Using bilayer antiferromagnetic (AFM) CrSBr as a prototype, we theoretically demonstrate the emergence of CSC and CIC. Compared with conventional photovoltaic currents arising from noncentrosymmetric crystal structures or collinear magnetic orderings, CSC and CIC not only possess comparable magnitudes but also exhibit exceptional tunability. Specifically, they can be switched on and off by magnetic-field-induced spin canting, reversed in direction upon canting-direction reversal, and continuously modulated in intensity via canting-angle variation. Furthermore, we reveal an unusual optical transition channel governing both currents in CrSBr. Our work establishes an unconventional magnetic BPVE with remarkable controllability, offering opportunities for optoelectronic and magnetic-sensing applications in noncollinear magnets.