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The chiral organic-inorganic halide perovskites (OIHPs) are vital candidatesfor superior nonlinear optical (NLO) effects associated with circularlypolarized (CP) light. NLO in chiral materials often couples with magneticdipole (MD) transition, as well as the conventional electric dipole (ED)transition. However, the importance of MD in NLO process of chiral OIHPs hasnot yet been well recognized. Here, the analysis of second harmonic generationcircular dichroism (SHG-CD) provides the direct evidence that the MDcontribution leads to a large anisotropic response to CP lights in chiralOIHPs, (R-/S-MBACl)2PbI4. The thin films exhibit great sensitivity to CP lightsover a wide wavelength range, and the g-value reaches up to 1.57 at thewavelength where the contribution of MD is maximized. Furthermore, it is alsoeffective as CP light generator, outputting CP-SHG with maximum g-factor of1.76 upon the stimulation of linearly polarized light. This study deepens theunderstanding of the magneto-optical NLO processes in chiral systems.

Magneto-chiral nonlinear optical effect with large anisotropic response in two-dimensional halide perovskite