Abstract Chiral hybrid metal halides (HMHs) have attracted considerable attention due to their promising application in various optoelectronic devices. In this work, one kind of zero‐dimensional (0D) R/S‐methylbenzylammonium) 2 PdCl 4 (R/S‐MBA) 2 PdCl 4 single crystals have been synthesized, which possess an indirect bandgap and exhibit energy band splitting at the valence band maximum (VBM) due to the distortion in the PdCl 4 2− square‐planar structure. Notably, the chiral single crystals demonstrate a significant second‐order nonlinear optical (NLO) coefficient i.e., 15 times that of Y‐cut quartz and second‐harmonic generation‐circular dichroism (SHG‐CD) with an anisotropy factor (g SHG‐CD ) of 0.54. Interestingly, circularly polarized‐SHG (CP‐SHG) with an anisotropy factor ( g CP‐SHG ) up to 0.88 is observed in the lead‐free HMHs. These findings highlight the potential of chiral hybrid palladium (Pd) halides for applications in nonlinear optoelectronic devices.
Qiu et al. (Mon,) studied this question.
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