Chirality‐Dependent Anisotropic Nonlinear Optical Effect in Low‐Dimensional Hybrid Metal Halides

Low‐dimensional hybrid metal halides (LDHMHs) have emerged as a highly promising class of functional materials for a wide range of optoelectronic applications. Their exceptional structural tunability, facilitated by the hybridization of metal halides with organic compounds, enables the formation of three‐, two‐, one‐, or zero‐dimensional structures. This flexibility in structural design also allows the incorporation of chirality into the crystalline lattice, giving rise to novel LDHMH materials that are capable of selectively interacting with the spin angular momentum of electrons and photons. Among the unique optoelectronic properties of LDHMHs, the focus of this concept article is their chiroptical nonlinear optical (NLO) effect. LDHMHs demonstrate a highly effective discrimination and generation of circularly polarized (CP) light in the NLO regime, particularly in the second harmonic generation (SHG) process, referred to as SHG‐circular dichroism (SHG‐CD) and CP‐SHG. These anisotropic responses are several orders of magnitude larger than linear chiroptical responses, such as CD and CP luminescence; consequently, LDHMHs are expected to be promising candidates for future optical‐information devices and encryption systems. This article introduces recently reported chiral LDHMH materials that exhibit excellent CP‐dependent anisotropic SHG responses.