Halogen-Dependent Circular Dichroism and Magneto-Photoluminescence Effects in Chiral 2D Lead Halide Perovskites

Chiral lead halide perovskites (chiral LHPs) have emerged as one of the best candidates for opto-spintronics due to their large spin-orbit coupling (SOC) and unique chirality-induced spin selectivity (CISS) even in the absence of a magnetic field. Here, we report the impact of halide composition on circular dichroism (CD) and magneto-photoluminescence (PL) effects of chiral 2D LHPs (<i>R</i>/<i>S</i>-MBA)₂PbBr_<i>x</i>I_4-<i>x</i> (MBA = C₆H₅CH₂(CH₃)NH₃). By tuning the mixing ratio of Br/I halide anions, we find that (<i>R</i>/<i>S</i>-MBA)₂PbBr_<i>x</i>I_4-<i>x</i> thin films exhibit tunable and wide wavelength range CD signals. Simultaneously, the main CD signals near the exciton absorption band gradually blue shift until they disappear. Moreover, the halogen-dependent negative magneto-PL effects of (<i>R</i>/<i>S</i>-MBA)₂PbBr_<i>x</i>I_4-<i>x</i> thin films excited by left/right circularly polarized light can be detected at room temperature. We demonstrated that the halide composition can effectively modulate exciton splitting and chirality transfer in (<i>R</i>/<i>S</i>-MBA)₂PbBr_<i>x</i>I_4-<i>x</i> owing to the chirality-induced SOC and crystalline structure transition, which lead to the adjustable CD signals. The interplay of Rashba-type band spin splitting and spin mixing among bright triplet exciton states is responsible for the halogen-dependent magneto-PL effect of chiral 2D LHPs. This study enables chiral 2D LHPs with CISS to be a new class of promising opto-spintronics materials for exploring high-performance spin-light-emitting diodes by halide engineering.