Decoding Chirality Transfer Strengths and Structure–Property Relationships in Bismuth-Containing Chiral Hybrid Organic–Inorganic Semiconductors

Chiral hybrid organic-inorganic semiconductors (CHOIS), which integrate chiral organic cations by hydrogen-bonding interactions with anionic metal halide subunits, have recently emerged as cutting-edge materials with the potential to revolutionize energy-efficient information processing, particularly in the realms of spintronics. By harnessing the inherent chirality of organic cations, CHOIS can effectively manipulate spin dynamics, a crucial factor for enhancing the device performance in next-generation electronics. However, the challenge lies in the limited understanding of structure-property relationships, which hinders the ability to control and fine-tune the chirality within these materials. To address this gap, we developed a systematic approach that provides rational chemical control over the structural characteristics of bismuth (Bi)-containing CHOIS by incorporating chiral organic cations with adjustable hydrogen-bonding interactions. Our work, which combines in-depth crystallographic analysis with advanced spectroscopic techniques, uncovers a clear correlation between specific local structural features and enhanced chiroptical responses, as well as spin-related phenomena, such as the Rashba-Dresselhaus effects. Our findings not only pave the way for the design of advanced chiral materials with precisely tailored chiroptical and spin-related properties, but also open new frontiers for their application in optoelectronic and spintronic devices, offering unprecedented potential for future technologies.