Mind the gap: From resolving theoretical foundations of chiral(ity)-induced spin selectivity to pioneering implementations in quantum sensing

The chiral(ity)-induced spin selectivity (CISS) effect, where electrons passing through a chiral medium acquire significant spin polarization at ambient temperatures, has been widely observed experimentally, yet its theoretical foundations remain actively debated. Open questions persist regarding whether CISS originates from helical geometry or more general chirality and whether a unified mechanism can account for phenomena across solid-state and soft-matter systems, mesoscopic films, and single molecules. Clarifying the interrelations between existing models is essential to determine if a universal picture of CISS can be found or whether system-specific models are required, and if so, where their common starting point should lie for a workable classification of CISS manifestations. Despite this theoretical fragmentation, recent studies of CISS effects in electron-transfer systems, magnetic field sensitivity and coherence of radical pair reactions, polarized electroluminescence in chiral hybrid perovskites, DNA-based biosensors, and enantioselective detection highlight its broad conceptual relevance and potential applications in spintronics, molecular sensors, and quantum information processing. In this review, we help bridge the gap between theory, experiment, and implementation, with a particular focus on prospects for quantum sensing and metrology. We outline fundamental frameworks of CISS, clarifying what constitutes the “chiral,” the “induced,” and the “spin selectivity” that make up CISS, before going on to survey key model realizations and their assumptions. We examine some of the emerging quantum sensing applications and assess the model-specific implications, in particular exemplifying these in the context of spin-correlated radical pairs, which offer a promising, tunable, and biomimetic platform for emerging molecular quantum technologies.