Quantifying the interplay between chirality and spin splitting in hybrid organic-inorganic Perovskites

Chirality in hybrid organic–inorganic perovskites (HOIPs), inherited from chiral organic ligands through chirality transfer, profoundly influences their structural and electronic properties [1]. Yet, a quantitative understanding of how the degree of chirality of the organic cations governs its transfer to the inorganic framework - and how this, in turn, affects spin-related phenomena, particularly the spin splitting of electronic bands - remains elusive.  Here we employ the electronic chirality measure (ECM) [2], a relativistic, wavefunction-based descriptor, to quantify molecular chirality and explore its correlation with  spin splitting in a family of chiral HOIPs. We show that the ECM, together with the electric dipole moment of the organic ligands, serves as an effective predictor of the Rashba effect’s magnitude. Systematic chemical modification of the ligands reveals how these descriptors capture the interplay between chirality and spin–orbit splitting effects, providing a framework to design chiral HOIPs with tailored spin functionalities for spin-optoelectronic applications.