Relation of Continuous Chirality Measure to Spin and Orbital Polarization, and Chiroptical Properties in Solids (2504.11596v1)

Abstract: Chirality introduces intriguing topological, electronic, and optical properties to molecules and solids. In this work, we investigate the influence of structural chirality on spin and orbital polarization as well as optical activity through first-principles calculations and continuous chirality measure (CCM). By using chiral selenium (Se) and 2D hybrid perovskites as examples, we demonstrate that chirality continuously modifies spin-orbit splitting and orbital angular momentum (OAM) polarization. We establish a direct relation between chirality transfer across organic-inorganic interfaces and inversion symmetry breaking, which induces Rashba-Dresselhaus spin splitting in hybrid perovskites. Additionally, we examine the effects of chirality on circular dichroism (CD) and the circular photogalvanic effect (CPGE), demonstrating how the continuous tuning of chirality dictates their magnitude and anisotropy. Our findings highlight that applying hydrostatic pressure can effectively tune the CCM, thereby enhancing the chirality-induced effects such as spin selectivity. By integrating CCM with electronic structure calculations, we present a predictive strategy for designing chiral materials with tailored optical and spintronic functionalities.