Enhancing Hot-Carrier Lifetime through Spin Splitting and Strain Interaction in Chiral Perovskite Materials.

The dynamical control over electronic properties represents a key area of research in condensed-matter physics. Here, we demonstrate all-optical control of carrier-strain-mediated giant enhancement of spin splitting (100 meV) in a chiral 2D perovskite. Ultrafast circular dichroism measurements and ab initio calculations reveal that anisotropic strain from confined photoexcited excitons enhances spin splitting, thereby creating a spin-dependent hot-carrier relaxation pathway and tripling hot-carrier lifetimes. Our findings establish a versatile optical strategy for coherent spin manipulation and open avenues for developing spin-based hot-carrier devices.