Giant chiral amplification of chiral 2D perovskites via dynamic crystal reconstruction.

Chiral hybrid perovskites show promise for advanced spin-resolved optoelectronics due to their excellent polarization-sensitive properties. However, chiral perovskites developed to date rely solely on the interaction between chiral organic ligand cations exhibiting point chirality and an inorganic framework, leading to a poorly ordered short-range chiral system. Here, we report a powerful method to overcome this limitation using dynamic long-range organization of chiral perovskites guided by the incorporation of chiral dopants, which induces strong interactions between chiral dopants and chiral cations. The additional interplay of chiral cations with chiral dopants reorganizes the morphological and crystallographic properties of chiral perovskites, notably enhancing the asymmetric behavior of chiral 2D perovskites by more than 10-fold, along with the highest dissymmetry factor of photocurrent () of ~1.16 reported to date. Our findings present a pioneering approach to efficiently amplify the chiroptical response in chiral perovskites, opening avenues for exploring their potential in cutting-edge optoelectronic applications.