Orientation-Driven Chirality Funnels in Chiral Low-Dimensional Lead-Halide Perovskite Heterostructures

Chiral hybrid metal-halide perovskites show low-symmetry crystal structures, large Rashba splitting, spin-filtering, and strong chiroptical activity. Circular dichroism and circularly polarized photoluminescence have been investigated in chiral perovskites with increasingly distorted chiral structures. Here, we report the fabrication of chiral (<i>R</i>/<i>S</i>)-EBAPbI₃ (EBA = α-ethylbenzylamine) single crystals, which possess highly distorted octahedral structures with a high angle variance value of ∼68 degree². Using control in the fabrication conditions, we transfer chiral single crystals to thin films and achieve different crystal orientation preferences that induce tunable chiroptical properties to their heterostructures with PbI₂ nanodomains, which we characterize with in situ X-ray diffraction and grazing-incidence wide-angle X-ray scattering measurements. Using transient chiroptical spectroscopies, we resolve photoexcited charge carrier dynamics and chirality transfer processes in such heterostructures down to cryogenic temperatures. We observe rapid carrier transfer along the in-plane (002) facets in chiral perovskite phases to PbI₂ nanostructures within the initial few picoseconds, while carrier transfer along the out-of-plane (002) facets occurs at a slower rate. This fast transfer process leads to high photoluminescence intensities and large degrees of circular polarization in the emission from PbI₂ nanodomains at cryogenic temperatures. Our findings report a multidimensional chiral-achiral heterostructure which takes advantage of controllable chirality transfer and offers new routes for future spintronic and chiroptical applications.