Leveraging Coupling in Chiral Low-Dimensional/3-Dimensional Perovskite Heterostructure for Spin-Optoelectronics

Spin-optoelectronics, which exploit the spin degree of freedom in addition to charge,offer transformative advantages including ultrafast response, nonvolatile memory retention, and reduced power consumption. Chiral metal halide perovskites have recently emerged as promising candidates for spin-optoelectronic devices, where spin transport is facilitated by the combined effects of molecular chirality and strong spin-orbit coupling (SOC), primarily driven by the distortion of inorganic lattices. However, purely chiral low-dimensional (low-D) perovskites exhibit low conductivity and short spin coherence,while 3D perovskites, though highly conductive, lack inversion asymmetry for efficient spin polarization. To overcome these trade-offs, this project proposes coherent chiral low-D/3D perovskite heterostructures that integrate the spin-filtering ability of chiral perovskites with the transport efficiency of 3D lattices. Such coherent coupling is promising for surpassing the limitations of isolated chiral low-D or 3D systems by achieving long spin transport lifetimes and large spin polarization at ambient conditions.⁠⁠⁠⁠⁠⁠⁠We will first design and synthesize coherent chiral low-D/3D perovskite heterostructures through a ligand diffusion-driven growth strategy, considering lattice matching, 3D component ligand diffusion, as well as nucleation control. The heterostructure will be characterized by X-ray diffraction (XRD), Grazing-Incident Wide-Angle X-Ray Scattering (GIWAXS), and Transmission Electron Microscopy (TEM)to confirm lattice coherence and extract structural chiral metrics. Then, we will characterize the chirality penetration depth from chiral low-D to 3D perovskite using circular dichroism (CD) and circularly polarized luminescence (CPL) spectroscopy. Spin-dependent transport will also be quantitatively analyzed using magnetic conductive (mc)-AFM, and helicity-resolved photocurrent, while ultrafast circularly polarized light pump–probe experiments will probe transient spin dynamics. First-principles calculations will link structural chirality metrics with experimental spin polarization and lifetime, providing a predictive framework for optimizing SOC. Ultimately, this study will enable the rational design of next-generation spin-optoelectronic devices, such as circular photogalvanic effect (CPGE)-based photodetectors and circularly polarized (CP)-LEDs, advancing perovskite-based spintronics toward room-temperature energy-efficient devices.The proposed work will establish a new paradigm in coherently coupled chiral heterostructures, providing both a synthesis strategy and a mechanistic model linking structural chirality, SOC, and spin dynamics. Beyond advancing fundamental understanding, this project is expected to unlock applications in future spin-optoelectronic development.