Elucidating Interfacial Carrier Transfer Dynamics for Circularly Polarized Emission in Self-Assembled Perovskite Heterostructures

By integrating carrier transfer with spin-selectivity in mixed-dimensional perovskites heterostructures (HSs), exceptional chiroptical behaviors can be activated, offering avenues for advanced applications in spintronics and quantum information technologies. However, the critical role of interface effects in this photophysical process remains insufficiently explored. We demonstrate the fabrication of self-assembled chiral 2D/achiral nanocrystal (NC) HSs with different morphologies and chiroptical activities. Using femtosecond transient reflection spectroscopy, the underlying interface-dependent carrier transfer was unraveled. Spin-polarized holes generated in the chiral 2D component can transfer within an ultrafast time scale of ∼362 fs across the coherent heterointerface, inducing circularly polarized luminescence (CPL) in the intrinsically achiral NCs with a high <i>P</i>_c of ∼10.3%. Furthermore, interfacial halide exchange can be utilized to extend the CPL wavelength from green to near-infrared. Our findings reveal the correlation between interfacial properties, charge transfer, and CPL activity, providing insights for the development of high-quality HSs with optimized optical properties.