Thermally Activated Circularly Polarized Photoluminescence in a 2D Hybrid Perovskite with Giant Spin Splitting

Abstract Circularly polarized light generation and detection are critical for future spin‐based technologies that inter‐convert circularly polarized photons and electron spins. However, detailed mechanisms in such spin‐photon interfaces are often either poorly understood or operate at cryogenic temperatures since typically small energies separating spin‐split electronic bands facilitate thermally driven spin depolarization. Recently, several 2D hybrid perovskites with polar achiral cations were theoretically demonstrated to exhibit conduction and valence band spin‐splitting energies greatly exceeding room‐temperature thermal energy, suggesting their utility as spin‐photon interfaces with practical operating temperatures. Here, a strong “spin memory” effect is reported in such a polar achiral layered perovskite that enables large room‐temperature circularly polarized emission anisotropy following excitation with circularly polarized light. The polarization anisotropy depends strongly on temperature (thermally activated), excitation energy, and crystal orientation with respect to the excitation source. Temperature‐dependent photoconductance measurements reveal similar thermally activated carrier generation. These observations suggest a mechanism whereby giant in‐plane splitting of single‐particle levels protects spin‐polarization of photogenerated electrons and holes before recombination. Although polarized light emission is explored in greater detail in chiral perovskites, these results reveal that even without chirality, large spin memory in polar achiral perovskites can enable spin‐photon interfaces that operate at elevated temperatures.