Femtosecond Optical Logic Gates Based on Tailored Spin‐Selective Optical Stark Effect in Perovskite Chiral Metasurface

Abstract The optical logic gates are the building blocks for all‐optical computing and optical interconnect. Spin‐based optical logic gates have the potential to enhance information capacity and processing speed, addressing the demand for handling the ever‐growing amounts of information in next‐generation optical networks. Rashba‐Dresselhaus perovskites exhibit strong spin‐orbit coupling and high exciton binding energy, making them promising candidates for realizing spin‐based logic at room temperature. However, neither perovskite thin films nor single crystals are capable of delivering the high transient circular dichroism response necessary for developing ultrafast spin logic devices. Here, chiral metasurfaces are employed to tailor the spin‐selective optical Stark effect in 2D perovskites by harnessing the unique chiral electric field distributions. All‐optical spin‐based AND, NOR, is demonstrated and NOT gates in the perovskite chiral metasurfaces with an ultrafast response time of 120 fs. This study offers a novel strategy for manipulating spin‐dependent ultrafast electronic dynamics and highlights the potential applications of 2D perovskites in ultrafast optical spin‐based devices.