Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.008
Publication date: 16th December 2024
Coherent manipulation of solid-state spins is important for quantum information processing. Current solid-state spin systems either operate at very low temperatures or are difficult to scale-up. Colloidal quantum dots (QDs), by contrast, can be synthesized in large quantity in solution at low cost, yet with high finesse in size and shape control. Further, they are usually strongly quantum-confined, thus their carriers well isolated from the phonon bath, which could enable long-lived spin coherence at room temperature. We studied coherent spin dynamics in solution-grown lead halide perovskite QDs using transient magneto-optical spectroscopy. We observed ensemble-level quantum beats resulting from an exciton fine-structure gap and quantitatively controlled the gap energy using temperature-programmable lattice distortion. This unique mechanism has important implications for the application of perovskite QDs in quantum light-sources and coherent exciton control. Further, by dissociating excitons using ultrafast interfacial electron transfer, we achieved room-temperature all-optical initialization, manipulation and readout of hole spins in CsPbBr3 QDs. This represents a milestone towards a scalable and sustainable future of spin-based quantum information processing.
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