Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.007
Publication date: 16th December 2024
The interconversion between singlet and triplet spin states of photogenerated radical pairs is a genuine quantum process, which can be harnessed to coherently manipulate the recombination products through a magnetic field. This control is central to such diverse fields as molecular optoelectronics, quantum sensing, quantum biology and spin chemistry, but its effect is typically fairly weak in pure molecular systems. Here we introduce hybrid radical pairs constructed from semiconductor quantum dots (QDs) and organic molecules. The large g-factor difference allows us to directly observe the radical-pair spin quantum beats usually hidden in previous studies, which are further accelerated by the strong exchange coupling of the radical pairs enabled by quantum confinement of QDs. The rapid quantum beats enable efficient and coherent control of charge recombination dynamics at room temperature, with the modulation level of the yield of spin-triplet products reaching 400%. As spin-triplets are ubiquitously involved in molecular and hybrid inorganic/organic photocatalytic and photonic devices, an efficient, quantum-coherent control over the triplet recombination yields of radical pairs could offer disruptive solutions to engineering the performance of such devices. Additionally, hybrid radical pairs constitute a unique material platform to merge the field of emerging molecular quantum sciences with solid-state quantum platforms to enable novel physical phenomena and quantum technologies.
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