Coherent manipulation of photochemical spin-triplet formation in quantum dot–molecule hybrids

Abstract

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 and organic molecules. The large g-factor difference enables 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 radical pairs enabled by the quantum confinement of quantum dots. The rapid quantum beats enable the efficient and coherent control of charge recombination dynamics at room temperature, with the modulation level of the yield of spin-triplet products reaching 400%. Photochemical quantum process in quantum dot–molecule hybrids is normally weak and difficult to be coherently controlled. Radical-pair spin quantum beats can enable the efficient and coherent control of charge recombination at room temperature.