Ye Chen, Mallick Suman, Hertzog Manuel, Kowalewski Markus, Börjesson Karl
Department of Chemistry and Molecular Biology, University of Gothenburg, Kemigården 4, 412 96 Gothenburg, Sweden.
Department of Physics, Stockholm University, Albanova University Centre, 106 91 Stockholm, Sweden.
J Am Chem Soc. 2021 May 19;143(19):7501-7508. doi: 10.1021/jacs.1c02306. Epub 2021 May 11.
Strong light-matter coupling generates hybrid states that inherit properties of both light and matter, effectively allowing the modification of the molecular potential energy landscape. This phenomenon opens up a plethora of options for manipulating the properties of molecules, with a broad range of applications in photochemistry and photophysics. In this article, we use strong light-matter coupling to transform an endothermic triplet-triplet annihilation process into an exothermic one. The resulting gradual on-off photon upconversion experiment demonstrates a direct conversion between molecular states and hybrid light-matter states. Our study provides a direct evidence that energy can relax from nonresonant low energy molecular states directly into hybrid light-matter states and lays the groundwork for tunable photon upconversion systems that modify molecular properties in situ by optical cavities rather than with chemical modifications.
强光与物质的强耦合产生了兼具光和物质特性的混合态，从而有效地实现了分子势能面的改变。这一现象为操控分子性质提供了大量选择，在光化学和光物理领域有着广泛应用。在本文中，我们利用强光与物质的强耦合将一个吸热的三重态-三重态湮灭过程转变为放热过程。由此产生的逐渐开启-关闭的光子上转换实验展示了分子态与混合光-物质态之间的直接转换。我们的研究提供了直接证据，证明能量可以从非共振的低能分子态直接弛豫到混合光-物质态，为通过光学腔而非化学修饰原位改变分子性质的可调谐光子上转换系统奠定了基础。
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