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- W2134266727 abstract "We investigate theoretically the control of the ultrafast excited state dynamics of adenine in water by laser pulse trains, with the aim to extend the excited state lifetime and to suppress nonradiative relaxation processes. For this purpose, we introduce the combination of our field-induced surface hopping method (FISH) with the quantum mechanical–molecular mechanical (QM/MM) technique for simulating the laser-driven dynamics in the condensed phase under explicit inclusion of the solvent environment. Moreover, we employ parametric pulse shaping in the frequency domain in order to design simplified laser pulse trains allowing to establish a direct link between the pulse parameters and the controlled dynamics. We construct pulse trains which achieve a high excitation efficiency and at the same time keep a high excited state population for a significantly extended time period compared to the uncontrolled dynamics. The control mechanism involves a sequential cycling of the population between the lowest and higher excited states, thereby utilizing the properties of the corresponding potential energy surfaces to avoid conical intersections and thus to suppress the nonradiative decay to the ground state. Our findings provide a means to increase the fluorescence yield of molecules with an intrinsically very short excited state lifetime, which can lead to novel applications of shaped laser fields in the context of biosensing." @default.
- W2134266727 created "2016-06-24" @default.
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- W2134266727 date "2012-01-01" @default.
- W2134266727 modified "2023-10-01" @default.
- W2134266727 title "Laser pulse trains for controlling excited state dynamics of adenine in water" @default.
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- W2134266727 doi "https://doi.org/10.1039/c2cp24002e" @default.
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