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    A general approach for all-visible-light switching of diarylethenes through triplet sensitization using semiconducting nanocrystals
    (London [u.a.] : RSC, 2022) Hou, Lili; Larsson, Wera; Hecht, Stefan; Andréasson, Joakim; Albinsson, Bo
    Coupling semiconducting nanocrystals (NCs) with organic molecules provides an efficient route to generate and transfer triplet excitons. These excitons can be used to power photochemical transformations such as photoisomerization reactions using low energy radiation. Thus, it is desirable to develop a general approach that can efficiently be used to control photoswitches using all-visible-light aiming at future applications in life- and materials sciences. Here, we demonstrate a simple ‘cocktail’ strategy that can achieve all-visible-light switchable diarylethenes (DAEs) through triplet energy transfer from the hybrid of CdS NCs and phenanthrene-3-carboxylic acid, with high photoisomerization efficiency and improved fatigue resistance. The size-tunable excitation energies of CdS NCs make it possible to precisely match the clear spectral window of the relevant DAE photoswitch. We demonstrate reversible all-visible-light photoisomerization of a series of DAE derivatives both in the liquid and solid state, even in the presence of oxygen. Our general strategy is promising for fabrication of all-visible-light activated optoelectronic devices as well as memories, and should in principle be adaptable to photopharmacology.
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    Few-cycle 65-µJ pulses at 11.4 µm for ultrafast nonlinear longwave-infrared spectroscopy
    (Washington, DC : Optical Society of America, OSA, 2022) Fuertjes, Pia; Bock, Martin; Grafenstein, Lorenz von; Ueberschaer, Dennis; Griebner, Uwe; Elsaesser, Thomas
    Low-energy excitations can provide insight into the basic ultrafast nonequilibrium dynamics of condensed matter. High-energy femtosecond pulses in the long-wavelength infrared are required to induce such processes, and can be generated in an optical parametric chirped pulse amplification (OPCPA) system comprising three GaSe stages. A femtosecond Cr:ZnS laser serves as the front-end, providing the seed for the 2.0-µm pump and the 2.4-µm signal pulses without nonlinear conversion processes. The OPCPA system is pumped at 2.05 µm by a picosecond Ho:YLF regenerative amplifier at a 1-kHz repetition rate. The recompressed idler pulses at 11.4 µm have a duration of 185 fs and an unprecedented energy of 65 µJ, corresponding to a pump-to-idler conversion efficiency of 1.2%. Nonlinear transmission experiments in the range of the L2 infrared band of liquid water demonstrate the potential of the pulses for nonlinear vibrational spectroscopy of liquids and solids.