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Sökning: WFRF:(Sølling Theis I.)

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1.
  • Lissau, Jonas Sandby, et al. (författare)
  • Conformational Impact on Energy Storage Efficiency of Subphthalocyanine-Fullerene Hybrids
  • 2018
  • Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 122:33, s. 6683-6692
  • Tidskriftsartikel (refereegranskat)abstract
    • Hybrid molecules involving subphthalocyanine and Buckminsterfullerene derivatives are interesting candidates as heavy metal free triplet sensitizers. Subphthalocyanine efficiently absorbs visible photons and transfer the singlet excited state energy to the Buckminsterfullerene where intersystem crossing produces triplet states in high yield. Thus, far the efficiency of the triplet-generating photophysics in these systems has been hampered by back energy transfer to the subphthalocyanine triplet state resulting in loss of excitation energy. Herein an efficient strategy is realized to avoid loss of triplet energy by back energy transfer. A hybrid molecule based on subphthalocyanine and Buckminsterfullerene is presented in which dispersion-induced π-π interactions result in a molecular geometry where highly efficient through-space singlet excited state energy transfer takes place in one direction, whereas energy flow in the opposite direction via the triplet manifold is blocked by lack of orbital overlap. The approach opens for a new class of heavy-metal-free triplet sensitizers of particular relevance to the fields of photodynamic therapy and noncoherent photon upconversion.
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2.
  • Skov, Anders B., et al. (författare)
  • Excited‐State Topology Modifications of the Dihydroazulene Photoswitch Through Aromaticity
  • 2019
  • Ingår i: ChemPhotoChem. - : Wiley. - 2367-0932. ; 3:8, s. 619-629
  • Tidskriftsartikel (refereegranskat)abstract
    • The gain and loss of aromaticity plays a key role in organic chemistry and in the prediction of rate‐determining steps. Herein, we explore the concept of aromaticity in photoisomerization reactions. Benzannulated derivatives of the dihydroazulene‐vinylheptafulvene (DHA‐VHF) photoswitch were investigated using transient absorption spectroscopy and time‐dependent density functional theory to elucidate the effect of built‐in aromaticity on the switching properties. We found that benzannulation hampered the switching ability by enhancing an already existing barrier on the excited state surface. This enhancement was found to arise from a significant loss of aromaticity in the DHA‐to‐VHF transition state on the excited state potential energy surface. The VHF was found to be highly aromatic on the excited state surface, showing a reversal of aromaticity compared to the ground state. The barrier was found to be dependent on the position of benzannulation, since one derivative was found to switch as fast as the non‐benzannulated molecule although with lower efficiency, whereas another derivative completely lost the ability to undergo reversible photoswitching. The findings herein provide novel principles for the design of molecular photoswitches, shedding new light on excited state aromaticity, as previous discussions have mainly considered excited state aromaticity to be beneficial to switching. Our findings show that this view must be reconsidered.
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