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Search: WFRF:(Bachmann Julien)

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1.
  • Borne, Kurtis D., et al. (author)
  • Ultrafast electronic relaxation pathways of the molecular photoswitch quadricyclane
  • 2024
  • In: NATURE CHEMISTRY. - 1755-4330 .- 1755-4349. ; 16, s. 499-505
  • Journal article (peer-reviewed)abstract
    • The light-induced ultrafast switching between molecular isomers norbornadiene and quadricyclane can reversibly store and release a substantial amount of chemical energy. Prior work observed signatures of ultrafast molecular dynamics in both isomers upon ultraviolet excitation but could not follow the electronic relaxation all the way back to the ground state experimentally. Here we study the electronic relaxation of quadricyclane after exciting in the ultraviolet (201 nanometres) using time-resolved gas-phase extreme ultraviolet photoelectron spectroscopy combined with non-adiabatic molecular dynamics simulations. We identify two competing pathways by which electronically excited quadricyclane molecules relax to the electronic ground state. The fast pathway (<100 femtoseconds) is distinguished by effective coupling to valence electronic states, while the slow pathway involves initial motions across Rydberg states and takes several hundred femtoseconds. Both pathways facilitate interconversion between the two isomers, albeit on different timescales, and we predict that the branching ratio of norbornadiene/quadricyclane products immediately after returning to the electronic ground state is approximately 3:2.
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2.
  • Waidhas, Fabian, et al. (author)
  • Electrochemically controlled energy release from a norbornadiene-based solar thermal fuel: increasing the reversibility to 99.8% using HOPG as the electrode material
  • 2020
  • In: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7496 .- 2050-7488. ; 8:31, s. 15658-15664
  • Journal article (peer-reviewed)abstract
    • Solar energy conversion using molecular photoswitches holds great potential to store energy from sunlight in the form of chemical energy in a process that can be easily implemented in a direct solar energy storage device. In this context, we investigated the electrochemically triggered energy release of a solar thermal fuel based on the norbornadiene (NBD)/quadricyclane (QC) couple by photoelectrochemical IR reflection absorption spectroscopy (PEC-IRRAS). We studied the photo-induced conversion of the energy-lean 2-cyano-3-(3,4-dimethoxyphenyl)-norbornadiene (NBD ') to the energy-rich 2-cyano-3-(3,4-dimethoxyphenyl)-quadricyclane (QC ') and the electrochemically triggered reconversion using highly oriented pyrolytic graphite (HOPG) as an electrode material. We compared our results with the results obtained previously using Pt(111) electrodes and we characterized the photochemical and electrochemical properties of the storage system. NBD ' can be photochemically converted and electrochemically reconverted with very high selectivity. HOPG largely suppresses the unwanted catalytic reconversion which was observed on Pt(111). We performed repetitive cycling experiments for 1000 cycles to determine the reversibility of the system. Our results show that it is possible to reach reversibility above 99.8% using HOPG as an electrode material.
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