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Ultrafast electroni...
Ultrafast electronic relaxation pathways of the molecular photoswitch quadricyclane
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- Borne, Kurtis D. (author)
- Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA.
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- Cooper, Joseph C. (author)
- Univ Oxford, Dept Chem, Phys & Theoret Chem Lab, Oxford, England.,Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Ashfold, Michael N. R. (author)
- Univ Bristol, Sch Chem, Bristol, England.
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- Bachmann, Julien (author)
- Friedrich Alexander Univ Erlangen Nurnberg, Chem Thin Film Mat, Erlangen, Germany.
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- Bhattacharyya, Surjendu (author)
- Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA.
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- Boll, Rebecca (author)
- European XFEL, Schenefeld, Germany.
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- Bonanomi, Matteo (author)
- CNR, Ist Foton & Nanotecnol, IFN, Milan, Italy.;Politecn Milan, Dipartimento Fis, Milan, Italy.
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- Bosch, Michael (author)
- Friedrich Alexander Univ Erlangen Nurnberg, Chem Thin Film Mat, Erlangen, Germany.
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- Callegari, Carlo (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Centurion, Martin (author)
- Univ Nebraska Lincoln, Dept Phys & Astron, Lincoln, NE USA.
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- Coreno, Marcello (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.;CNR, Ist Struttura Mat ISM, Trieste, Italy.
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- Curchod, Basile F. E. (author)
- Univ Bristol, Sch Chem, Bristol, England.
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- Danailov, Miltcho B. (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Demidovich, Alexander (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Di Fraia, Michele (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Erk, Benjamin (author)
- Deutsch Elektronen Synchrotron DESY, Hamburg, Germany.
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- Facciala, Davide (author)
- CNR, Ist Foton & Nanotecnol, IFN, Milan, Italy.
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- Feifel, Raimund (author)
- Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU),Univ Gothenburg, Dept Phys, Gothenburg, Sweden.
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- Forbes, Ruaridh J. G. (author)
- SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA USA.
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- Hansen, Christopher S. (author)
- Univ New South Wales, Sch Chem, Sydney, NSW, Australia.
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- Holland, David M. P. (author)
- Daresbury Lab, Warrington, England.
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- Ingle, Rebecca A. (author)
- UCL, Dept Chem, London, England.
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- Lindh, Roland, Professor, 1958- (author)
- Uppsala universitet,Organisk kemi
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- Ma, Lingyu (author)
- Brown Univ, Dept Chem, Providence, RI USA.
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- Mcghee, Henry G. (author)
- UCL, Dept Chem, London, England.
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- Muvva, Sri Bhavya (author)
- Univ Nebraska Lincoln, Dept Phys & Astron, Lincoln, NE USA.
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- Nunes, Joao Pedro Figueira (author)
- Univ Nebraska Lincoln, Dept Phys & Astron, Lincoln, NE USA.
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- Odate, Asami (author)
- Brown Univ, Dept Chem, Providence, RI USA.
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- Pathak, Shashank (author)
- Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA.
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- Plekan, Oksana (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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Prince, Kevin C. (author)
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- Rebernik, Primoz (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Rouzee, Arnaud (author)
- Max Born Inst, Berlin, Germany.
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- Rudenko, Artem (author)
- Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA.
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- Simoncig, Alberto (author)
- Elettra Sincrotrone Trieste SCpA, Trieste, Italy.
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- Squibb, Richard J. (author)
- Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU),Univ Gothenburg, Dept Phys, Gothenburg, Sweden.
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- Venkatachalam, Anbu Selvam (author)
- Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA.
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- Vozzi, Caterina (author)
- CNR, Ist Foton & Nanotecnol, IFN, Milan, Italy.
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- Weber, Peter M. (author)
- Brown Univ, Dept Chem, Providence, RI USA.
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- Kirrander, Adam (author)
- Univ Oxford, Dept Chem, Phys & Theoret Chem Lab, Oxford, England.
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- Rolles, Daniel (author)
- Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA.
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Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA Univ Oxford, Dept Chem, Phys & Theoret Chem Lab, Oxford, England. (creator_code:org_t)
- Springer Nature, 2024
- 2024
- English.
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In: NATURE CHEMISTRY. - : Springer Nature. - 1755-4330 .- 1755-4349. ; 16, s. 499-505
- Related links:
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https://doi.org/10.1...
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https://uu.diva-port... (primary) (Raw object)
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https://gup.ub.gu.se...
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https://doi.org/10.1...
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https://urn.kb.se/re...
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Abstract
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- 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.
Subject headings
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Publication and Content Type
- ref (subject category)
- art (subject category)
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- By the author/editor
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Borne, Kurtis D.
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Cooper, Joseph C ...
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Ashfold, Michael ...
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Bachmann, Julien
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Bhattacharyya, S ...
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Boll, Rebecca
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show more...
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Bonanomi, Matteo
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Bosch, Michael
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Callegari, Carlo
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Centurion, Marti ...
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Coreno, Marcello
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Curchod, Basile ...
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Danailov, Miltch ...
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Demidovich, Alex ...
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Di Fraia, Michel ...
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Erk, Benjamin
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Facciala, Davide
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Feifel, Raimund
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Forbes, Ruaridh ...
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Hansen, Christop ...
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Holland, David M ...
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Ingle, Rebecca A ...
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Lindh, Roland, P ...
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Ma, Lingyu
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Mcghee, Henry G.
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Muvva, Sri Bhavy ...
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Nunes, Joao Pedr ...
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Odate, Asami
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Pathak, Shashank
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Plekan, Oksana
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Prince, Kevin C.
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Rebernik, Primoz
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Rouzee, Arnaud
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Rudenko, Artem
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Simoncig, Albert ...
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Squibb, Richard ...
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Venkatachalam, A ...
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Vozzi, Caterina
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Weber, Peter M.
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Kirrander, Adam
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Rolles, Daniel
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- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Physical Science ...
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and Atom and Molecul ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Physical Chemist ...
- Articles in the publication
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NATURE CHEMISTRY
- By the university
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University of Gothenburg
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Uppsala University