Capturing Ring Opening in Photoexcited Enolic Acetylacetone upon Hydrogen Bond Dissociation by Ultrafast Electron Diffraction Article Swipe
Valeriu Scutelnic
,
Denis S. Tikhonov
,
Sonia Marggi Poullain
,
Eric A. Haugen
,
Andrew Attar
,
Lou Barreau
,
Kristina F. Chang
,
Ashley P. Fidler
,
James D. Gaynor
,
Yen-Cheng Lin
,
Jie Yang
,
Elio G. Champenois
,
Xijie Wang
,
Xiaozhe Shen
,
Duan Luo
,
Fuhao Ji
,
Stephen Weathersby
,
Yury V. Vishnevskiy
,
Melanie Schnell
,
Thomas Wolf
,
Ming‐Fu Lin
,
Stephen R. Leone
·
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1021/acs.jpclett.5c00285
YOU?
·
· 2025
· Open Access
·
· DOI: https://doi.org/10.1021/acs.jpclett.5c00285
Photoinduced biological and chemical reactions are often based on key structural transformations of a molecule driven across multiple electronic states. Acetylacetone (AcAc) is a prototypical system for complex chemical pathways involving several conical intersections (CI) and singlet-triplet intersystem crossings (ISC) characterized by distinct geometries. In the gas phase, AcAc is predominantly in a planar ring-like enolic form stabilized by a strong intramolecular O-H···O hydrogen bond. Following excitation into the S2 (ππ*) state at 266 nm, acetylacetone undergoes rapid internal conversion followed by intersystem crossing. Such relaxation pathways are associated with structural changes including ring opening, deplanarization, and bond elongation. In this work, ultrafast electron diffraction (UED) at the SLAC MeV-UED setup is employed as a direct structural probe with a time resolution of 160 fs. Together with trajectory surface hopping simulations, analysis of the UED data provides a new perspective on the early time nuclear dynamics in acetylacetone. Specifically, AcAc is observed to undergo ring opening, deplanarization, and bond elongation all within the first 700 fs after photoexcitation. The monitored dynamics is associated mainly with the nuclear motion on the S1 potential energy surface, formed after very rapid transfer from S2 to S1, allowing AcAc to reach the conical intersection to intersystem crossing. Such time scales of nuclear motion are contrasted with the time scales of electronic transitions in AcAc that were previously characterized with spectroscopic methods, specifically internal conversion (<100 fs) and intersystem crossing (∼1.5 ps).
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Metadata
- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acs.jpclett.5c00285
- OA Status
- hybrid
- Cited By
- 1
- References
- 42
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W4410374315
All OpenAlex metadata
Raw OpenAlex JSON
- OpenAlex ID
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https://openalex.org/W4410374315Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1021/acs.jpclett.5c00285Digital Object Identifier
- Title
-
Capturing Ring Opening in Photoexcited Enolic Acetylacetone upon Hydrogen Bond Dissociation by Ultrafast Electron DiffractionWork title
- Type
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articleOpenAlex work type
- Language
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enPrimary language
- Publication year
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2025Year of publication
- Publication date
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2025-05-14Full publication date if available
- Authors
-
Valeriu Scutelnic, Denis S. Tikhonov, Sonia Marggi Poullain, Eric A. Haugen, Andrew Attar, Lou Barreau, Kristina F. Chang, Ashley P. Fidler, James D. Gaynor, Yen-Cheng Lin, Jie Yang, Elio G. Champenois, Xijie Wang, Xiaozhe Shen, Duan Luo, Fuhao Ji, Stephen Weathersby, Yury V. Vishnevskiy, Melanie Schnell, Thomas Wolf, Ming‐Fu Lin, Stephen R. LeoneList of authors in order
- Landing page
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https://doi.org/10.1021/acs.jpclett.5c00285Publisher landing page
- Open access
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YesWhether a free full text is available
- OA status
-
hybridOpen access status per OpenAlex
- OA URL
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https://doi.org/10.1021/acs.jpclett.5c00285Direct OA link when available
- Concepts
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Acetylacetone, Dissociation (chemistry), Hydrogen bond, Ring (chemistry), Photochemistry, Electron diffraction, Chemistry, Electron, Diffraction, Physical chemistry, Molecule, Physics, Inorganic chemistry, Organic chemistry, Optics, Quantum mechanicsTop concepts (fields/topics) attached by OpenAlex
- Cited by
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1Total citation count in OpenAlex
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2025: 1Per-year citation counts (last 5 years)
- References (count)
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42Number of works referenced by this work
- Related works (count)
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10Other works algorithmically related by OpenAlex
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