ArticleJournal of the American Chemical Society2025
Mapping Excited-State Decay Mechanisms in Acetylacetone by Sub-20 fs Time-Resolved Photoelectron Spectroscopy.
Article in Journal of the American Chemical Society, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 3 papers.
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Who cites it
3 citing papers in PubMed.
- 3-fs-resolved UV/XUV photoelectron spectroscopy in the gas phase.Nature communications · 2026Article
- Electronic and Inertial Effects of Methylation on Excited-State Hydrogen Transfer.The journal of physical chemistry. A · 2026Article
- Simulation of time-resolved site-selective X-ray spectroscopy tracing nonadiabatic dynamics inPhysical chemistry chemical physics : PCCP · 2025Article
Corrections and comments
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Authors and funding
13 authors.
Funding
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Abstract
Excited-State Intramolecular Hydrogen Transfer (ESIHT) is one of the fastest chemical reactions, occurring on the order of tens of femtoseconds and playing a critical role in light-driven biological processes and technological applications. Here, we investigate the early stages of coupled nuclear-electron dynamics using acetylacetone (AcAc) as a model system exhibiting ESIHT. We employ ultraviolet-extreme ultraviolet (UV-XUV) time-resolved photoelectron spectroscopy (tr-PES) with sub-20 fs resolution in combination with high-level dynamically correlated simulations (CASPT2) to map the electronic relaxation pathways and vibrational modes driving this process. Our results provide distinct spectroscopic signatures of ESIHT occurring within the first 20 fs and resolve the active vibrational modes, showing the intricate evolution of the electronic and nuclear degrees of freedom. Moreover, the analysis reveals the key role of ultrafast intersystem crossing (ISC) to triplet states in modulating the excited-state dynamics and its implications for the overall relaxation pathways. These findings refine our understanding of the photochemistry of AcAc and suggest general principles that can be applied to similar conjugated systems.
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Registered trials
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