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Record W4414691310 · doi:10.1021/jacs.5c08730

Visualizing the Three-Dimensional Arrangement of Hydrogen Atoms in Organic Molecules by Coulomb Explosion Imaging

2025· article· en· W4414691310 on OpenAlexaff
Alice E. Green, Keyu Chen, Surjendu Bhattacharyya, Felix Allum, Sergey Usenko, Michael N. R. Ashfold, T. Baumann, Kurtis Borne, M. Brouard, Michael Burt, Basile F. E. Curchod, Benjamin Erk, Ruaridh Forbes, Lea M. Ibele, Rebecca A. Ingle, Huynh Van Sa Lam, Xiang Li, Kang Lin, Tommaso Mazza, Joseph McManus, Michaël Meyer, Terry Mullins, J. Pedro F. Nunes, Daniel E. Rivas, Aljoscha Roerig, Arnaud Rouzée, Philipp Schmidt, John S. Searles, Björn Senfftleben, Henrik Stapelfeldt, Rico Mayro P. Tanyag, Florian Trinter, Anbu Selvam Venkatachalam, Enliang Wang, Emily M. Warne, Thomas Wolf, T. Jahnke, Artem Rudenko, Rebecca Boll, Daniel Rolles

Bibliographic record

VenueJournal of the American Chemical Society · 2025
Typearticle
Languageen
FieldChemistry
TopicMass Spectrometry Techniques and Applications
Canadian institutionsTrent University
FundersHORIZON EUROPE Marie Sklodowska-Curie ActionsH2020 European Research CouncilBasic Energy SciencesEngineering and Physical Sciences Research CouncilLaboratoire d’excellence Physique Atomes Lumière MatièreDivision of PhysicsAgence Nationale de la RechercheHORIZON EUROPE Framework ProgrammeOffice of ScienceU.S. Department of EnergyEuropean CommissionDeutsche ForschungsgemeinschaftVillum FondenChemical Sciences, Geosciences, and Biosciences DivisionNational Science Foundation
KeywordsCoulomb explosionFemtosecondMoleculeHydrogenAtom (system on chip)CoulombMolecular dynamicsMolecular orbitalCoupling (piping)

Abstract

fetched live from OpenAlex

Structure-sensitive methods based on femtosecond light or electron pulses are now making it possible to measure how molecular structures change during light-induced processes. Despite significant progress, high-fidelity imaging of nuclear positions remains a challenge even for relatively small molecular systems and, notably, regarding the positions of hydrogen atoms. As demonstrated in recent work, X-ray-induced Coulomb explosion imaging (CEI) may overcome this obstacle, as its sensitivity does not depend on the mass of the imaged atoms. The photoinduced ring opening of the heterocyclic molecule 2(5 H )-thiophenone has attracted recent interest. Here, we show that CEI offers a powerful route to imaging the peripheral H atoms in this molecule and thus, more generally, to tracking detailed nuclear motions (e.g., isomerizations) in organic molecules on ultrafast time scales. Specifically, we record momentum-space Coulomb explosion images that report on the three-dimensional positioning of all nuclei within the molecule, for instance, distinguishing H atoms in C–H bonds that lie within or are directed out of the plane defined by the heavy atoms. The prospect of imaging peripheral H atoms to probe photochemical dynamics is explored by coupling ab initio molecular dynamics with classical Coulomb explosion simulations, thereby differentiating potential photoproduct isomers, including those whose structures primarily differ in the position of the hydrogens.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.001
Threshold uncertainty score0.004

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0010.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.007
GPT teacher head0.268
Teacher spread0.262 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations3
Published2025
Admission routes1
Has abstractyes

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