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Atomic Trajectories of a Bimolecular Reaction Visualized by Ultrafast Electron Diffraction

2025· preprint· en· W4411882476 on OpenAlexafffund
R. Patrick Xian, Stuart A. Hayes, Gastón Corthey, Carole A. Morrison, Alexander Marx, Hazem Daoud, Cheng Lü, R. J. Dwayne Miller

Bibliographic record

VenueChemRxiv · 2025
Typepreprint
Languageen
FieldChemistry
TopicVarious Chemistry Research Topics
Canadian institutionsUniversity of Toronto
FundersMax-Planck-GesellschaftEngineering and Physical Sciences Research CouncilUniversity of TorontoHamburg Centre for Ultrafast ImagingAlexander von Humboldt-Stiftung
KeywordsUltrafast electron diffractionDiffractionUltrashort pulseElectronElectron diffractionAtomic physicsChemistryPhysicsMaterials scienceOpticsLaserNuclear physics

Abstract

fetched live from OpenAlex

Bimolecular reactions are ubiquitous in chemistry, but it is exceptionally difficult to resolve the motion of atoms for such processes on the ultrafast timescales that the breaking and creation of chemical bonds occur. Detecting small changes in atom positions requires high temporal and spatial resolution and reliable signal-to-noise characteristics. Here, we have exploited solid-state alignment to track a photoinduced bimolecular disproportionation reaction that transforms two pairs of adjacent triiodide anions into the metastable tetraiodide molecule and the diiodide fragment. We use ultrafast electron diffraction and dynamic structure refinement, where the atomic displacements are directly reconstructed from the diffraction data with plausible restraints on the atomic trajectories starting from the known ground-state structure. The excited-state structures are supported by theoretical calculations in the solid state and the reaction courses show clear site dependence on the ultrafast timescale. Our results provide a close-up view of the atomic motions involved in this classic reaction in real time, from bond elongation to breaking at the parent ion, to collision and subsequent bond formation of the liberated I atom with the neighbouring triiodide, all within a picosecond.

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 distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
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 score0.007
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0010.002
Insufficient payload (model declined to judge)0.0000.000

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 head0.013
GPT teacher head0.310
Teacher spread0.297 · 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 teacher head, not a consensus.

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

Citations0
Published2025
Admission routes2
Has abstractyes

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