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Record W4410731533 · doi:10.1021/jacs.5c03968

Herzberg Type-I or Type-II Predissociation Dynamics at the Conical Intersection: Bifurcation into Adiabatic or Nonadiabatic Pathway

2025· article· en· W4410731533 on OpenAlexaff
Kyung Chul Woo, Sang Kyu Kim

Bibliographic record

VenueJournal of the American Chemical Society · 2025
Typearticle
Languageen
FieldPhysics and Astronomy
Topicstochastic dynamics and bifurcation
Canadian institutionsKootenay Association for Science & Technology
FundersNational Research Foundation of Korea
KeywordsChemistryConical intersectionBifurcationAdiabatic processType (biology)Intersection (aeronautics)Conical surfaceDynamics (music)GeometryQuantum mechanicsPhysicsMoleculeAerospace engineering

Abstract

fetched live from OpenAlex

Bifurcation dynamics into Herzberg type-I and type-II predissociation pathways at the conical intersection have been characterized in terms of their distinct reaction rates and energy-disposal dynamics from the picosecond time-resolved product state distributions measured at multiple S 1 /S 2 vibronic states of thioanisole (C 6 H 5 SCH 3 ). Electronic predissociation (type-I) occurs on a faster time scale and leads to the larger translational energies being released to the fragments (C 6 H 5 S • + • CH 3 ) compared to the vibrational predissociation (type-II). While type-II dominates at the S 1 zero-point level, the type-I quantum yield increases sharply near the S 1 /S 2 conical intersection, which is consistent with the striking dynamic resonance observed for the reactive flux in the proximity of the conical intersection. Nonadiabatic product yield at the asymptotic limit was found to be enhanced predominantly through the type-I channel, suggesting that the quantum-mechanical nature of the reactive flux prepared near the first S 1 /S 2 conical intersection is likely to be retained at the second S 0 /S 2 conical intersection encountered in the later stage as there is little time to be altered during the ultrafast S-CH 3 bond extension on the repulsive potential energy curve linking two conical intersections, enabling nonadiabatic control over product yields through the state-selection of the reactive flux.

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 categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Simulation or modeling · Consensus signal: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.717
Threshold uncertainty score0.277

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

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 head0.006
GPT teacher head0.258
Teacher spread0.252 · 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.

The models applied no category: nothing in the taxonomy fit this work.
Study designSimulation or modeling
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

Citations4
Published2025
Admission routes1
Has abstractyes

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