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Record W4295907191 · doi:10.1039/d2cp03029b

Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis

2022· article· en· W4295907191 on OpenAlexaff
Joseph McManus, Tiffany Walmsley, Kiyonobu Nagaya, James Harries, Yoshiaki Kumagai, Hiroshi Iwayama, Michael N. R. Ashfold, Mathew Britton, P. H. Bucksbaum, Taran Driver, David Heathcote, Paul Hockett, Andrew J. Howard, Edwin Kukk, Jason W. L. Lee, Yusong Liu, Dennis Milešević, Russell S. Minns, Akinobu Niozu, Johannes Niskanen, Andrew J. Orr‐Ewing, Shigeki Owada, Daniel Rolles, Patrick A. Robertson, Artem Rudenko, Kiyoshi Ueda, James Unwin, Claire Vallance, Michael Burt, M. Brouard, Ruaridh Forbes, Felix Allum

Bibliographic record

VenuePhysical Chemistry Chemical Physics · 2022
Typearticle
Languageen
FieldEngineering
TopicIon-surface interactions and analysis
Canadian institutionsNational Research Council Canada
FundersSLAC National Accelerator LaboratoryBasic Energy SciencesJesus College, University of OxfordHelmholtz AssociationJesus College, University of CambridgeEngineering and Physical Sciences Research CouncilJapan Society for the Promotion of ScienceOffice of ScienceU.S. Department of EnergyUniversity of SouthamptonScience and Technology Facilities CouncilStanford UniversityNational Science Foundation
KeywordsFragmentation (computing)IonDissociation (chemistry)Triatomic moleculeRotational–vibrational spectroscopyChemistryMetastabilityFemtosecondMolecular dynamicsAtomic physicsExcited statePhysicsComputational chemistryLaserMoleculeOpticsPhysical chemistry

Abstract

fetched live from OpenAlex

). By incorporating the recently developed native frames analysis approach into the three-dimensional covariance imaging procedure, contributions from three-body concerted and sequential fragmentation mechanisms can be isolated. The angular distribution of the fragment ions is much more complex than in previously reported studies for triatomic polycations, and differs substantially between the two isomeric species. With support of simple simulations of the dissociation channels of interest, detailed physical insights into the fragmentation dynamics are obtained, including how the initial dissociation step in a sequential mechanism influences rovibrational dynamics in the metastable intermediate ion and how signatures of this nuclear motion manifest in the measured signals.

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)0.001
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: none
Teacher disagreement score0.003
Threshold uncertainty score0.006

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0010.000
Science and technology studies0.0000.000
Scholarly communication0.0010.001
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0020.000

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 head0.229
Teacher spread0.224 · 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

Citations30
Published2022
Admission routes1
Has abstractyes

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