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Record W7137545147

Exploring the ultrafast and isomer-dependent photodissociation of iodothiophenes via site-selective ionization

2024· article· en· W7137545147 on OpenAlexaff
Razmus Weronika O., Allum Felix, Harries James, Kumagai Yoshiaki, Nagaya Kiyonobu, Bhattacharyya Surjendu, Britton Mathew, Brouard Mark, Bucksbaum Philip H., Cheung Kieran, Crane Stuart W., Fushitani Mizuho, Gabalski Ian, Gejo Tatsuo, Ghrist Aaron, Heathcote David, Hikosaka Yasumasa, Hishikawa Akiyoshi, Hockett Paul, Jones Ellen, Kukk Edwin, Iwayama Hiroshi, Lam Huynh V. S., McManus Joseph W., Milesevic Dennis, Mikosch Jochen, Minemoto Shinichirou, Niozu Akinobu, Orr-Ewing Andrew J., Owada Shigeki, Rolles Daniel, Rudenko Artem, Townsend Dave, Ueda Kiyoshi, Unwin James, Vallance Claire, Venkatachalam Anbu, Wada Shin-ichi, Walmsley Tiffany, Warne Emily M., Woodhouse Joanne L., Burt Michael, Ashfold Michael N. R., Minns Russell S., Forbes Ruaridh

Bibliographic record

VenueInstitutional Repositories DataBase (IRDB) · 2024
Typearticle
Languageen
FieldPhysics and Astronomy
TopicLaser-Matter Interactions and Applications
Canadian institutionsNational Research Council Canada
FundersSLAC National Accelerator LaboratoryChemical Sciences, Geosciences, and Biosciences DivisionBasic Energy SciencesJapan Society for the Promotion of ScienceJesus College, University of OxfordJesus College, University of CambridgeOffice of ScienceKing Saud UniversityUniversity of BristolScience and Technology Facilities CouncilEuropean CommissionU.S. Department of EnergyLincoln College, University of OxfordLeverhulme TrustUniversity of SouthamptonEngineering and Physical Sciences Research CouncilUniversity of Oxford
KeywordsDissociation (chemistry)Coulomb explosionPhotoexcitationPhotodissociationIonizationKinetic energyIonExcitation
DOInot available

Abstract

fetched live from OpenAlex

C-I bond extension and fission following ultraviolet (UV, 262 nm) photoexcitation of 2- and 3-iodothiophene is studied using ultrafast time-resolved extreme ultraviolet (XUV) ionization in conjunction with velocity map ion imaging. The photoexcited molecules and eventual I atom products are probed by site-selective ionization at the I 4d edge using intense XUV pulses, which induce multiple charges initially localized to the iodine atom. At C-I separations below the critical distance for charge transfer (CT), charge can redistribute around the molecule leading to Coulomb explosion and charged fragments with high kinetic energy. At greater C-I separations, beyond the critical distance, CT is no longer possible and the measured kinetic energies of the charged iodine atoms report on the neutral dissociation process. The time and momentum resolved measurements allow determination of the timescales and the respective product momentum and kinetic energy distributions for both isomers, which are interpreted in terms of rival 'direct' and 'indirect' dissociation pathways. The measurements are compared with a classical over the barrier model, which reveals that the onset of the indirect dissociation process is delayed by ∼1 ps relative to the direct process. The kinetics of the two processes show no discernible difference between the two parent isomers, but the branching between the direct and indirect dissociation channels and the respective product momentum distributions show isomer dependencies. The greater relative yield of indirect dissociation products from 262 nm photolysis of 3-iodothiophene (cf. 2-iodothiophene) is attributed to the different partial cross-sections for (ring-centred) π∗ ← π and (C-I bond localized) σ∗ ← (n/π) excitation in the respective parent isomers.

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 head0.024
GPT teacher head0.258
Teacher spread0.234 · 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

Citations0
Published2024
Admission routes1
Has abstractyes

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