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Record W2914763788 · doi:10.1063/1.5085011

<i>Ab initio</i> investigation of Br-3<i>d</i> core-excited states in HBr and HBr+ toward XUV probing of photochemical dynamics

2019· article· en· W2914763788 on OpenAlexafffund
Yuki Kobayashi, Tao Zeng, Daniel M. Neumark, Stephen R. Leone

Bibliographic record

VenueStructural Dynamics · 2019
Typearticle
Languageen
FieldPhysics and Astronomy
TopicX-ray Spectroscopy and Fluorescence Analysis
Canadian institutionsCarleton University
FundersArmy Research OfficeDivision of ChemistryNatural Sciences and Engineering Research Council of CanadaCarleton UniversityNational Institutes of HealthNational Science Foundation
KeywordsExcited stateValence (chemistry)Absorption spectroscopyChemistryAtomic physicsElectronic structureUltrafast laser spectroscopyMolecular electronic transitionSpectroscopyMolecular physicsPhysicsComputational chemistryQuantum mechanics

Abstract

fetched live from OpenAlex

Ultrafast X-ray/XUV transient absorption spectroscopy is a powerful tool for real-time probing of chemical dynamics. Interpretation of the transient absorption spectra requires knowledge of core-excited potentials, which necessitates assistance from high-level electronic-structure computations. In this study, we investigate Br-3d core-excited electronic structures of hydrogen bromide (HBr) using spin-orbit general multiconfigurational quasidegenerate perturbation theory (SO-GMC-QDPT). Potential energy curves and transition dipole moments are calculated from the Franck-Condon region to the asymptotic limit and used to construct core-to-valence absorption strengths for five electronic states of HBr (Σ10+, 3Π1, 1Π1, 3Π0+, 3Σ1) and two electronic states of HBr+ (2Π3∕2, 2Σ1∕2). The results illustrate the capabilities of Br-3d edge probing to capture transitions of the electronic-state symmetry as well as nonadiabatic dissociation processes that evolve across avoided crossings. Furthermore, core-to-valence absorption spectra are simulated from the neutral Σ10+ state and the ionic Π21/2,3/2 states by numerically solving the time-dependent Schrödinger equation and exhibit excellent agreement with the experimental spectrum. The comprehensive and quantitative picture of the core-excited states obtained in this work allows for transparent analysis of the core-to-valence absorption signals, filling gaps in the theoretical understanding of the Br-3d transient absorption spectra.

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: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.003
Threshold uncertainty score0.005

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 science0.0010.000
Research integrity0.0010.000
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 head0.006
GPT teacher head0.234
Teacher spread0.227 · 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 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

Citations11
Published2019
Admission routes2
Has abstractyes

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