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Record W4409333601 · doi:10.1063/5.0253539

Signatures of rotation–translation couplings, symmetry-breaking, and intermolecular interactions in the rovibrational spectra of solid H2O@C60

2025· article· en· W4409333601 on OpenAlexafffund
J.-C. Chartrand, T. Putaud, Guillaume Bélanger, M. Bertin, J.-H. Fillion, Pascal Léveillé, X. Michaut, Patrick Ayotte

Bibliographic record

VenueThe Journal of Chemical Physics · 2025
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsUniversité de Sherbrooke
FundersInstitut national des sciences de l'UniversNatural Sciences and Engineering Research Council of CanadaAgence Nationale de la Recherche
KeywordsRotational–vibrational spectroscopyExcited stateIntermolecular forceSpectral lineMolecular physicsGround stateAtomic physicsChemistryPhysicsMoleculeQuantum mechanics

Abstract

fetched live from OpenAlex

Some spectral features observed in the rovibrational spectra of solid H2O@C60 are shown to provide spectroscopic signatures of confinement-induced perturbations related to the coupling between the orientational and positional degrees-of-freedom of the water molecules. Their attribution to either para-H2O@C60 or ortho-H2O@C60 is established from their behavior during nuclear spin conversion. The frequency of the rovibrational transitions that emanate from their ground ro-translational (RT) states appears conspicuously redshifted from that of the corresponding transitions in the free water molecule in the gas phase. However, a few of the 21 hot band spectral features, and one ground state transition, observed in the infrared spectrum of solid H2O@C60 and reported here for the first time, cannot be straightforwardly assigned based on the softening of its intramolecular HOH bending and OH stretching vibrational modes due to confinement within C60. The most strongly perturbed transitions provide insights into the complex confinement-induced quantum nuclear dynamics arising from rotation-translation coupling, allowing the topology of the confinement potential to be revealed using a simple confined rotor model [Putaud et al., J. Chem. Phys. 162, 144313 (2025)]. While the line profiles exhibited by most of the transitions are consistent with symmetry-breaking interactions arising from merohedral disorder in solid H2O@C60, evidence for additional perturbations of the 10100 RT state, in the ground and vibrationally excited manifolds, is reported. Moreover, the line profiles displayed by the transitions emanating from the ground RT state of para-H2O@C60 and the observation of nominally forbidden Q-branch transitions, in the intramolecular HOH bending and symmetric OH stretching ranges of solid H2O@C60 samples with a fill ratio of 75%, are shown to provide a spectroscopic signature of intermolecular dipolar interactions between nearest-neighbor H2O@C60 molecules.

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: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.003
Threshold uncertainty score0.010

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0010.000
Science and technology studies0.0000.001
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.001
Insufficient payload (model declined to judge)0.0030.000

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 head0.010
GPT teacher head0.290
Teacher spread0.280 · 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

Citations5
Published2025
Admission routes2
Has abstractyes

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