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Record W2094790566 · doi:10.1063/1.1589734

Accurate analytic He–H2 potential energy surface from a greatly expanded set of <i>ab initio</i> energies

2003· article· en· W2094790566 on OpenAlex
Arnold I. Boothroyd, P. G. Martin, Michael R. Peterson

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueThe Journal of Chemical Physics · 2003
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsCanadian Institute for Theoretical AstrophysicsUniversity of Toronto
Fundersnot available
KeywordsAb initioDissociation (chemistry)Ab initio quantum chemistry methodsBond-dissociation energyAtomic physicsBasis setChemistryMoleculePotential energy surfaceMolecular physicsPhysicsPhysical chemistry

Abstract

fetched live from OpenAlex

The interaction potential energy surface (PES) of He–H2 is of great importance for quantum chemistry, as the simplest test case for interactions between a molecule and a closed-shell atom. It is also required for a detailed understanding of certain astrophysical processes—namely, collisional excitation and dissociation of H2 in molecular clouds—at densities too low to be accessible experimentally. A new set of 23 703 ab initio energies was computed for He–H2 geometries where the interaction energy was expected to be non-negligible. These have an estimated rms “random” error of ∼0.2 mhartree and a systematic error of ∼0.6 mhartree (0.4 kcal/mol). A new analytic He–H2 PES, with 112 parameters, was fitted to 20 203 of these new ab initio energies (and to an additional 4862 points generated at large separations). This yielded an improvement by better than an order of magnitude in the fit to the interaction region, relative to the best previous surfaces (which were accurate only for near-equilibrium H2 molecule sizes). This new PES has an rms error of 0.95 mhartree (0.60 kcal/mol) relative to the 14 585 ab initio energies that lie below twice the H2 dissociation energy and 2.97 mhartree (1.87 kcal/mol) relative to the full set of 20 203 ab initio energies (the fitting procedure used a reduced weight for high energies, yielding a weighted rms error of 1.42 mhartree—i.e., 0.89 kcal/mol). These rms errors are comparable to the estimated error in the ab initio energies themselves; the conical intersection between the ground state and the first excited state is the largest source of error in the PES.

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.

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: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.285
Threshold uncertainty score0.845

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
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)0.0000.000

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 head0.016
GPT teacher head0.250
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