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Record W4406706160 · doi:10.1063/5.0241872

Alchemical harmonic approximation based potential for iso-electronic diatomics: Foundational baseline for Δ-machine learning

2025· article· en· W4406706160 on OpenAlex

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.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenueThe Journal of Chemical Physics · 2025
Typearticle
Languageen
FieldMaterials Science
TopicMachine Learning in Materials Science
Canadian institutionsVector InstituteUniversity of Toronto
FundersHORIZON EUROPE European Research CouncilNatural Sciences and Engineering Research Council of CanadaCanada First Research Excellence Fund
KeywordsDiatomic moleculeAtomic physicsAnsatzWave functionElectronic structureHarmonic oscillatorElectronPhysicsCharge (physics)Potential energyChemistryQuantum mechanics

Abstract

fetched live from OpenAlex

We introduce the alchemical harmonic approximation (AHA) of the absolute electronic energy for charge-neutral iso-electronic diatomics at fixed interatomic distance d0. To account for variations in distance, we combine AHA with this ansatz for the electronic binding potential, E(d)=(Eu-Es)Ec-EsEu-Esd/d0+Es, where Eu, Ec, Es correspond to the energies of the united atom, calibration at d0, and the sum of infinitely separated atoms, respectively. Our model covers the two-dimensional electronic potential energy surface spanned by distances of 0.7-2.5 Å and differences in nuclear charge from which only one single point (with elements of nuclear charge Z1, Z2, and distance d0) is drawn to calibrate Ec. Using reference data from pbe0/cc-pVDZ, we present numerical evidence for the electronic ground-state of all neutral diatomics with 8, 10, 12, and 14 electrons. We assess the validity of our model by comparison to legacy interatomic potentials (harmonic oscillator, Lennard-Jones, and Morse) within the most relevant range of binding (0.7-2.5 Å) and find comparable accuracy if restricted to single diatomics and significantly better predictive power when extrapolating to the entire iso-electronic series. We also investigated Δ-learning of the electronic absolute energy using our model as a baseline. This baseline model results in a systematic improvement, effectively reducing training data needed for reaching chemical accuracy by up to an order of magnitude from ∼1000 to ∼100. By contrast, using AHA+Morse as a baseline hardly leads to any improvement and sometimes even deteriorates the predictive power. Inferring the energy of unseen CO converges to a prediction error of ∼0.1 Ha in direct learning and ∼0.04 Ha with our baseline.

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)0.003
metaresearch head score (Gemma)0.001
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: none
Teacher disagreement score0.633
Threshold uncertainty score0.527

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0030.001
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 integrity0.0000.000
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 head0.010
GPT teacher head0.270
Teacher spread0.261 · 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