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Record W4377565549 · doi:10.1063/5.0142465

Many-body dispersion in model systems and the sensitivity of self-consistent screening

2023· article· en· W4377565549 on OpenAlexafffund
Kyle R. Bryenton, Erin R. Johnson

Bibliographic record

VenueThe Journal of Chemical Physics · 2023
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsDalhousie University
FundersNatural Sciences and Engineering Research Council of CanadaKillam Trusts
KeywordsDipoleLondon dispersion forceIntermolecular forceFormalism (music)Dispersion (optics)Statistical physicsHarmonic oscillatorPhysicsPolarization (electrochemistry)ChemistryQuantum mechanicsMoleculePhysical chemistryvan der Waals force

Abstract

fetched live from OpenAlex

London dispersion is a weak, attractive, intermolecular force that occurs due to interactions between instantaneous dipole moments. While individual dispersion contributions are small, they are the dominating attractive force between nonpolar species and determine many properties of interest. Standard semi-local and hybrid methods in density-functional theory do not account for dispersion contributions, so a correction such as the exchange-hole dipole moment (XDM) or many-body dispersion (MBD) models must be added. Recent literature has discussed the importance of many-body effects on dispersion, and attention has turned to which methods accurately capture them. By studying systems of interacting quantum harmonic oscillators from first principles, we directly compare computed dispersion coefficients and energies from XDM and MBD and also study the influence of changing oscillator frequency. Additionally, the 3-body energy contributions for both XDM, via the Axilrod-Teller-Muto term, and MBD, via a random-phase approximation formalism, are calculated and compared. Connections are made to interactions between noble gas atoms as well as to the methane and benzene dimers and to two layered materials, graphite and MoS2. While XDM and MBD give similar results for large separations, some variants of MBD are found to be susceptible to a polarization catastrophe at short range, and the MBD energy calculation is seen to fail in some chemical systems. Additionally, the self-consistent screening formalism used in MBD is shown to be surprisingly sensitive to the choice of input polarizabilities.

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)0.001
metaresearch head score (Gemma)0.005
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 score0.004
Threshold uncertainty score0.009

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0010.005
Meta-epidemiology (narrow)0.0010.000
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0010.001
Science and technology studies0.0010.002
Scholarly communication0.0010.001
Open science0.0010.001
Research integrity0.0010.001
Insufficient payload (model declined to judge)0.0020.000

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 head0.015
GPT teacher head0.246
Teacher spread0.231 · 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

Citations9
Published2023
Admission routes2
Has abstractyes

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