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Record W3015137859 · doi:10.1039/d0cp01213k

What is “many-body” dispersion and should I worry about it?

2020· article· en· W3015137859 on OpenAlexafffund
Alberto Otero‐de‐la‐Roza, Luc M. LeBlanc, Erin R. Johnson

Bibliographic record

VenuePhysical Chemistry Chemical Physics · 2020
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsDalhousie University
FundersNatural Sciences and Engineering Research Council of CanadaMinisterio de Asuntos Económicos y Transformación Digital, Gobierno de España
KeywordsDispersion (optics)WorryStatistical physicsChemical physicsPhysicsMaterials scienceOpticsPsychology

Abstract

fetched live from OpenAlex

Inclusion of dispersion effects in density-functional calculations is now standard practice in computational chemistry. In many dispersion models, the dispersion energy is written as a sum of pairwise atomic interactions consisting of a damped asymptotic expansion from perturbation theory. There has been much recent attention drawn to the importance of "many-body" dispersion effects, which by their name imply limitations with a pairwise atomic expansion. In this perspective, we clarify what is meant by many-body dispersion, as this term has previously referred to two very different physical phenomena, here classified as electronic and atomic many-body effects. Atomic many-body effects refer to the terms in the perturbation-theory expansion of the dispersion energy involving more than two atoms, the leading contribution being the Axilrod-Teller-Muto three-body term. Conversely, electronic many-body effects refer to changes in the dispersion coefficients of the pairwise terms induced by the atomic environment. Regardless of their nature, many-body effects cause pairwise non-additivity in the dispersion energy, such that the dispersion energy of a system does not equal the sum of the dispersion energies of its atomic pairs taken in isolation. A series of examples using the exchange-hole dipole moment (XDM) method are presented to assess the relative importance of electronic and atomic many-body effects on the dispersion energy. Electronic many-body effects can result in variation in the leading-order C6 dispersion coefficients by as much as 50%; hence, their inclusion is critical for good performance of a pairwise asymptotic dispersion correction. Conversely, atomic many-body effects represent less than 1% of the total dispersion energy and are much less significant than higher-order (C8 and C10) pairwise terms. Their importance has been previously overestimated through empirical fitting, where they can offset underlying errors stemming either from neglect of higher-order pairwise terms or from the base density functional.

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 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 categoriesMeta-epidemiology (narrow)
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 score0.064
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.001
Open science0.0000.001
Research integrity0.0000.001
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 head0.019
GPT teacher head0.272
Teacher spread0.253 · 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 teacher head, not a consensus.

Study designBench or experimental
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

Citations47
Published2020
Admission routes2
Has abstractyes

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