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Record W2418357297 · doi:10.1021/acs.jctc.5b00044

Predicting Energetics of Supramolecular Systems Using the XDM Dispersion Model

2015· article· en· W2418357297 on OpenAlexafffund
Alberto Otero‐de‐la‐Roza, Erin R. Johnson

Bibliographic record

VenueJournal of Chemical Theory and Computation · 2015
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsDalhousie UniversityNational Institute for Nanotechnology
FundersMinisterio de Ciencia e InnovaciónAlberta Innovates - Technology Futures
KeywordsCounterpoiseBasis setQuadrupoleSupramolecular chemistryDipoleDispersion (optics)ChemistryMaterials sciencePhysicsComputational chemistryStatistical physicsDensity functional theoryAtomic physicsQuantum mechanicsMolecule

Abstract

fetched live from OpenAlex

In this article, we examine the ability of the exchange-hole dipole moment (XDM) model of dispersion to treat large supramolecular systems. We benchmark several XDM-corrected functionals on the S12L set proposed by Grimme, which comprises large dispersion-bound host-guest systems, for which back-corrected experimental and Quantum Monte Carlo (QMC) reference data are available. PBE-XDM coupled with the relatively economical and efficient pc-2-spd basis set gives excellent statistics (mean absolute error (MAE) = 1.5 kcal/mol), below the deviation between experimental and QMC data. When compared only to the (more accurate) QMC results, PBE-XDM/pc-2-spd (MAE = 1.2 kcal/mol) outperforms all other dispersion-corrected DFT results in the literature, including PBE-dDsC/QZ4P (6.2 kcal/mol), PBE-NL/def2-QZVP (4.7 kcal/mol), PBE-D2/def2-QZVP' (3.5 kcal/mol), PBE-D3/def2-QZVP'(2.3 kcal/mol), M06-L/def2-QZVP (1.9 kcal/mol), and PBE-MBD (1.8 kcal/mol), with no significant bias (mean error (ME) = 0.04 kcal/mol). PBE-XDM/pc-2-spd gives binding energies relatively close to the complete basis-set limit and does not necessitate the use of counterpoise corrections, which facilitates its use. The dipole-quadrupole and quadrupole-quadrupole pairwise dispersion terms (C8 and C10) are critical for the correct description of the dimers. XDM-corrected functionals different from PBE that work well for small dimers do not yield good accuracy for the large supramolecular systems in the S12L, presenting errors that scale linearly with the dispersion contribution to the binding energy.

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 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 score0.470
Threshold uncertainty score0.178

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
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 science0.0000.000
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 head0.020
GPT teacher head0.276
Teacher spread0.256 · 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.

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

Citations42
Published2015
Admission routes2
Has abstractyes

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