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Record W3021973509 · doi:10.1063/5.0006081

A collocation-based multi-configuration time-dependent Hartree method using mode combination and improved relaxation

2020· article· en· W3021973509 on OpenAlexafffund
Robert Wodraszka, Tucker Carrington

Bibliographic record

VenueThe Journal of Chemical Physics · 2020
Typearticle
Languageen
FieldChemistry
TopicAdvanced NMR Techniques and Applications
Canadian institutionsQueen's University
FundersNatural Sciences and Engineering Research Council of Canada
KeywordsHartreeCollocation (remote sensing)Relaxation (psychology)Interpolation (computer graphics)Applied mathematicsBasis functionMathematicsMathematical optimizationComputer scienceMathematical analysisQuantum mechanicsPhysics

Abstract

fetched live from OpenAlex

Although very useful, the original multi-configuration time-dependent Hartree (MCTDH) method has two weaknesses: (1) its cost scales exponentially with the number of atoms in the system; (2) the standard MCTDH implementation requires that the potential energy surface (PES) be in the sum-of-product (SOP) form in order to reduce the cost of computing integrals in the MCTDH basis. One way to deal with (1) is to lump coordinates into groups. This is mode combination (MC). One way to deal with (2) is to reformulate MCTDH using collocation so that there are no integrals. In this paper, we combine MC and collocation to formulate a MC collocation multi-configuration time-dependent Hartree (MC-C-MCTDH) method. In practice, its cost does not scale exponentially with the number of atoms, and it can be used with any general PES; the PES need not be an SOP and need not have a special form. No integrals and, hence, no quadratures are necessary. We demonstrate the accuracy and efficiency of the new method by computing vibrational energy eigenstates of methyl radical, methane, and acetonitrile. To do this, we use MC-C-MCTDH with a variant of improved relaxation, derived by evaluating a residual at points. Because the MC basis functions are multivariate, collocation points in multi-dimensional spaces are required. We use two types of collocation points: (1) discrete variable representation-like points obtained from (approximate) simultaneous diagonalization of matrices and (2) Leja points, which are known to be good interpolation points, determined from a generalized recipe suitable for any basis.

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: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: none
Teacher disagreement score0.812
Threshold uncertainty score0.302

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 head0.028
GPT teacher head0.313
Teacher spread0.285 · 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 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

Citations17
Published2020
Admission routes2
Has abstractyes

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