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Record W4244207035 · doi:10.26434/chemrxiv.11907288.v1

A Collocation-Based Multi-Configuration Time-Dependent Hartree Method Using Mode Combination and Improved Relaxation

2020· preprint· en· W4244207035 on OpenAlexafffund
Robert Wodraszka, Tucker Carrington

Bibliographic record

VenueChemRxiv · 2020
Typepreprint
Languageen
FieldChemistry
TopicAdvanced NMR Techniques and Applications
Canadian institutionsQueen's University
FundersCompute Canada
KeywordsHartreeCollocation (remote sensing)Relaxation (psychology)Applied mathematicsBasis functionCollocation methodMathematicsMathematical optimizationComputer scienceMathematical analysisQuantum mechanicsPhysicsOrdinary differential equationDifferential equation

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 PES be in 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 called 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 mode combination collocation multiconfiguration time-dependent Hartree method (MC-C-MCTDH). In practice, its cost does not scale exponentially with the number of atoms in the system and it can be easily used with any general potential energy surfaces (PES); the PES need not be a 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 the 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 rather than starting from a variational principle. Because the MC basis functions are multivariate, collocation points in multidimensional spaces are required. We use two types of collocation points: 1) DVR (discrete variable representation)-like points obtained from (approximate) simultaneous diagonalisation of matrices; and 2) Leja points, which are known to be good interpolation points, determined from a generalised recipe suitable for any (not necessarily polynomial-type) 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 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)0.001
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: Methods · Consensus signal: Methods
Teacher disagreement score0.003
Threshold uncertainty score0.008

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0010.000
Meta-epidemiology (broad)0.0010.001
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0010.001
Open science0.0020.001
Research integrity0.0010.001
Insufficient payload (model declined to judge)0.0020.001

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 head0.037
GPT teacher head0.335
Teacher spread0.298 · 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
GenreMethods

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".

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Citations0
Published2020
Admission routes2
Has abstractyes

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