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Record W2061699954 · doi:10.1021/ct100012y

Dual Grid Methods for Finding the Reaction Path on Reduced Potential Energy Surfaces

2010· article· en· W2061699954 on OpenAlexafffund
Steven K. Burger, Paul W. Ayers

Bibliographic record

VenueJournal of Chemical Theory and Computation · 2010
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsMcMaster University
FundersNatural Sciences and Engineering Research Council of CanadaInstitute of Museum and Library Services
KeywordsGridInterpolation (computer graphics)OverfittingComputer scienceFast marching methodExtrapolationPath (computing)Curse of dimensionalityAlgorithmMathematical optimizationLimitingEnergy (signal processing)MathematicsArtificial intelligenceStatisticsGeometryArtificial neural network

Abstract

fetched live from OpenAlex

Two new algorithms are presented for determining the minimum energy reaction path (MEP) on the reduced potential energy surface (RPES) starting with only the reactant. These approaches are based on concepts from the fast marching method (FMM), which expands points outward as a wavefront on a multidimensional grid from the reactant until the product is reached. The MEP is then traced backward to the reactant. Since the number of possible grid points that must be considered grows exponentially with increasing dimensionality of the RPES, interpolation is important for maintaining manageable computational costs. In this work, we use Shepard interpolation, which we have modified to resolve problems in overfitting. In contrast to FMM, which accurately locates the MEP, the new algorithms focus on locating the single rate-limiting transition state and provide only a rough estimate of the MEP. They do this by mapping out the RPES on a coarse grid and then refining a least action path on a finer grid. This is done so that the majority of the interpolation is done on the finer grid, which minimizes the amount of extrapolation inherent in an outward searching algorithm. The first method scans the entire PES before iteratively locating the transition state (TS) for the MEP on the lower bound estimate of the fine PES. The second method explores the coarse grid in a similar manner to FMM and then iteratively locates the rate-limiting TS in the same manner as the first method. Both methods are shown to be capable of rapidly obtaining (in less than 30 constrained optimization cycles) an approximation to the MEP and the rate limiting TS for three example systems: the 4-well potential, the molecule N-hydroxymethyl-methylnitrosaminee (HMMN), and a cluster model of DNA-uracil glycosylase.

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: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.498
Threshold uncertainty score0.230

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 head0.013
GPT teacher head0.325
Teacher spread0.313 · 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

Citations22
Published2010
Admission routes2
Has abstractyes

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