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Diagonal perturbative triple corrections to the general‐model‐space state‐universal coupled‐cluster method: Are they warranted and useful?

2006· article· en· W2149821388 on OpenAlex

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A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.

Bibliographic record

VenueMolecular Physics · 2006
Typearticle
Languageen
FieldPhysics and Astronomy
TopicAdvanced Chemical Physics Studies
Canadian institutionsUniversity of Waterloo
Fundersnot available
KeywordsCoupled clusterHamiltonian (control theory)Excited stateDiagonalExcitationPhysicsSpace (punctuation)Quantum mechanicsAtomic physicsMoleculeMathematicsGeometryComputer science

Abstract

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The recently developed general‐model‐space (GMS) state‐universal (SU) coupled‐cluster (CC) approach, together with its version corrected for triples via a single‐reference (SR) CCSD(T)‐type correction of the diagonal elements of the effective Hamiltonian, is applied to several molecular electronic structure problems in order to assess their performance and the role of triples. These results are compared with an alternative handling of higher‐than‐pair clusters via the externally corrected SU CCSD method, denoted (M,N)‐CCSD, which employs N wave functions of the M‐reference CISD as an external source for N‐reference SU CCSD. These methods are applied to the problem of bond breaking in the ground and excited states of the F2 and HF molecules, where the high‐spin triplet component is also handled via the SR CCSD method. We further examine the vertical excitation energies of water and the basic spectroscopic constants (equilibrium geometries, harmonic frequencies, and excitation energies) for several low‐lying states of oxygen. The results are encouraging and are discussed from the viewpoint of the applicability and usefulness of perturbative‐type triple corrections.

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.

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: none
Teacher disagreement score0.771
Threshold uncertainty score0.908

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 head0.008
GPT teacher head0.249
Teacher spread0.241 · 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