On the accuracy and efficiency of different methods to calculate Raman vibrational shifts of parahydrogen clusters
Bibliographic record
Abstract
The Raman vibrational frequency shifts of pure parahydrogen and orthodeuterium clusters of sizes N = 4-9 are calculated using the Langevin equation path integral ground state method. The shifts are calculated using three different methods; the results obtained from each are compared to experiment and variance properties are assessed. The first method requires the direct calculation of energies from two simulations: one when the cluster is in the v = 0 vibrational state and one when the cluster has v = 1 total quantum of vibration. The shift is directly calculated from the difference in those two energies. The second method requires only a v = 0 simulation to be performed. The ground state energy is calculated as usual and the excited state energy is calculated by using the distribution of the v = 0 simulation and the ratio of the density matrices between the v = 1 state and the v = 0 state. The shift is calculated from the difference in those two energies. These first two are both exact methods. The final method is based on perturbation theory where the shift is calculated by averaging the pairwise difference potential over the pair distribution function. However, this is an approximate approach. It is found that for large enough system sizes, despite the approximations, the perturbation theory method has the strongest balance between accuracy and precision when weighing against computational cost.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot 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.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.001 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
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".