Influence of the Excitation Wavelength on First Order Hyperpolarizabilities and Optimal Gap Tuning of Range Separated Hybrid Functionals
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Bibliographic record
Abstract
In this study, we compute the hyperpolarizability of the nitroaniline isomers, para-nitroaniline (pNA), ortho-nitroaniline (oNA), and meta-nitroaniline (mNA), by density functional theory (DFT), including with optimally tuned range separated hybrid (RSH) functionals. By utilizing the nitroanilines hyperpolarizability trend based on charge transfer (pNA>oNA>mNA), we can uncover how the excitation wavelength affects the prediction of the hyperpolarizabilities in both on and off resonant regimes, and optimal gap tuning of RSH functionals. In non-resonant regions, with reference to CCSD/aug-cc-pVDZ and experimental studies, we find that some computational approaches do not always reproduce the nitroanilines trend at specific excitation wavelengths. For example, RSH functionals require optimal gap tuning to reproduce the trend. In resonant regions, we find that the damped response theory predicts that the trend is maintained at the two-photon absorption, however, it breaks near the one photon pole. This suggests that the underlying charge transfer characteristics are undermined in the one-photon pole which in comparison to the two-state model suggests that this is due to the presence of other electronic states in some of the isomers. Furthermore, we find that cases where optimal gap tuning is ineffective (pathological behavior) are dependent on the excitation wavelength.
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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 | 0.001 |
| 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 | 0.001 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.001 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 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 it