Effects of the locality of a potential derived from hybrid density functionals on Kohn–Sham orbitals and excited states
Bibliographic record
Abstract
Density functional theory (DFT) has been an essential tool for electronic structure calculations in various fields. In particular, its hybrid method including the Hartree-Fock (HF) exchange term remarkably improves the reliability of DFT for chemical applications and computational material design. There are two different types of exchange-correlation potential that can be derived from hybrid functionals. The conventional approach adopts a non-multiplicative potential including the non-local HF exchange operator. Herein, we propose to use a local multiplicative potential as an alternative for accurate excited state calculations. We show that such a local potential can be derived from existing global hybrid functionals using the optimized effective potential method. As a proof-of-concept, we chose PBE0 and investigated its performance for the Caricato benchmark set. Unlike the conventional one, the local potential produced orbital energy gaps with no strong dependence on the mixing ratio as a good approximation for optical excitations. Furthermore, its time-dependent DFT resulted in a surprisingly small mean absolute error even with a local density approximation kernel, surpassing all reported values with various popular functionals. In particular, most excitations were dictated by single orbital transitions due to physically meaningful virtual orbitals, which is beneficial to clear interpretations in the molecular orbital picture.
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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 | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.001 | 0.001 |
| 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".