التفاصيل البيبلوغرافية
| العنوان: |
Full Implementation, Optimization, and Evaluation of a Range-Separated Local Hybrid Functional with Wide Accuracy for Ground and Excited States |
| المؤلفون: |
Susanne Fürst (14374014), Matthias Haasler (9254263), Robin Grotjahn (4458394), Martin Kaupp (1265817) |
| سنة النشر: |
2023 |
| مصطلحات موضوعية: |
Biophysics, Medicine, Evolutionary Biology, Sociology, Space Science, Biological Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, turbomole program package, separated hybrids available, reoptimized b95c correlation, provides good balance, pig2 calibration function, d4 dispersion corrections, best local hybrids, basis set size, 2 – 3, ωlh22t performs excellently, rydberg excitation energies, range hf exchange, excitation energies, atomization energies, wide range, valence systems, valence singlet, transfer excitations, top rung, successful range, reaction barriers, range pbe |
| الوصف: |
We report the first full and efficient implementation of range-separated local hybrid functionals (RSLHs) into the TURBOMOLE program package. This enables the computation of ground-state energies and nuclear gradients as well as excitation energies. Regarding the computational effort, RSLHs scale like regular local hybrid functionals (LHs) with system or basis set size and increase timings by a factor of 2–3 in total. An advanced RSLH, ωLH22t, has been optimized for atomization energies and reaction barriers. It is an extension of the recent LH20t local hybrid and is based on short-range PBE and long-range HF exchange-energy densities, a pig2 calibration function to deal with the gauge ambiguity of exchange-energy densities, and reoptimized B95c correlation. ωLH22t has been evaluated for a wide range of ground-state and excited-state quantities. It further improves upon the already successful LH20t functional for the GMTKN55 main-group energetics test suite, and it outperforms any global hybrid while performing close to the top rung-4 functional, ωB97M-V, for these evaluations when augmented by D4 dispersion corrections. ωLH22t performs excellently for transition-metal reactivity and provides good balance between delocalization errors and left–right correlation for mixed-valence systems, with a somewhat larger bias toward localized states compared to LH20t. It approaches the accuracy of the best local hybrids to date for core, valence singlet and triplet, and Rydberg excitation energies while improving strikingly on intra- and intermolecular charge-transfer excitations, comparable to the most successful range-separated hybrids available. |
| نوع الوثيقة: |
article in journal/newspaper |
| اللغة: |
unknown |
| العلاقة: |
https://figshare.com/articles/journal_contribution/Full_Implementation_Optimization_and_Evaluation_of_a_Range-Separated_Local_Hybrid_Functional_with_Wide_Accuracy_for_Ground_and_Excited_States/21859905Test |
| DOI: |
10.1021/acs.jctc.2c00782.s001 |
| الإتاحة: |
https://doi.org/10.1021/acs.jctc.2c00782.s001Test |
| حقوق: |
CC BY-NC 4.0 |
| رقم الانضمام: |
edsbas.2173A426 |
| قاعدة البيانات: |
BASE |
