Analytical Time-Dependent Long-Range Corrected Density Functional Tight Binding (TD-LC-DFTB) Gradients in DFTB+: Implementation and Benchmark for Excited-State Geometries and Transition Energies

2021 ◽  
Vol 17 (4) ◽  
pp. 2266-2282
Author(s):  
Monja Sokolov ◽  
Beatrix M. Bold ◽  
Julian J. Kranz ◽  
Sebastian Höfener ◽  
Thomas A. Niehaus ◽  
...  
Keyword(s):  
Excited State ◽  
Long Range ◽  
Density Functional ◽  
Tight Binding ◽  
Time Dependent ◽  
Transition Energies ◽  
Analytical Time

scholarly journals Time-Dependent Long-Range Corrected Density-Functional Tight-Binding Method Combined with the Polarizable Continuum Model

2019 ◽  
Author(s):  
Yoshio Nishimoto
Keyword(s):  
Excited State ◽  
Long Range ◽  
Continuum Model ◽  
Density Functional ◽  
Tight Binding ◽  
Polarizable Continuum Model ◽  
Time Dependent ◽  
Dual Emission ◽  
Tight Binding Method ◽  
Polarizable Continuum

In this study, excited-state free energies and geometries were efficiently evaluated using a linear-response time-dependent long-range corrected density-functional tight-binding method integrated with the polarizable continuum model (TD-LC-DFTB/PCM). Although the LC-DFTB method required the evaluation of the exchange-type term, which was moderately computationally expensive, a single evaluation of the excited-state gradient for a system consisting of more than 1000 atoms in a vacuum was completed within 30 minutes using one CPU core. Benchmark calculations were conducted for 3-hydroxy avone, which exhibits dual emission: the absorption and enol-form emission wavelengths calculated by TD-LC-DFTB/PCM agreed well with those predicted based on density functional theory using a long-range corrected functional; however, there was a large error in the predicted keto-form emission wavelength. Further benchmark calculations for more than 20 molecules indicated that the conventional TD-DFTB method underestimated the absorption and 0-0 transition energies compared with those which were measured experimentally while the TD-LC-DFTB method systematically overestimated these metrics. Nevertheless, the agreement of the results of the TD-LC-DFTB method with those obtained by the CAM-B3LYP method demonstrates the potential of the TD-LC-DFTB/PCM method. Moreover, changing the range-separation parameter to 0.15 minimized this deviation.<br>

scholarly journals Time-Dependent Long-Range Corrected Density-Functional Tight-Binding Method Combined with the Polarizable Continuum Model

2019 ◽  
Author(s):  
Yoshio Nishimoto
Keyword(s):  
Excited State ◽  
Long Range ◽  
Continuum Model ◽  
Density Functional ◽  
Tight Binding ◽  
Polarizable Continuum Model ◽  
Time Dependent ◽  
Dual Emission ◽  
Tight Binding Method ◽  
Polarizable Continuum

In this study, excited-state free energies and geometries were efficiently evaluated using a linear-response time-dependent long-range corrected density-functional tight-binding method integrated with the polarizable continuum model (TD-LC-DFTB/PCM). Although the LC-DFTB method required the evaluation of the exchange-type term, which was moderately computationally expensive, a single evaluation of the excited-state gradient for a system consisting of more than 1000 atoms in a vacuum was completed within 30 minutes using one CPU core. Benchmark calculations were conducted for 3-hydroxy avone, which exhibits dual emission: the absorption and enol-form emission wavelengths calculated by TD-LC-DFTB/PCM agreed well with those predicted based on density functional theory using a long-range corrected functional; however, there was a large error in the predicted keto-form emission wavelength. Further benchmark calculations for more than 20 molecules indicated that the conventional TD-DFTB method underestimated the absorption and 0-0 transition energies compared with those which were measured experimentally while the TD-LC-DFTB method systematically overestimated these metrics. Nevertheless, the agreement of the results of the TD-LC-DFTB method with those obtained by the CAM-B3LYP method demonstrates the potential of the TD-LC-DFTB/PCM method. Moreover, changing the range-separation parameter to 0.15 minimized this deviation.<br>

Time-Dependent Extension of the Long-Range Corrected Density Functional Based Tight-Binding Method

2017 ◽  
Vol 13 (4) ◽  
pp. 1737-1747 ◽  
Author(s):  
Julian J. Kranz ◽  
Marcus Elstner ◽  
Bálint Aradi ◽  
Thomas Frauenheim ◽  
Vitalij Lutsker ◽  
...  
Keyword(s):  
Long Range ◽  
Density Functional ◽  
Tight Binding ◽  
Time Dependent ◽  
Tight Binding Method

scholarly journals Benchmark and performance of long-range corrected time-dependent density functional tight binding (LC-TD-DFTB) on rhodopsins and light-harvesting complexes

2020 ◽  
Vol 22 (19) ◽  
pp. 10500-10518 ◽  
Author(s):  
Beatrix M. Bold ◽  
Monja Sokolov ◽  
Sayan Maity ◽  
Marius Wanko ◽  
Philipp M. Dohmen ◽  
...  
Keyword(s):  
Long Range ◽  
Density Functional ◽  
Light Harvesting ◽  
Tight Binding ◽  
Time Dependent ◽  
Light Harvesting Complexes ◽  
Benchmark Study ◽  
Td Dft ◽  
And Performance ◽  
Dependent Density

In the present work, we perform a benchmark study on both the isolated chromophores retinal and BChl a as well as on the biological systems, to determine the accuracy of LC-TD-DFT and LC-TD-DFTB for describing color-tuning effects.

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