scholarly journals Photoinduced charge-transfer in chromophore-labeled gold nanoclusters: quantum evidence of the critical role of ligands and vibronic couplings

Nanoscale ◽  
2021 ◽  
Vol 13 (14) ◽  
pp. 6786-6797
Author(s):  
Adrian Domínguez-Castro ◽  
Carlos R. Lien-Medrano ◽  
Khaoula Maghrebi ◽  
Sabri Messaoudi ◽  
Thomas Frauenheim ◽  
...  
Keyword(s):  
Density Functional ◽  
Critical Role ◽  
Gold Nanoclusters ◽  
Tight Binding ◽  
Time Dependent ◽  
Tight Binding Method ◽  
Photo Induced Electron Transfer ◽  
Vibronic Couplings ◽  
Photoinduced Charge

We present the first application of the time-dependent density functional tight-binding method to rationalize the photo-induced electron transfer in an experimental hexyl-protected Au25 cluster labeled with a pyrene fluorophore.

Impact of vibronic coupling effects on light-driven charge transfer in pyrene-functionalized middle and large-sized Metalloid Gold Nanoclusters from Ehrenfest dynamics.

2021 ◽  
Author(s):  
Adrian Dominguez-Castro ◽  
Thomas Frauenheim
Keyword(s):  
Molecular Dynamics ◽  
Charge Transfer ◽  
Density Functional ◽  
Theoretical Calculations ◽  
Gold Nanoclusters ◽  
Tight Binding ◽  
Time Dependent ◽  
Effective Strategy ◽  
Dynamics Simulations ◽  
Dependent Density

Theoretical calculations are an effective strategy to comple- ment and understand experimental results in atomistic detail. Ehrenfest molecular dynamics simulations based on the real-time time-dependent density functional tight-binding (RT-TDDFTB) approach...

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
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