Modeling ultrafast exciton deactivation in oligothiophenes via nonadiabatic dynamics

2015 ◽  
Vol 17 (12) ◽  
pp. 7787-7799 ◽  
Author(s):  
Daniele Fazzi ◽  
Mario Barbatti ◽  
Walter Thiel
Keyword(s):  
Excited State ◽  
Relaxation Processes ◽  
Nonadiabatic Dynamics ◽  
Torsional Oscillations ◽  
Excited State Dynamics ◽  
Exciton Localization ◽  
Bond Stretching ◽  
Ring Puckering

Nonadiabatic excited-state dynamics reveal the exciton relaxation processes in oligothiophenes. Ultrafast deactivation and exciton localization are predicted to occur within 200 fs, involving bond stretching, ring puckering, and torsional oscillations.

scholarly journals Methods to Calculate Electronic Excited-state Dynamics For Molecules on Large Metal Clusters with Many States: Ensuring Fast Overlap Calculations and a Robust Choice of Phase

2021 ◽  
Author(s):  
Hsing-Ta Chen ◽  
Junhan Chen ◽  
Vale Cofer-Shabica ◽  
Zeyu Zhou ◽  
Vishikh Athavale ◽  
...  
Keyword(s):  
Excited State ◽  
Collective Excitation ◽  
Metal Cluster ◽  
Computational Cost ◽  
Electronic States ◽  
Relaxation Processes ◽  
Nuclear Dynamics ◽  
Excited State Dynamics ◽  
Electronic Excited State ◽  
Unified Protocol

We present an efficient set of methods for propagating excited-state dynamics involving a large number of electronic states based on a CIS electronic state overlap scheme. Specifically, (i) following Head-Gordon et al, we implement an exact evaluation of the overlap of singly-excited electronic states at different nuclear geometries using a biorthogonal basis, and (ii) we employ a unified protocol for choosing the correct phase for each adiabat at each geometry. For many-electron systems, the combination of these techniques significantly reduces the computational cost of integrating the electronic Schrodinger equation and imposes minimal overhead on top of the underlying electronic structure calculation. As a demonstration, we calculate the electronic excited-state dynamics for a hydrogen molecule scattering off a silver metal cluster, focusing on high-lying excited states where many electrons can be excited collectively and crossings are plentiful. Interestingly, we find that the high-lying, plasmon-like collective excitation spectrum changes with nuclear dynamics, highlighting the need to simulate non-adiabatic nuclear dynamics and plasmonic excitations simultaneously. In the future, the combination of methods presented here should help theorists build a mechanistic understanding of plasmon-assisted charge transfer and excitation energy relaxation processes near a nanoparticle or metal surface.

scholarly journals Photoinduced electron-driven proton transfer from water to an N-heterocyclic chromophore: nonadiabatic dynamics studies for pyridine–water clusters

2019 ◽  
Vol 21 (26) ◽  
pp. 14073-14079 ◽  
Author(s):  
Xiaojuan Pang ◽  
Chenwei Jiang ◽  
Weiwei Xie ◽  
Wolfgang Domcke
Keyword(s):  
Excited State ◽  
Proton Transfer ◽  
Gas Phase ◽  
Water Splitting ◽  
Water Clusters ◽  
Water Molecules ◽  
Nonadiabatic Dynamics ◽  
Excited State Dynamics ◽  
Dynamics Simulations

We performed the excited-state dynamics simulations for pyridine–water clusters and found the more water molecules involved in the cluster, the higher efficiency the water-splitting reaction has, which is qualitatively in consistent with a recent gas-phase experimental observations.

scholarly journals Exciton localization in excited-state dynamics of a tetracene trimer: a surface hopping LC-TDDFTB study

2018 ◽  
Vol 20 (40) ◽  
pp. 25995-26007 ◽  
Author(s):  
Evgenii Titov ◽  
Alexander Humeniuk ◽  
Roland Mitrić
Keyword(s):  
Excited State ◽  
Long Range ◽  
Surface Hopping ◽  
Excited State Dynamics ◽  
Exciton Localization

Ultrafast exciton localization in a tetracene trimer is revealed with long-range corrected DFTB surface hopping simulations.

scholarly journals Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au3−[H2O]n (n = 0–2)

2016 ◽  
Vol 18 (9) ◽  
pp. 6411-6419 ◽  
Author(s):  
Polina G. Lisinetskaya ◽  
Christian Braun ◽  
Sebastian Proch ◽  
Young Dok Kim ◽  
Gerd Ganteför ◽  
...  
Keyword(s):  
Experimental Study ◽  
Excited State ◽  
Gold Clusters ◽  
Nonadiabatic Dynamics ◽  
Excited State Dynamics

We present a joint theoretical and experimental study of excited state dynamics in pure and hydrated anionic gold clusters Au3−[H2O]n (n = 0–2).

Excited-State Dynamics in the RNA Nucleotide Uridine 5’-Monophosphate Investigated by Femtosecond Broadband Transient Absorption Spectroscopy

2019 ◽  
Author(s):  
Matthew M. Brister ◽  
Carlos Crespo-Hernández
Keyword(s):  
Excited State ◽  
Excited States ◽  
Ground State ◽  
Transient Absorption ◽  
Electronic Energy ◽  
Transient Absorption Spectroscopy ◽  
Electronic Relaxation ◽  
Vibrationally Excited ◽  
Excited State Dynamics ◽  
Π State

<p></p><p> Damage to RNA from ultraviolet radiation induce chemical modifications to the nucleobases. Unraveling the excited states involved in these reactions is essential, but investigations aimed at understanding the electronic-energy relaxation pathways of the RNA nucleotide uridine 5’-monophosphate (UMP) have not received enough attention. In this Letter, the excited-state dynamics of UMP is investigated in aqueous solution. Excitation at 267 nm results in a trifurcation event that leads to the simultaneous population of the vibrationally-excited ground state, a longlived <sup>1</sup>n<sub>O</sub>π* state, and a receiver triplet state within 200 fs. The receiver state internally convert to the long-lived <sup>3</sup>ππ* state in an ultrafast time scale. The results elucidate the electronic relaxation pathways and clarify earlier transient absorption experiments performed for uracil derivatives in solution. This mechanistic information is important because long-lived nπ* and ππ* excited states of both singlet and triplet multiplicities are thought to lead to the formation of harmful photoproducts.</p><p></p>

Modulation of Excited State Dynamics in Lead Halide Perovskite Films with Electrical Bias

2019 ◽  
Author(s):  
Gergely Samu ◽  
R.A. Scheidt ◽  
A. Balog ◽  
C. Janáky ◽  
P.V. Kamat
Keyword(s):  
Excited State ◽  
Excited State Dynamics ◽  
Halide Perovskite ◽  
Electrical Bias ◽  
Lead Halide
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