Probing the π → π* photoisomerization mechanism of trans-azobenzene by multi-state ab initio on-the-fly trajectory dynamics simulations

2018 ◽  
Vol 20 (37) ◽  
pp. 23885-23897 ◽  
Author(s):  
Chao Xu ◽  
Le Yu ◽  
Feng Long Gu ◽  
Chaoyuan Zhu
Keyword(s):  
Ab Initio ◽  
Electronic States ◽  
Quantum Level ◽  
Surface Hopping ◽  
Trajectory Dynamics ◽  
Dynamics Simulations ◽  
Trans Azobenzene

Global nonadiabatic switching on-the-fly trajectory surface hopping simulations at the 5SA-CASSCF(6,6)/6-31G quantum level have been employed to probe the photoisomerization mechanism of trans-azobenzene upon ππ* excitation within four coupled singlet low-lying electronic states (S0, S1, S2, and S3).

Chiral conversion and periodical decay in bridged-azobenzene photoisomerization: an ab initio on-the-fly nonadiabatic dynamics simulation

RSC Advances ◽  
2016 ◽  
Vol 6 (46) ◽  
pp. 39542-39552 ◽  
Author(s):  
Wanqing Gao ◽  
Le Yu ◽  
Xiaolei Zheng ◽  
Yibo Lei ◽  
Chaoyuan Zhu ◽  
...  
Keyword(s):  
Ab Initio ◽  
Dynamics Simulation ◽  
Nonadiabatic Dynamics ◽  
Surface Hopping ◽  
Dynamics Simulations

On-the-fly trajectory surface hopping dynamics simulations on the cis ↔ trans photoisomerization mechanisms of bridged-azobenzene upon S1 excitation at the CASSCF level.

scholarly journals Ab initio molecular dynamics study of solvated electrons in methanol clusters

2018 ◽  
Vol 20 (45) ◽  
pp. 28741-28750 ◽  
Author(s):  
Letif Mones ◽  
Gábor Pohl ◽  
László Turi
Keyword(s):  
Molecular Dynamics ◽  
Ab Initio ◽  
Molecular Dynamics Simulations ◽  
Electronic States ◽  
Ab Initio Molecular Dynamics ◽  
Cluster Anions ◽  
Surface Excess ◽  
Solvated Electrons ◽  
Stable Surface ◽  
Dynamics Simulations

Stable surface excess electronic states in small methanol cluster anions were identified and characterized in ab initio molecular dynamics simulations.

Structural and electronic properties of organo-halide hybrid perovskites from ab initio molecular dynamics

2015 ◽  
Vol 17 (14) ◽  
pp. 9394-9409 ◽  
Author(s):  
Claudio Quarti ◽  
Edoardo Mosconi ◽  
Filippo De Angelis
Keyword(s):  
Molecular Dynamics ◽  
Ab Initio ◽  
Molecular Dynamics Simulations ◽  
Electronic Properties ◽  
Electronic States ◽  
Ab Initio Molecular Dynamics ◽  
Structural Flexibility ◽  
Structural And Electronic Properties ◽  
Dynamics Simulations

Ab initio molecular dynamics simulations of MAPbI3 and FAPbI3 perovskites demonstrate their structural flexibility and a cation-induced sub-ps localization of electronic states.

Active Learning Accelerates Ab Initio Molecular Dynamics on Pericyclic Reactive Energy Surfaces

2020 ◽  
Author(s):  
Shi Jun Ang ◽  
Wujie Wang ◽  
Daniel Schwalbe-Koda ◽  
Simon Axelrod ◽  
Rafael Gomez-Bombarelli
Keyword(s):  
Molecular Dynamics ◽  
Potential Energy ◽  
Transition State ◽  
Potential Energy Surface ◽  
Ab Initio ◽  
Energy Surface ◽  
Computational Cost ◽  
Reactive Trajectories ◽  
Dynamics Simulations ◽  
Energy Surfaces

<div>Modeling dynamical effects in chemical reactions, such as post-transition state bifurcation, requires <i>ab initio</i> molecular dynamics simulations due to the breakdown of simpler static models like transition state theory. However, these simulations tend to be restricted to lower-accuracy electronic structure methods and scarce sampling because of their high computational cost. Here, we report the use of statistical learning to accelerate reactive molecular dynamics simulations by combining high-throughput ab initio calculations, graph-convolution interatomic potentials and active learning. This pipeline was demonstrated on an ambimodal trispericyclic reaction involving 8,8-dicyanoheptafulvene and 6,6-dimethylfulvene. With a dataset size of approximately</div><div>31,000 M062X/def2-SVP quantum mechanical calculations, the computational cost of exploring the reactive potential energy surface was reduced by an order of magnitude. Thousands of virtually costless picosecond-long reactive trajectories suggest that post-transition state bifurcation plays a minor role for the reaction in vacuum. Furthermore, a transfer-learning strategy effectively upgraded the potential energy surface to higher</div><div>levels of theory ((SMD-)M06-2X/def2-TZVPD in vacuum and three other solvents, as well as the more accurate DLPNO-DSD-PBEP86 D3BJ/def2-TZVPD) using about 10% additional calculations for each surface. Since the larger basis set and the dynamic correlation capture intramolecular non-covalent interactions more accurately, they uncover longer lifetimes for the charge-separated intermediate on the more accurate potential energy surfaces. The character of the intermediate switches from entropic to thermodynamic upon including implicit solvation effects, with lifetimes increasing with solvent polarity. Analysis of 2,000 reactive trajectories on the chloroform PES shows a qualitative agreement with the experimentally-reported periselectivity for this reaction. This overall approach is broadly applicable and opens a door to the study of dynamical effects in larger, previously-intractable reactive systems.</div>

scholarly journals Proton Transport Mechanism and Pathways in the Superprotonic Phase of M3H(AO4)2 Solid Acids from Ab Initio Molecular Dynamics Simulations

2021 ◽  
Author(s):  
Boris Merinov ◽  
Sergey Morozov
Keyword(s):  
Molecular Dynamics ◽  
Ab Initio ◽  
Proton Transport ◽  
Transport Mechanism ◽  
Solid Acids ◽  
Ab Initio Molecular Dynamics ◽  
Theoretical Studies ◽  
Dynamics Simulations ◽  
Experimental And Theoretical Studies ◽  
Superprotonic Phase

The proton transport mechanism in superprotonic phases of solid acids is a subject of experimental and theoretical studies for a number of years. Despite this, details of the mechanism still...

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