Nuclear dynamics of several decaying overlapping electronic states: A time‐dependent formulation

1993 ◽  
Vol 99 (8) ◽  
pp. 5871-5884 ◽  
Author(s):  
L. S. Cederbaum ◽  
F. Tarantelli
Keyword(s):  
Electronic States ◽  
Time Dependent ◽  
Nuclear Dynamics

scholarly journals Control of nuclear dynamics in the benzene cation by electronic wavepacket composition

2021 ◽  
Vol 4 (1) ◽  
Author(s):  
Thierry Tran ◽  
Graham A. Worth ◽  
Michael A. Robb
Keyword(s):  
Extreme Ultraviolet ◽  
Initial Conditions ◽  
Chemical Reactivity ◽  
Electronic States ◽  
Time Dependent ◽  
Electronic Control ◽  
Electron Dynamics ◽  
Nuclear Dynamics ◽  
Successive Passage ◽  
Dynamics Simulations

AbstractThe study of coupled electron-nuclear dynamics driven by coherent superpositions of electronic states is now possible in attosecond science experiments. The objective is to understand the electronic control of chemical reactivity. In this work we report coherent 8-state non-adiabatic electron-nuclear dynamics simulations of the benzene radical cation. The computations were inspired by the extreme ultraviolet (XUV) experimental results in which all 8 electronic states were prepared with significant population. Our objective was to study the nuclear dynamics using various bespoke coherent electronic state superpositions as initial conditions in the Quantum-Ehrenfest method. The original XUV measurements were supported by Multi-configuration time-dependent Hartree (MCTDH) simulations, which suggested a model of successive passage through conical intersections. The present computations support a complementary model where non-adiabatic events are seen far from a conical intersection and are controlled by electron dynamics involving non-adjacent adiabatic states. It proves to be possible to identify two superpositions that can be linked with two possible fragmentation paths.

Introduction

2018 ◽  
Author(s):  
Niels Engholm Henriksen ◽  
Flemming Yssing Hansen
Keyword(s):  
Schrödinger Equation ◽  
Schrodinger Equation ◽  
Degrees Of Freedom ◽  
State Level ◽  
Boltzmann Distribution ◽  
Theoretical Description ◽  
Time Dependent ◽  
Nuclear Dynamics ◽  
Molecular Reaction ◽  
Oppenheimer Approximation

This introductory chapter considers first the relation between molecular reaction dynamics and the major branches of physical chemistry. The concept of elementary chemical reactions at the quantized state-to-state level is discussed. The theoretical description of these reactions based on the time-dependent Schrödinger equation and the Born–Oppenheimer approximation is introduced and the resulting time-dependent Schrödinger equation describing the nuclear dynamics is discussed. The chapter concludes with a brief discussion of matter at thermal equilibrium, focusing at the Boltzmann distribution. Thus, the Boltzmann distribution for vibrational, rotational, and translational degrees of freedom is discussed and illustrated.

Nuclear dynamics of decaying states: A time‐dependent formulation

1993 ◽  
Vol 98 (12) ◽  
pp. 9691-9706 ◽  
Author(s):  
L. S. Cederbaum ◽  
F. Tarantelli
Keyword(s):  
Time Dependent ◽  
Nuclear Dynamics ◽  
Decaying States

DFT and TD-DFT calculations of axially substituted tin porphyrins and an ethynyl-linked tin porphyrin dimer

2015 ◽  
Vol 19 (04) ◽  
pp. 610-621 ◽  
Author(s):  
Neha Agnihotri ◽  
Ronald P. Steer
Keyword(s):  
Density Functional ◽  
Electronic States ◽  
Density Functional Theory Calculations ◽  
Time Dependent ◽  
Functional Theory ◽  
Covalently Bonded ◽  
Td Dft ◽  
Satisfactory Analysis ◽  
Tin Porphyrin ◽  
Porphyrin Dimer

Time-dependent density functional theory calculations have been employed to characterize the inter-macrocycle interactions introduced when two tin(IV) porphyrins are axially covalently bonded via an ethynyl linker. The effect of changing the relative orientations of the two metalloporphyrin macrocycles is explored, with particular attention given to electronic states at energies up to the Soret-correlated states in the dimer. Expansion of the Gouterman four orbital approach for the monomer to an eight orbital approach in the dimer produces a satisfactory analysis. The results are used to examine the feasibility of using such linked structures in photon harvesting schemes.

scholarly journals The Density Matrix via Few Dominant Observables: The Quantum Interference in the Isotope Effect for Atto-Pumped N2

2021 ◽  
Author(s):  
Ksenia Komarova ◽  
Francoise Remacle ◽  
Raphael D. Levine
Keyword(s):  
Density Matrix ◽  
Time Evolution ◽  
Isotope Effect ◽  
Lagrange Multipliers ◽  
Quantum Interference ◽  
Electronic States ◽  
Compact Representation ◽  
Nuclear Dynamics ◽  
Analytical Results

In our paper a compact representation of the density as a function of a few observables is examined for the coupled electron-nuclear dynamics unfolding on three electronic states. The time-evolution of the density, populations and coherences, is accurately captured by the time-evolution of only nine coefficients, the Lagrange multipliers of these observables. We use a specific example of the isotope effect in atto-pumped N<sub>2</sub> to show that both classical and quantal effects of mass are well reproduced by this compact description. Simple analytical results for the surprisal are given, which allows a factorization of these two effects.

Regarding the validity of the time-dependent Kohn–Sham approach for electron-nuclear dynamics via trajectory surface hopping

2011 ◽  
Vol 134 (2) ◽  
pp. 024102 ◽  
Author(s):  
Sean A. Fischer ◽  
Bradley F. Habenicht ◽  
Angeline B. Madrid ◽  
Walter R. Duncan ◽  
Oleg V. Prezhdo
Keyword(s):  
Time Dependent ◽  
Nuclear Dynamics ◽  
Surface Hopping
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