Quantum Wave-Packet Dynamics in Spin-Coupled Vibronic States

Falge, Mirjam; Engel, Volker; Lein, Manfred; Vindel-Zandbergen, Patricia; Chang, Bong‐Soon; Solá, Ignacio R.

doi:10.1021/jp306566x

Cited by 15 publications

(14 citation statements)

References 41 publications

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“…Recently, there has been a surge of studies that aim to analyze and control electron–nuclear processes − to create novel transient molecular properties in the presence of strong fields, for instance, huge electronic dipoles, − to manipulate nonadiabatic transitions − or to unravel the electron–nuclear dynamical features in conical intersections − particularly at so-called light-induced conical intersections. − Our goal is to design a simple model that can provide qualitative predictions of quantum control in one-active electron systems, treating strong field laser couplings, nonadiabatic couplings, and ionization on equal footing, that can be extended to polyatomic molecules. One possible avenue is to use the multiconfiguration time-dependent Hartree (MCTDH) method, , the ab-initio multiple spawning (AIMS) method, , or other schemes that incorporate quantum features to the nuclear motion. − …”

Section: Introductionmentioning

confidence: 99%

Grid-Based Ehrenfest Model To Study Electron–Nuclear Processes

et al. 2019

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The two-dimensional electron-nuclear Schrödinger equation using soft-core Coulomb potentials has been a cornerstone for modeling and predicting the behavior of one-active-electron diatomic molecules, particularly for processes where both bound and continuum states are important. The model, however, is computationally expensive to extend to more electron or nuclear coordinates.Here we propose to use the Ehrenfest approach to treat the nuclear motion, while the electronic motion is still solved by quantum propagation on a grid. In this work we present results for a one-dimensional treatment of H + 2 , where the quantum and semi-classical dynamics can be directly compared, showing remarkably good agreement for a variety of situations. The advantage of the Ehrenfest approach is that it can be easily extended to treat as many nuclear degrees of freedom as needed. * Electronic address: isola@quim.ucm.es 1 arXiv:1905.13702v1 [physics.chem-ph]

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Section: Introductionmentioning

confidence: 99%

Grid-Based Ehrenfest Model To Study Electron–Nuclear Processes

et al. 2019

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“…where R e scales the electron-electron interaction [34][35][36][37][38][39][40]. The fixed nuclei have a distance of L = 10 Å.…”

Section: A the Full Model Systemmentioning

confidence: 99%

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Fröbel

Ziems

Peschel

et al. 2020

J. Phys. B: At. Mol. Opt. Phys.

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The attosecond ultrafast ionization dynamics of correlated two-or many-electron systems have, so far, been mainly addressed investigating atomic systems. In the case of single ionization, it is well known that electronelectron correlation modifies the ionization dynamics and observables beyond the single active electron picture, resulting in effects such as the Auger effect or shake-up/down and knock-up/down processes. Here, we extend these works by investigating the attosecond ionization of a molecular system involving correlated two-electron dynamics, as well as non-adiabatic nuclear dynamics. Employing a charge-transfer molecular model system with two differently bound electrons, a strongly and a weakly bound electron, we distinguish different pathways leading to ionization, be it direct ionization or ionization involving elastic and inelastic electron scattering processes. We find that different pathways result in a difference in the electronic population of the parent molecular ion, which, in turn, involves different subsequent (non-adiabatic) postionization dynamics on different time scales.

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“…The simple Shin-Metiu model was later extended to include the motion of a second electron, which made it possible to introduce time-dependent electron localisation functions (ELF) and characterise the influence of nuclear motion on these (Erdmann et al, 2004). Also, the wave-packet dynamics in spin-coupled electronic states could be described (Falge et al, 2012b).…”

Section: Introductionmentioning

confidence: 99%

Nuclear–Electron Correlation Effects and Their Photoelectron Imprint in Molecular XUV Ionisation

et al. 2022

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The ionisation of molecules by attosecond XUV pulses is accompanied by complex correlated dynamics, such as the creation of coherent electron wave packets in the parent ion, their interplay with nuclear wave packets, and a correlated photoelectron moving in a multi-centred potential. Additionally, these processes are influenced by the dynamics prior to and during the ionisation. To fully understand and subsequently control the ionisation process on different time scales, a profound understanding of electron and nuclear correlation is needed. Here, we investigate the effect of nuclear–electron correlation in a correlated two-electron and one-nucleus quantum model system. Solving the time-dependent Schrödinger equation allows to monitor the correlation impact pre, during, and post-XUV ionisation. We show how an initial nuclear wave packet displaced from equilibrium influences the post-ionisation dynamics by means of momentum conservation between the target and parent ion, whilst the attosecond electron population remains largely unaffected. We calculate time-resolved photoelectron spectra and their asymmetries and demonstrate how the coupled electron–nuclear dynamics are imprinted on top of electron–electron correlation on the photoelectron properties. Finally, our findings give guidelines towards when correlation resulting effects have to be incorporated and in which instances the exact correlation treatment can be neglected.

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Quantum Wave-Packet Dynamics in Spin-Coupled Vibronic States

Cited by 15 publications

References 41 publications

Grid-Based Ehrenfest Model To Study Electron–Nuclear Processes

Grid-Based Ehrenfest Model To Study Electron–Nuclear Processes

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Nuclear–Electron Correlation Effects and Their Photoelectron Imprint in Molecular XUV Ionisation

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