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Awasthi, Manohar; Sáenz, Alejandro

doi:10.1103/physreva.81.063406

Cited by 14 publications

(9 citation statements)

References 44 publications

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“…In the above theoretical approaches, only one atomic or molecular orbital is considered as the main ionizing orbital and is allowed to interact with the applied field [61][62][63]. This is the so-called single active electron (SAE) approximation, where the time-dependent (TD) Schrödinger equation to be solved for the least-bound one-electron is constructed by modelling an "effective potential" after the interaction with the remaining electrons, the nuclei, and the applied fields.…”

Section: Introductionmentioning

confidence: 99%

Manipulation of Multielectron Dynamics of Molecules by Fourier-Synthesized Intense Laser Pulses: Effective Potential Analysis of CO

Ohmura

Katō

et al. 2021

Front. Phys.

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We present a theoretical investigation as to how multielectron dynamics of CO are manipulated by Fourier-synthesized intense laser pulses. The pulses used are assumed to be comprised of harmonics up to the fourth order. The multiconfiguration time-dependent (TD) Hartree-Fock (MCTDHF) method, where the multielectron wavefunction Ψ(t) is expressed as a linear combination of various electron configurations, is employed to simulate the dynamics of CO interacting with Fourier-synthesized pulses. The multielectron nature such as electron correlation is quantified by using our effective potential approach. To begin with, the time-dependent natural orbitals {ϕj(r,t)} which diagonalize the first order reduced density matrix are obtained from Ψ(t), where r is the one-electron coordinate. The effective potentials υjeff(r,t) that determine the dynamics of ϕj(r,t) are then derived from the equations of motion for {ϕj(r,t)}. υjeff(r,t) consists of the one-body part υ1(t) including the interaction with the laser electric field ε(t) and the two-body part υ2,j(t) originating from electron-electron interaction. In this way, the role of electron correlation can be quantified by comparing υjeff(r,t) with those obtained by the TDHF method, where Ψ(t) is approximated by a single Slater determinant. We found a very similar profile in υ5σeff(r,t) of the 5σ highest occupied molecular orbital for both near-infrared one-color (ω) and directionally asymmetric ω+2ω two-color pulses; when ε(t) points from the nucleus C to O, a hump appears in υ5σeff(r,t) only 2 bohrs outward from C. The hump formation, which originates from the field-induced change in υ2,5σ(t) (especially, due to electron correlation), is responsible for preferential electron ejection from the C atom side (experimentally observed anisotropic ionization). A coherent superposition of ω and 2ω fields with an appropriate relative phase thus works as a one-color pulse of which either positive or negative peaks are filtered out. More sophisticated manipulation is possible by adding higher harmonics to a synthesized field. We show that the 5σ orbital can be squeezed toward the inside of the potential valley in υ5σeff(r,t), which encloses the molecule at a radius of ∼7 bohrs (semicircle in the region of z <0), by adjusting the phases of a ω+2ω+3ω+4ω field. The hump and valley formation in υ5σeff(r,t) are closely correlated with domains of increasing and decreasing electron density, respectively.

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Section: Introductionmentioning

confidence: 99%

Manipulation of Multielectron Dynamics of Molecules by Fourier-Synthesized Intense Laser Pulses: Effective Potential Analysis of CO

Ohmura

Katō

et al. 2021

Front. Phys.

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“…no electron correlated dynamics occurs. However, it has been shown by Awasthi et al that electron correlation even upon XUV-or X-ray-induced ionization of multi-electron systems plays an important role and cannot be neglected [29,30].…”

Section: Introductionmentioning

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 topic molecular hydrogen in strong laser fields has received continued attention in theory [6][7][8][9][10][11][12] and experiment [13][14][15][16][17][18][19][20][21]. A preponderance of short-pulse experiments on H 2 have been conducted at wavelengths near 800 nm, many concentrating on the question of Coulomb explosion, double ionization, and molecular alignment.…”

Section: Introductionmentioning

confidence: 99%

Nonponderomotive effects in multiphoton ionization of molecular hydrogen

Wilbois

Helm

2011

Phys. Rev. A

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Breakdown of the single-active-electron approximation for one-photon ionization of theB1Σu+

Cited by 14 publications

References 44 publications

Manipulation of Multielectron Dynamics of Molecules by Fourier-Synthesized Intense Laser Pulses: Effective Potential Analysis of CO

Manipulation of Multielectron Dynamics of Molecules by Fourier-Synthesized Intense Laser Pulses: Effective Potential Analysis of CO

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

Nonponderomotive effects in multiphoton ionization of molecular hydrogen

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