Multiconfiguration time-dependent Hartree approach for electron-nuclear correlation in strong laser fields

Jhala, Chirag; Lein, Manfred

doi:10.1103/physreva.81.063421

Cited by 16 publications

(17 citation statements)

References 40 publications

(35 reference statements)

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“…For molecules, numerical solutions of the TDSE including the nuclear degrees of freedom have been derived for only one-electron systems [12][13][14]. Alternatively, approximate approaches have been developed such as the method describing electrons by quantum mechanics and nuclei by classical mechanics [15][16][17], the multiconfiguration time-dependent Hartree-Fock method in which both electrons and nuclei are treated quantum mechanically [18][19][20], and the surface-hopping Monte Carlo wave packet method [21].…”

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confidence: 99%

Classical Dynamics of Laser-DrivenD3+

2011

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A classical model of the triatomic D₃⁺ molecule subjected to an intense, few-cycle laser pulse is introduced. The model is capable of describing the laser-induced correlated motion of both electrons and nuclei in three dimensions, and allows us to follow the motion of the two electrons and three deuterons from the initial field-free state, during the pulse, and until the bond breaking into the final fragments. By averaging over many trajectories, we calculate the relative yields of the ionization and dissociation channels, as well as the kinetic energy release (KER) from the fragment ions. A comparison with recent experimental KER spectra shows good qualitative agreement. In addition, we find a pathway in which an emitted electron recombines into a high-lying Rydberg state, resulting in D + D⁺ + D⁺ fragments with the same KER as in the D⁺ + D⁺ + D⁺ channel.

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confidence: 99%

Classical Dynamics of Laser-DrivenD3+

2011

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“…The increasing number of discrete transitions should finally result in a continuous spectrum if enough orbitals are taken into account. For the TDH case N o = 1 this behavior has already been observed [23,26,41]. Using the Hartree approximation, only one sharp peak-corresponding to a transition to a bound state-appears in the spectrum for the first electronic transition.…”

Section: A Ground Statementioning

confidence: 56%

“…We apply TDRNOT to the widely used one-dimensional H + 2 model system [20,23,26,[31][32][33][34]. This collinear model utilizes the fact that the ionization and dissociation dynamics of H + 2 is predominantly constrained to the polarization direction when interacting with a strong, linearly polarized laser field.…”

Section: A Model Systemmentioning

confidence: 99%

“…Especially in the case of fragmentation of molecules in intense laser fields the adiabatic BO approximation may break down as electronic and nuclear energy scales are not well separated at avoided crossings or conical intersections. Several approaches aiming at the description of correlated electron-nuclear dynamics beyond the BO approximation were presented in the last few years, e.g., * Corresponding author: dieter.bauer@uni-rostock.de the exact factorization of the molecular wavefunction [18][19][20], a multiconfigurational time-dependent Hartree (Fock) approach [MCTDH(F)] [21][22][23], or a multicomponent extension of (TD)DFT (MC(TD)DFT) [24][25][26], which, besides the single-particle electron density, also takes the diagonal of the nuclear density matrix into account.…”

Section: Introductionmentioning

confidence: 99%

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Time-dependent renormalized-natural-orbital theory applied to laser-drivenH2+

et al. 2016

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Recently introduced time-dependent renormalized-natural orbital theory (TDRNOT) is extended towards a multi-component approach in order to describe H + 2 beyond the Born-Oppenheimer approximation. Two kinds of natural orbitals, describing the electronic and the nuclear degrees of freedom are introduced, and the exact equations of motion for them are derived. The theory is benchmarked by comparing numerically exact results of the time-dependent Schrödinger equation for a H + 2 model system with the corresponding TDRNOT predictions. Ground state properties, linear response spectra, fragmentation, and high-order harmonic generation are investigated.

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“…In order to understand the mechanism of ultrafast hydrogen migration processes, we formulated the time-dependent multiconfiguration wave-function description of a system composed of two kinds of Fermi particles [13][14][15][16] (i.e., electrons and protons) by extending the theory developed to describe electronic dynamics in an intense laser field [17][18][19][20].…”

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confidence: 99%

Protonic structure of CH3OH described by electroprotonic wave functions

Katō

Yamanouchi

2012

Phys. Rev. A

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The electroprotonic ground-state wave function of CH 3 OH is calculated beyond the Born-Oppenheimer (BO) approximation using multiconfiguration wave-function theory for a system composed of electrons and protons. A CH 3 OH molecule is treated as a quasidiatomic molecule in which orbitals for both electrons and protons are described in a laboratory fixed cylindrical coordinate system with C and O atoms being fixed on the z axis. The probability density of the four protons shows that the C atom is surrounded by three protons and the O atom by one proton, and that the dihedral angle of the O-H bond axis with respect to one of the C-H bond axes becomes 180 • , exhibiting appropriately the conformational correlation between the two functional groups. The optimized spatial configuration of the protons was found to be in good agreement with that obtained by the standard BO-based electronic structure calculation. The non-BO electroprotonic wave functions introduced here afford the basis for describing ultrafast hydrogen migration in hydrocarbon molecules in an intense laser field.

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Multiconfiguration time-dependent Hartree approach for electron-nuclear correlation in strong laser fields

Cited by 16 publications

References 40 publications

Classical Dynamics of Laser-DrivenD3+

Classical Dynamics of Laser-DrivenD3+

Time-dependent renormalized-natural-orbital theory applied to laser-drivenH2+

Protonic structure of CH3OH described by electroprotonic wave functions

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