Correlated multielectron systems in strong laser fields: A multiconfiguration time-dependent Hartree-Fock approach

Caillat, Jérémie; Zanghellini, Jürgen; Kitzler, Markus; Koch, Othmar; Kreuzer, W.; Scrinzi, Armin

doi:10.1103/physreva.71.012712

Cited by 311 publications

(302 citation statements)

References 47 publications

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“…The opportunity to explain and predict novel effects motivates computational approaches, which face the challenge of vast complexity [2,3]. Variational multimode dynamics seeks to reduce the computational complexity by expanding the wave function with a small number M of optimized mode functions [4][5][6][7]. Specifically adapted for bosonic particles is the multiconfigurational timedependent Hartree method for bosons (MCTDHB) [8].…”

Section: Introductionmentioning

confidence: 99%

Center-of-mass motion as a sensitive convergence test for variational multimode quantum dynamics

2016

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Publisher's copyright statement:Reprinted with permission from the American Physical Society: Physical Review A 94, 043603 c (2016) by the American Physical Society. Readers may view, browse, and/or download material for temporary copying purposes only, provided these uses are for noncommercial personal purposes. Except as provided by law, this material may not be further reproduced, distributed, transmitted, modi ed, adapted, performed, displayed, published, or sold in whole or part, without prior written permission from the American Physical Society.Additional information: Use policyThe full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-pro t purposes provided that:• a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders.Please consult the full DRO policy for further details. Multimode expansions in computational quantum dynamics promise convergence toward exact results upon increasing the number of modes. Convergence is difficult to ascertain in practice due to the unfavorable scaling of required resources for many-particle problems and therefore a simplified criterion based on a threshold value for the least occupied mode function is often used. Here we show how the separable quantum motion of the center of mass can be used to sensitively detect unconverged numerical multiparticle dynamics in harmonic potentials. Based on an experimentally relevant example of attractively interacting bosons in one dimension, we demonstrate that the simplified convergence criterion fails to assure qualitatively correct results. Furthermore, the numerical evidence for the creation of two-hump fragmented bright soliton-like states presented by A. I. Streltsov et al. [Phys. Rev. Lett. 100, 130401 (2008)] is shown to be inconsistent with exact results. Implications for understanding dynamical fragmentation in attractive boson systems are briefly discussed.

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Section: Introductionmentioning

confidence: 99%

Center-of-mass motion as a sensitive convergence test for variational multimode quantum dynamics

2016

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“…(23) and (24) have timedependent coefficients h jk , u jklm , and Γ jk which must be computed along the flow. This is a non-trivial task in general, and techniques common for Ψ-MCTDH can be employed to deal with this in approximate ways [8,17].…”

Section: Discussionmentioning

confidence: 99%

“…That is, the Hamiltonian H is mapped to H −iΓ, where Γ ≥ 0 is a local one-body potential vanishing on the domain of interest, and only taking nonzero values outside the domain. This approach is also used in order to calculate properties like reaction and ionization probabilities, and CAPs are routinely implemented in MCTDH codes [4,8,[15][16][17]. * Electronic address: simen.kvaal@cma.uio.no…”

Section: Introductionmentioning

confidence: 99%

“…With MCTDH for identical particles the exponential scaling of the Hilbert space dimension with respect to N is "postponed" to higher number of particles, and the N = 2 propagation can be done on a single desktop computer. Current implementations can handle N ≤ 8 electrons in cylindrical geometries reliably [8,9]. For bosons, the Pauli exclusion principle is absent, and MCTDH can treat hundreds [10] and even thousands of particles [11] in one-dimensional geometries, and recent multi-layer MCTDH techniques allow distinguishable dimensions in the thousands with relative ease [7], showing great promise of extending the domain of application of MCTDH methods.…”

Section: Introductionmentioning

confidence: 99%

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Multiconfigurational time-dependent Hartree method to describe particle loss due to absorbing boundary conditions

Kvaal

2011

Phys. Rev. A

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Absorbing boundary conditions in the form of a complex absorbing potential are routinely introduced in the Schrödinger equation to limit the computational domain or to study reactive scattering events using the multi-configurational time-dependent Hartree method (MCTDH). However, it is known that a pure wavefunction description does not allow the modeling and propagation of the remnants of a system of which some parts are removed by the absorbing boundary. It was recently shown [S. Selstø and S. Kvaal, J. Phys. B: At. Mol. Opt. Phys. 43 (2010), 065004] that a master equation of Lindblad form was necessary for such a description. We formulate a multiconfigurational time-dependent Hartree method for this master equation, usable for any quantum system composed of any mixture of species. The formulation is a strict generalization of pure-state propagation using standard MCTDH. We demonstrate the formulation with a numerical experiment.

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“…The multiconfiguration time-dependent Hartree-Fock (MCTDHF) algorithm [24][25][26][27][28][29][30][31][32] is an adaptive method for calculating nonpertubative electronic dynamics in molecules. In a recently described numerical implementation [33,34] that we use here, all electrons are active, all orbitals are time-dependent, and any number of them may be ionized.…”

Section: Methodsmentioning

confidence: 99%

Ultrafast population transfer to excited valence levels of a molecule driven by x-ray pulses

Haxton

McCurdy

2014

Phys. Rev. A

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First-principles quantum mechanical calculations of an intense-field ultrafast two-color core hole stimulated Raman process in nitric oxide are presented. They employ the Multiconfiguration TimeDependent Hartree-Fock (MCTDHF) method with all 15 electrons active. These calculations demonstrate a robust excitation localized on an atom through a core-electron stimulated Raman transition, the first step in proposed stimulated X-ray Raman spectroscopy experiments. A total population transfer of approximately 41% into valence excited states and 30% ionization is obtained via two concurrent 1.31fs pulses of maximum intensity 0.5 and 3 ×10 17 W cm −2 . It is found that both resonant and nonresonant (via the continuum) Raman transitions contribute. All aspects of these calculations except for AC stark shifts are converged with a modest basis of 11 orbitals, demonstrating the efficiency of MCTDHF for the treatment of nonperturbative electronic dynamics in molecules.

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Correlated multielectron systems in strong laser fields: A multiconfiguration time-dependent Hartree-Fock approach

Cited by 311 publications

References 47 publications

Center-of-mass motion as a sensitive convergence test for variational multimode quantum dynamics

Center-of-mass motion as a sensitive convergence test for variational multimode quantum dynamics

Multiconfigurational time-dependent Hartree method to describe particle loss due to absorbing boundary conditions

Ultrafast population transfer to excited valence levels of a molecule driven by x-ray pulses

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