Accurate high-harmonic spectra from time-dependent two-particle reduced density matrix theory

Abstract

The accurate description of the non-linear response of many-electron systems to strong-laser fields remains a major challenge. Methods that bypass the unfavorable exponential scaling with particle number are required to address larger systems. In this paper we present a fully three-dimensional implementation of the time-dependent two-particle reduced density matrix (TD-2RDM) method for many-electron atoms. We benchmark this approach by a comparison with multi-configurational time-dependent Hartree-Fock (MCTDHF) results for the harmonic spectra of beryllium and neon. We show that the TD-2RDM is very well-suited to describe the non-linear atomic response and to reveal the influence of electron-correlation effects.

arXiv comment14 pages, 10 figures

References in corpus (13)

• Libxc: a library of exchange and correlation functionals for density functional theory
• Nonsequential two-photon double ionization of helium
• Time-dependent complete-active-space self-consistent field method for multielectron dynamics in intense laser fields
• Attosecond streaking of correlated two-electron transitions in helium
• Two-photon ionization of Helium studied with the multiconfigurational time-dependent Hartree-Fock method
• Time-dependent multiconfiguration self-consistent-field method based on occupation restricted multiple active space model for multielectron dynamics in intense laser fields
• Time-dependent complete-active-space self-consistent-field method for atoms: Application to high-harmonic generation
• Cross sections for short pulse single and double ionization of helium
• Propagating two-particle reduced density matrices without wavefunctions
• Challenges in Truncating the Hierarchy of Time-Dependent Reduced Density Matrices Equations: Open Problems
• Two-photon Double Ionization of H${}_2$ in Intense Femtosecond Laser Pulses
• Momentum distributions in time-dependent density functional theory: Product phase approximation for non-sequential double ionization in strong laser fields
• Truncation scheme of time-dependent density-matrix approach

Cited by in corpus (21)

• Future of Nuclear Fission Theory
• Multiconfigurational time-dependent Hartree approaches for indistinguishable particles
• Achieving the Ultimate Scaling Limit for Nonequilibrium Green Functions Simulations
• The G1--G2 Scheme: Dramatic Acceleration of Nonequilibrium Green Functions Simulations Within the Hartree--Fock-GKBA
• The dynamically screened ladder approximation: Simultaneous treatment of strong electronic correlations and dynamical screening out of equilibrium
• One-body reduced density-matrix functional theory in finite basis sets at elevated temperatures
• Time-dependent optimized coupled-cluster method for multielectron dynamics IV: Approximate consideration of the triple excitation amplitudes
• Non-equilibrium correlation dynamics in the one-dimensional Fermi-Hubbard model: A testbed for the two-particle reduced density matrix theory
• Density-based one-dimensional model potentials for strong-field simulations in $\text{He}$, ${\text{H}}_2^{+}$ and ${\text{H}}_2$
• Accelerating Nonequilibrium Green functions simulations: the G1-G2 scheme and beyond
• Nuclear Quantum Many-Body Dynamics: From Collective Vibrations to Heavy-Ion Collisions (2nd edition)
• Gauge Invariance beyond the Electric Dipole Approximation
• The BBGKY hierarchy for ultracold bosonic systems: II. Applications
• Accelerating Nonequilibrium Green functions simulations with embedding selfenergies
• Combining phase-space and time-dependent reduced density matrix approach to describe the dynamics of interacting fermions
• Implementation of gauge-invariant time-dependent configuration interaction singles method for three-dimensional atoms
• Multiconfigurational time-dependent density functional theory for atomic nuclei: Technical and numerical aspects
• Influence of coherent vibronic excitation on the high harmonics generation of diatomic molecules
• Single-photon double ionization: renormalized-natural-orbital theory vs multi-configurational Hartree-Fock
• Spin adaptation of the cumulant expansions of reduced density matrices
• Capturing reduced-order quantum many-body dynamics out of equilibrium via neural ordinary differential equations