Abstract
The ab initio description of the nonlinear response of many-electron systems to strong-laser fields remains a major challenge. In order to address larger systems, alternative methods need to be developed that bypass the exponential scaling with particle number inherent to conventional wave-function-based approaches. 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 multiconfigurational time-dependent Hartree-Fock results for the harmonic spectra of beryllium and neon. We show that the TD-2RDM is very well suited to describe the nonlinear atomic response and to reveal the influence of electron-correlation effects.
3 More- Received 3 November 2016
DOI:https://doi.org/10.1103/PhysRevA.95.033414
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