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

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.