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

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