The real-time contour formalism for Green's functions provides time-dependent information of quantum many-body systems. In practice, the long-time simulation of systems with a wide range of energy scales is challenging due to both the storage requirements of the discretized Green's function and the computational cost of solving the Dyson equation. In this paper, we apply a real-time discretization based on a piecewise high-order orthogonal-polynomial expansion to address these issues. We present a superconvergent algorithm for solving the real-time equilibrium Dyson equation using the Legendre spectral method and the recursive algorithm for Legendre convolution. We show that the compact high-order discretization in combination with our Dyson solver enables long-time simulations using far fewer discretization points than needed in conventional multistep methods. As a proof of concept, we compute the molecular spectral functions of ${\mathrm{H}}_2$, LiH, ${\mathrm{He}}_2$, and ${\mathrm{C}}_6{\mathrm{H}}_4{\mathrm{O}}_2$ using self-consistent second-order perturbation theory and compare the results with standard quantum chemistry methods as well as the auxiliary second-order Green's function perturbation theory method.

• Received 9 June 2022
• Revised 5 September 2022
• Accepted 9 September 2022

DOI:https://doi.org/10.1103/PhysRevB.106.125153

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Published by the American Physical Society