Discretization of time-dependent quantum systems: real-time propagation of the evolution operator

Abstract

We discuss time-dependent quantum systems on bounded domains. Our work may be viewed as a framework for several models, including linear iterations involved in time-dependent density functional theory, the Hartree-Fock model, or other quantum models. A key aspect of the analysis of the algorithms is the use of time-ordered evolution operators, which allow for both a well-posed problem and its approximation. The approximation theorems obtained for the time-ordered evolution operators complement those in the current literature. We discuss the available theory at the outset, and proceed to apply the theory systematically in later sections via approximations and a global existence theorem for a nonlinear system, obtained via a fixed point theorem for the evolution operator. Our work is consistent with first-principle real-time propagation of electronic states, aimed at finding the electronic responses of quantum molecular systems and nanostructures. We present two full 3D quantum atomistic simulations using the finite element method for discretizing the real space, and the FEAST eigenvalue algorithm for solving the evolution operator at each time step. These numerical experiments are representative of the theoretical results.

Keywords:

• time-dependent quantum systems
• TDDFT
• time-ordered evolution operators
• Hamiltonian
• potential functions
• Gauss quadrature

AMS Subject Classifications:

• 35Q41
• 81-08
• 47D08
• 81Q05

Notes

The second author is supported by the National Science Foundation under [grant number ECCS 0846457], [grant number ECCS 1028510].