On the exact treatment of Time Dependent Self-Interaction Correction

TL;DR

This paper introduces a new variational formulation of time-dependent self-interaction correction (TDSIC) that explicitly maintains orbital orthonormality, improving numerical implementation for laser-excited molecular dynamics.

Contribution

It develops a double-set TDSIC scheme with explicit symmetry constraints, enhancing the accuracy and practicality of TDSIC in time-dependent quantum simulations.

Findings

Successful implementation in 1D molecular models

Application to full 3D laser-excited dynamics

Improved numerical stability and accuracy

Abstract

We present a new formulation of the time-dependent self-interaction correction (TDSIC). It is derived variationally obeying explicitly the constraints on orthonormality of the occupied single-particle orbitals. The thus emerging rather involved symmetry condition amongst the orbitals is dealt with using two separate sets of (occupied) single-particle wavefunctions, related by a unitary transformation. The double-set TDSIC scheme is well suited for numerical implementation. We present results for laser-excited dynamics in a 1D model for a molecule and in fully fledged 3D calculations.