Convex Hartree–Fock theory for modeling ground state conical intersections

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Authors: Federico Rossi, Henrik Koch
Cited by: 2
References: 35

Abstract

Accurate modeling of conical intersections is crucial in nonadiabatic molecular dynamics, as these features govern processes such as radiationless transitions and photochemical reactions. Conventional electronic structure methods, including Hartree-Fock, density functional theory, and their time-dependent extensions, struggle in this regime. Due to their single reference nature and separate treatment of ground and excited states, they fail to capture ground state intersections. Multiconfigurational approaches overcome these limitations, but at a prohibitive computational cost. In this work, we propose a modified Hartree-Fock framework, referred to as Convex Hartree-Fock, that optimizes the reference within a tailored subspace by removing projections along selected Hessian eigenvectors. The ground and excited states are then obtained through subsequent Hamiltonian diagonalization. We validate the approach across several test cases and benchmark its performance against time-dependent Hartree-Fock within the Tamm-Dancoff approximation.

Fields of Study & Subjects

Advanced Chemical Physics Studies Spectroscopy and Quantum Chemical Studies Molecular spectroscopy and chirality

Publication details

Journal / source
Communications Chemistry
Publisher
Springer Science and Business Media LLC
Volume
9
Issue
1
Pages
32–32
Publication date
5 January 2026
Language
EN