A Constraint-Based Orbital-Optimized Excited State Method (COOX).

ABSTRACT: In this work, we present a novel method to directly calculate targeted electronic excited states within a self-consistent field calculation based on constrained density functional theory (cDFT). The constraint is constructed from the static occupied-occupied and virtual-virtual parts of the excited state difference density from (simplified) linear-response time-dependent density functional theory calculations (LR-TDDFT). Our new method shows a stable convergence behavior, provides an accurate excited state density adhering to the Aufbau principle, and can be solved within a restricted SCF for singlet excitations to avoid spin contamination. This also allows the straightforward application of post-SCF electron-correlation methods like MP2 or direct RPA methods. We present the details of our

SUBMITTER: Kussmann J 

PROVIDER: S-EPMC11465468 | biostudies-literature | 2024 Oct

REPOSITORIES: biostudies-literature