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Updated: May 27, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
A fast doubly hybrid density functional method close to chemical accuracy using a local opposite spin ansatz
Igor Ying Zhang1, Xin Xu, Yousung Jung
1Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Ministry of Education, Fudan University, Shanghai 200433, China.
Abstract:
We develop and validate the XYGJ-OS functional, based on the adiabatic connection formalism and Görling-Levy perturbation theory to second order and using the opposite-spin (OS) ansatz combined with locality of electron correlation. XYGJ-OS with local implementation scales as N(3) with an overall accuracy of 1.28 kcal/mol for thermochemistry, bond dissociation energies, reaction barrier heights, and nonbonded interactions, comparable to that of 1.06 kcal/mol for the accurate coupled-cluster based G3 method (scales as N(7)) and much better than many popular density functional theory methods: B3LYP (4.98), PBE0 (4.36), and PBE (12.10).
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