Intermediate state representation approach to physical properties of molecular electron-attached states

• Verfasst von: Dempwolff, Adrian [VerfasserIn]
• Verfasst von: Belogolova, Alexandra M. [VerfasserIn]
• Verfasst von: Trofimov, Alexander B. [VerfasserIn]
• Verfasst von: Dreuw, Andreas [VerfasserIn]
• Titel: Intermediate state representation approach to physical properties of molecular electron-attached states
• Titelzusatz: theory, implementation, and benchmarking
• Verf.angabe: Adrian L. Dempwolff, Alexandra M. Belogolova, Alexander B. Trofimov, and Andreas Dreuw
• E-Jahr: 2021
• Jahr: 10 March 2021
• Umfang: 17 S.
• Teil: volume:154
• Teil: year:2021
• Teil: number:10
• Teil: elocationid:104117
• Teil: pages:1-17
• Teil: extent:17
• Fussnoten: Gesehen am 26.04.2021
• Titel Quelle: Enthalten in: The journal of chemical physics
• Ort Quelle: Melville, NY : American Institute of Physics, 1933
• Jahr Quelle: 2021
• Band/Heft Quelle: 154(2021), 10, Artikel-ID 104117, Seite 1-17
• ISSN Quelle: 1089-7690
• DOI: doi:10.1063/5.0043337
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 1755951353

Abstract

Computational schemes for comprehensive studies of molecular electron-attached states and the calculation of electron affinities (EAs) are formulated and implemented employing the intermediate state representation (ISR) formalism and the algebraic-diagrammatic construction approximation for the electron propagator (EA-ADC). These EA-ADC(n)/ISR(m) schemes allow for a consistent treatment of not only electron affinities and pole strengths up to third-order of perturbation theory (n = 3) but also one-electron properties of electron-attached states up to second order (m = 2). The EA-ADC/ISR equations were implemented in the Q-Chem program for ŜzŜz<math display="inline" overflow="scroll" altimg="eq-00001.gif"><msub><mrow><mi>Ŝ</mi></mrow><mrow><mi>z</mi></mrow></msub></math>-adapted intermediate states, allowing also open-shell systems to be studied using unrestricted Hartree-Fock references. For benchmarking of the EA-(U)ADC/ISR schemes, EAs and dipole moments of various electron-attached states of small closed- and open-shell molecules were computed and compared to full configuration interaction data. As an illustrative example, EA-ADC(3)/ISR(2) has been applied to the thymine-thymine (6-4) DNA photolesion.