First time combination of frozen density embedding theory with the algebraic diagrammatic construction scheme for the polarization propagator of second order

Journal Article · Sat May 28 04:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4948741· OSTI ID:22657799

Prager, Stefan; Dreuw, Andreas ^[1]; Zech, Alexander; Aquilante, Francesco ^[2]

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1. Interdisciplinary Center for Scientific Computing, Ruprecht-Karls University, Im Neuenheimer Feld 368, 69120 Heidelberg (Germany)
2. Dipartimento di Chimica “G. Ciamician,” Università di Bologna, Via Selmi 2, 40126 Bologna (Italy)

The combination of Frozen Density Embedding Theory (FDET) and the Algebraic Diagrammatic Construction (ADC) scheme for the polarization propagator for describing environmental effects on electronically excited states is presented. Two different ways of interfacing and expressing the so-called embedding operator are introduced. The resulting excited states are compared with supermolecular calculations of the total system at the ADC(2) level of theory. Molecular test systems were chosen to investigate molecule–environment interactions of varying strength from dispersion interaction up to multiple hydrogen bonds. The overall difference between the supermolecular and the FDE-ADC calculations in excitation energies is lower than 0.09 eV (max) and 0.032 eV in average, which is well below the intrinsic error of the ADC(2) method itself.

• OSTI ID: 22657799
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 20 Vol. 144; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
COMPUTER CALCULATIONS
DENSITY
ENVIRONMENTAL EFFECTS
EXCITATION
EXCITED STATES
POLARIZATION
PROPAGATOR
SYNTHESIS