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Quantum Mechanical Versus Polarizable Embedding Schemes: A Study of the Xray Absorption Spectra of Aqueous Ammonia and Ammonium.
Folkestad, Sarai Dery; Paul, Alexander C; Paul Née Matveeva, Regina; Reinholdt, Peter; Coriani, Sonia; Odelius, Michael; Koch, Henrik.
Afiliación
  • Folkestad SD; Department of Chemistry, Norwegian University of Science and Technology, NTNU, 7491 Trondheim, Norway.
  • Paul AC; Department of Chemistry, Norwegian University of Science and Technology, NTNU, 7491 Trondheim, Norway.
  • Paul Née Matveeva R; Department of Chemistry, Norwegian University of Science and Technology, NTNU, 7491 Trondheim, Norway.
  • Reinholdt P; Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, SDU, Campusvej 55, 5230 Odense, Denmark.
  • Coriani S; Department of Chemistry, Technical University of Denmark, DTU, Kemitorvet Bldg 207, 2800 Kongens Lyngby, Denmark.
  • Odelius M; Department of Physics, Stockholm University, 10691 Stockholm, Sweden.
  • Koch H; Department of Chemistry, Norwegian University of Science and Technology, NTNU, 7491 Trondheim, Norway.
J Chem Theory Comput ; 20(10): 4161-4169, 2024 May 28.
Article en En | MEDLINE | ID: mdl-38713524
ABSTRACT
The X-ray absorption spectra of aqueous ammonia and ammonium are computed using a combination of coupled cluster singles and doubles (CCSD) with different quantum mechanical and molecular mechanical embedding schemes. Specifically, we compare frozen Hartree-Fock (HF) density embedding, polarizable embedding (PE), and polarizable density embedding (PDE). Integrating CCSD with frozen HF density embedding is possible within the CC-in-HF framework, which circumvents the conventional system-size limitations of standard coupled cluster methods. We reveal similarities between PDE and frozen HF density descriptions, while PE spectra differ significantly. By including approximate triple excitations, we also investigate the effect of improving the electronic structure theory. The spectra computed using this approach show an improved intensity ratio compared to CCSD-in-HF. Charge transfer analysis of the excitations shows the local character of the pre-edge and main-edge, while the post-edge is formed by excitations delocalized over the first solvation shell and beyond.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Chem Theory Comput Año: 2024 Tipo del documento: Article País de afiliación: Noruega Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Chem Theory Comput Año: 2024 Tipo del documento: Article País de afiliación: Noruega Pais de publicación: Estados Unidos