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Comparison of Frozen-Density Embedding and Discrete Reaction Field Solvent Models for Molecular Properties

Journal Article · · Physical Chemistry Chemical Physics. PCCP, 8(20):2349-2359
DOI:https://doi.org/10.1039/b601997h· OSTI ID:926970

We investigate the performance of two discrete solvent models in connection with density functional theory (DFT) for the calculation of molecular properties. In our comparison we include the discrete reaction field (DRF) model, a combined quantum mechanics and molecular mechanics (QM/MM) model using a polarizable force field, and the frozen-density embedding (FDE) scheme. We employ these solvent models for ground state properties (dipole and quadrupole moments) and response properties (electronic excitation energies and frequencydependent polarizabilities) of a water molecule in the liquid phase. It is found that both solvent models agree for ground state properties, while there are significant differences in the description of response properties. The origin of these differences is analyzed in detail and it is found that they are mainly caused by a different description of the ground state molecular orbitals of the solute. In addition, for the calculation of the polarizabilities, the inclusion of the response of the solvent to the polarization of the solute becomes important. This effect is included in the DRF model, but is missing in the FDE scheme. A way of including it in FDE calculations of the polarizabilities using finite field calculations is demonstrated.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
926970
Journal Information:
Physical Chemistry Chemical Physics. PCCP, 8(20):2349-2359, Journal Name: Physical Chemistry Chemical Physics. PCCP, 8(20):2349-2359
Country of Publication:
United States
Language:
English

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