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Dynamic polarizability, Cauchy moments, and the optical absorption spectrum of liquid water: A sequential molecular dynamics/quantum mechanical approach
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10.1063/1.3054184
/content/aip/journal/jcp/130/1/10.1063/1.3054184
http://aip.metastore.ingenta.com/content/aip/journal/jcp/130/1/10.1063/1.3054184

Figures

Image of FIG. 1.
FIG. 1.

Dependence of the static polarizability of water with the basis-set and number of states included in the SOS for dapvdz, dapvtz, and dapvqz basis sets.

Image of FIG. 2.
FIG. 2.

Comparison between SOS, PP, and FF calculations for the dynamic polarizability of the gas phase water molecule (top panel) and dynamic polarizability of liquid water (bottom panel) calculated with SOS.

Image of FIG. 3.
FIG. 3.

Low-energy behavior for the dynamic polarizability of water in the gas (G) and liquid (L) phases (BHandHLYP/dapvdz). Liquid phase calculations were performed for (circles), (squares), and (diamonds).

Image of FIG. 4.
FIG. 4.

Imaginary part of the dielectric constant of liquid water for . Top: comparison between TIP3P and NCC charge embedding with the dapvtz basis set. Middle: behavior of using TDDFT-BHandHLYP with different basis sets (dapvdz, dapvtz, and dapvqz) in the 6–18 eV range and comparison between calculated with the NCC frozen embedding and self-consistent charges (SCF). See text for details. Bottom: comparison between EOM-CCSD and TDDFT-BHandHLYP with the dapvdz basis set.

Image of FIG. 5.
FIG. 5.

Dependence of on the number of molecules in the quantum system and number of states included in the SOS from TDDFT-BHandHLYP calculations. Top: results for with the cc-pVDZ (H) and aug-cc-pVDZ (O) basis sets. Middle: results for with the dapvdz basis set. Bottom: dependence of on the number of states included in the SOS (dapvdz).

Image of FIG. 6.
FIG. 6.

Dependence of on the number of hydrogen bonds for (BHandHLYP/dapvdz). The central water can form one (a;d) or two (aa;ad;dd) H-bonds with the other two water molecules in the quantum system.

Image of FIG. 7.
FIG. 7.

Comparison between dielectric properties of water in the gas (G) and liquid (L) phases ( and BHandHLYP/dapvqz).

Image of FIG. 8.
FIG. 8.

Comparison between theoretical predictions (EOM-CCSD and TDDFT with the dapvdz basis set) and experimental data for the dielectric properties of liquid water. Vertical arrows indicate the maxima for the reflectance spectrum of liquid water reported by Hayashi (Ref. 10 ).

Tables

Generic image for table
Table I.

Lowest excitation energies ( in eV) from the ground state (1 )and oscillator strengths ( in a.u.) of the gas phase water molecule [Theoretical calculations with the d-aug-cc-pVTZ basis-set and NCC geometry for the water molecule ( and )].

Generic image for table
Table II.

Cauchy moments (a.u.) for the water molecule in the gas and liquid phase (values in parentheses). The Cauchy moments were fitted in the energy interval [0, 2.7] eV. The calculations were carried out with the NCC geometry for the water molecule.

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/content/aip/journal/jcp/130/1/10.1063/1.3054184
2009-01-06
2014-04-24
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Dynamic polarizability, Cauchy moments, and the optical absorption spectrum of liquid water: A sequential molecular dynamics/quantum mechanical approach
http://aip.metastore.ingenta.com/content/aip/journal/jcp/130/1/10.1063/1.3054184
10.1063/1.3054184
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