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Ultrafast energy relaxation and anisotropy decay of the librational motion in liquid water: A molecular dynamics study
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10.1063/1.3254518
/content/aip/journal/jcp/131/16/10.1063/1.3254518
http://aip.metastore.ingenta.com/content/aip/journal/jcp/131/16/10.1063/1.3254518
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

(a) Schematic of computational procedure for Eq. (8) and (b) that for Eq. (10). Solid, dotted, and dashed lines denote the equilibrium, forward nonequilibrium, and backward nonequilibrium trajectories, respectively.

Image of FIG. 2.
FIG. 2.

2D IR correlation spectra of the librational motion in liquid water for the all-parallel polarization.

Image of FIG. 3.
FIG. 3.

Loss of frequency correlation of the librational motion in liquid water. (a) Nodal slope, (b) inhomogeneity index, and (c) 3PEPS.

Image of FIG. 4.
FIG. 4.

Three-pulse stimulated photon echo signals of the librational motion in liquid water for several waiting times.

Image of FIG. 5.
FIG. 5.

Two-color 2D IR correlation spectra for the all-parallel polarization.

Image of FIG. 6.
FIG. 6.

Waiting time dependence of the integrated cross-peak intensity.

Image of FIG. 7.
FIG. 7.

Feynman diagrams for the cross peak at . 0, , and denote the ground state, the excited state of the librational motion, and that of the low frequency motion, respectively.

Image of FIG. 8.
FIG. 8.

Isotropic pump-probe signals for and five different probe frequencies.

Image of FIG. 9.
FIG. 9.

Energy level diagram of the kinetic model used to fit the pump-probe signals. 0, , and denote the ground state, the excited state of the librational motion, and that of the low frequency motion, respectively. and are the overtones of and . is the combination state. is the hot ground state in which the hydrogen bonds are weakened due to the thermalization. and are the excited state of the librational motion and that of the low frequency motion in the hot ground state.

Image of FIG. 10.
FIG. 10.

Differential cross-sections. The solid, dotted, and dashed lines are , , and , respectively.

Image of FIG. 11.
FIG. 11.

Temperature dependence of the linear IR absorption spectrum of liquid water. The solid, dotted, dashed, and dashed-dotted lines are the linear IR spectrum at 280, 300, 320, and 340 K, respectively.

Image of FIG. 12.
FIG. 12.

Density of states of liquid water (solid line). The dotted and dashed lines are contributions from the librational and translational motions, respectively.

Image of FIG. 13.
FIG. 13.

(a) Short- and (b) long-time behaviors of energy changes caused by the application of an electric field pulse. Solid, dotted, and dashed lines are potential, librational kinetic, and translational kinetic energy changes, respectively. Thin solid lines in (b) are single exponential functions with a time scale of 500 fs.

Image of FIG. 14.
FIG. 14.

Anisotropy decay of the librational motion. The pump and probe frequencies are 700 and , respectively. The solid line is a single exponential function with a time scale of 116 fs. The dotted line is the orientational correlation function of the total dipole moment.

Image of FIG. 15.
FIG. 15.

Kinetic energy changes caused by the excitation of one water molecule. Red, green, and blue solid lines are the parallel components of the changes in the kinetic energies of the excited molecule, four molecules adjacent to the excited molecule, and all the remaining molecules. Dotted lines are corresponding perpendicular components. The inset enlarges the low energy region.

Image of FIG. 16.
FIG. 16.

2D IR spectra calculated with the DID approximation. (a) 2D IR spectra for the librational motion. (b) Two-color 2D IR spectra.

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/content/aip/journal/jcp/131/16/10.1063/1.3254518
2009-10-29
2014-04-17
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Ultrafast energy relaxation and anisotropy decay of the librational motion in liquid water: A molecular dynamics study
http://aip.metastore.ingenta.com/content/aip/journal/jcp/131/16/10.1063/1.3254518
10.1063/1.3254518
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