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Solvation Dynamics in Water: 4. On the Initial Regime of Solvation Relaxation.

It is shown, by means of numerical and analytic work, that initial molecular momenta play little significant role in the initial fast solvation relaxation that follows electronic excitation of, and charge creation for, a standard model system of a solute in water. Instead, the nonequilibrium dynamics are predominantly described by non-inertial ``steering'' by the torques directly generated by the newly created charge distribution. It is this process that largely overcomes inertia, and drives the relaxation dynamics on a time scale of a few tens of femtoseconds in the key initial regime of the dynamics. These results are discussed in the context of commonly employed descriptions such as inertial, Gaussian, and underdamped dynamical behavior.