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See Supporting information
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The solvation correlation function of water was empirically fitted to a biexponential function with time constants 0.04 ps (40, and 0.73 ps (60, Alternatively, the function may be also fitted to a Gaussian (ω, 0.03 ps, 26, plus two exponentials: 0.15 ps (11, and 0.75 63, 53 To compare with the τ1e times published by Horng et al. for an extensive series of solvents,54 the solvation correlation function was fitted monoexponentially resulting on a τ1e of 0.5 ps
-
1e of 0.5 ps.
-
-
-
-
63
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57449090432
-
-
c is the number of kinetic components included in the analysis. A contains the traces of the kinetic components and depends on model parameters as pump-probe cross-correlation, rate constants, vibrational frequencies, and damping rates. The model parameters are optimized by a non-linear least squares routine to minimize the difference between the model Y and the experiment ΔOD(t,λ).
-
c is the number of kinetic components included in the analysis. A contains the traces of the kinetic components and depends on model parameters as pump-probe cross-correlation, rate constants, vibrational frequencies, and damping rates. The model parameters are optimized by a non-linear least squares routine to minimize the difference between the model Y and the experiment ΔOD(t,λ).
-
-
-
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64
-
-
57449104692
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-
Equation 2 only shows cos oscillations. Indeed, oscillations were fitted with sin(ωt) and cos(ωt) functions for each frequency with zero initial phase. The pure cosine oscillation was then reconstructed from the sumangle trigonometric relationships, and the time-zero phase of the pure cosine function can then be obtained between 0 and 2π with avoidance of the intrinsic phase uncertainty resulting from the symmetry of the cosine function.
-
Equation 2 only shows cos oscillations. Indeed, oscillations were fitted with sin(ωt) and cos(ωt) functions for each frequency with zero initial phase. The pure cosine oscillation was then reconstructed from the sumangle trigonometric relationships, and the time-zero phase of the pure cosine function can then be obtained between 0 and 2π with avoidance of the intrinsic phase uncertainty resulting from the symmetry of the cosine function.
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-1. This observation may indicate that out-of-plane modes are not optically active in the droplets at 0.3 K or else that these modes are strongly damped in the He first solvation shell. Private communication 2008
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-1. This observation may indicate that out-of-plane modes are not optically active in the droplets at 0.3 K or else that these modes are strongly damped in the He first solvation shell. Private communication 2008.
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-
0).
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