2009
DOI: 10.1063/1.3142861
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Strong temperature dependence of water reorientation in hydrophobic hydration shells

Abstract: We study the temperature dependence of the orientational mobility of water molecules solvating hydrophobic molecular groups with femtosecond midinfrared spectroscopy. We observe that these dynamics show a strong temperature dependence. At temperatures Ͻ30°C the solvating water molecules show a reorientation time Ͼ10 ps, which is more than four times slower than in bulk water. With increasing temperature, the reorientation of the solvating molecules strongly accelerates and becomes much more equal to the reorie… Show more

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Cited by 96 publications
(157 citation statements)
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“…Here, we observe that the effects of TMAO and TBA on the water dynamics are in fact quite similar, which suggests that the difference in the interaction with the hydrophilic groups is overwhelmed by another effect, i.e., the hydration of the hydrophobic parts of the molecules. This notion agrees with the results of previous NMR studies, 7,8,10,11 femtosecond anisotropy measurements, [12][13][14] and dielectric relaxation studies. 38 In all these studies, it was found that the effect of the solute on the dynamics of water scales with the size of the hydrophobic part of the solute molecule.…”
Section: B Polarization-resolved Pump-probe Experimentssupporting
confidence: 83%
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“…Here, we observe that the effects of TMAO and TBA on the water dynamics are in fact quite similar, which suggests that the difference in the interaction with the hydrophilic groups is overwhelmed by another effect, i.e., the hydration of the hydrophobic parts of the molecules. This notion agrees with the results of previous NMR studies, 7,8,10,11 femtosecond anisotropy measurements, [12][13][14] and dielectric relaxation studies. 38 In all these studies, it was found that the effect of the solute on the dynamics of water scales with the size of the hydrophobic part of the solute molecule.…”
Section: B Polarization-resolved Pump-probe Experimentssupporting
confidence: 83%
“…The anisotropy of aqueous solutions of amphiphilic solutes has been found to show a biexponential decay, with a fast component having a time constant of 2.5 ps, similar to what is observed for the reorientation of pure HDO: D 2 O, 29 and a slow component with a time constant Ͼ10 ps. [12][13][14] The amplitude of the slow component was observed to increase with the solute concentration. This latter component was assigned to the reorientation of water in the hydration shell of the hydrophobic part of the solute.…”
Section: B Polarization-resolved Pump-probe Experimentsmentioning
confidence: 98%
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“…Experiments and simulations show that near a hydrophobic (Φ) residue water-water HBs are more stable than in bulk [15,[49][50][51] with stronger water-water correlation [52]. We model this by replacing J of Eq.…”
mentioning
confidence: 99%