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• W2470777744 startingPage "7154" @default.
• W2470777744 abstract "We study the ultrafast O–H stretch vibrational relaxation dynamics of protonated water clusters embedded in a matrix of deuterated acetonitrile, using polarization-resolved mid-IR femtosecond spectroscopy. The clusters are produced by mixing triflic (trifluoromethanesulfonic) acid and H2O in molar ratios of 1:1, 1:2, and 1:3, thus varying the degree of hydration of the proton. At all hydration levels the excited O–H stretch vibration of the hydrated proton shows an ultrafast vibrational relaxation with a time constant T1 < 100 fs, leading to an ultrafast local heating of the protonated water cluster. This excess thermal energy, initially highly localized to the region of the excited proton, first re-distributes over the aqueous cluster and then dissipates into the surrounding acetonitrile matrix. For clusters with a triflic acid to H2O ratio of 1:3 these processes occur with time constants of 320 ± 20 fs and 1.4 ± 0.1 ps, respectively. The cooling of the clusters reveals a long-living, underlying transient absorption change with high anisotropy. We argue that this feature stems from the vibrational predissociation of a small fraction of the proton hydration structures, directly following the ultrafast infrared excitation." @default.
• W2470777744 created "2016-07-22" @default.
• W2470777744 creator A5007130708 @default.
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• W2470777744 date "2016-07-13" @default.
• W2470777744 modified "2023-09-26" @default.
• W2470777744 title "Vibrational Relaxation of the Aqueous Proton in Acetonitrile: Ultrafast Cluster Cooling and Vibrational Predissociation" @default.
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• W2470777744 doi "https://doi.org/10.1021/acs.jpcb.6b02799" @default.
• W2470777744 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/27333302" @default.
• W2470777744 hasPublicationYear "2016" @default.
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