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• W2076244804 startingPage "9352" @default.
• W2076244804 abstract "Vibrational relaxation of methanol-d (MeOD) in carbon tetrachloride has been investigated via ultrafast infrared pump–probe experiments. Exciting at 2690 cm−1, only the free O-D (where the D is not H-bonded) stretching mode is initially populated. For MeOD mole fractions ⩽0.025, a 2.15 ps single exponential decay is observed. At mole fractions ⩾0.0375, the signal decays (2.15 ps decay time) below zero (increased absorption) and then recovers on time scales of 22 ps and ≫300 ps. The increased absorption indicates the formation of additional free ODs caused by the breaking of H-bonds that are not directly coupled to the initially excited vibration. The two-time scale recovery of this signal arises from geminate and nongeminate recombination. The data are fit with a set of kinetic equations that accurately reproduce the data. The results suggest that vibrational relaxation of the initially excited free OD stretch into intramolecular modes of the methanol leads to H-bond breaking. This contrasts studies that suggest direct relaxation of a vibrationally excited OH stretch into an H-bond stretch is responsible for H-bond breaking." @default.
• W2076244804 created "2016-06-24" @default.
• W2076244804 creator A5005348091 @default.
• W2076244804 creator A5056327870 @default.
• W2076244804 creator A5078149381 @default.
• W2076244804 date "2001-11-22" @default.
• W2076244804 modified "2023-09-27" @default.
• W2076244804 title "Vibrational relaxation of the free terminal hydroxyl stretch in methanol oligomers: Indirect pathway to hydrogen bond breaking" @default.
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• W2076244804 doi "https://doi.org/10.1063/1.1415447" @default.
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