Ultrafast heterodyne detected infrared multidimensional vibrational stimulated echo studies of hydrogen bond dynamics

John B. Asbury; Tobias Steinel; C. Stromberg; K. J. Gaffney; I. R. Piletic; Alexi Goun; M. D. Fayer

doi:10.1016/S0009-2614(03)00643-2

Ultrafast heterodyne detected infrared multidimensional vibrational stimulated echo studies of hydrogen bond dynamics

John B. Asbury, Tobias Steinel, C. Stromberg, K. J. Gaffney, I. R. Piletic, Alexi Goun, M. D. Fayer

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80 Scopus citations

Abstract

Multidimensional vibrational stimulated echo correlation spectra with full phase information are presented for the broad hydroxyl stretch band of methanol-OD oligomers in CCl₄ using ultrashort (<50 fs) infrared pulses. Hydrogen bond breaking permits data to be acquired for times much greater than the vibrational lifetime. The data indicates that vibrational relaxation leads to preferential hydrogen bond breaking for oligomers on the red side of the spectrum. An off diagonal peak in the correlation spectrum that appears at long time (>1 ps) shows that there is frequency correlation between the initially excited hydroxyl stretch and the frequency shifted hydroxyl stretch formed by hydrogen bond breaking.

Original language	English (US)
Pages (from-to)	362-371
Number of pages	10
Journal	Chemical Physics Letters
Volume	374
Issue number	3-4
DOIs	https://doi.org/10.1016/S0009-2614(03)00643-2
State	Published - Jun 11 2003

All Science Journal Classification (ASJC) codes

General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1016/S0009-2614(03)00643-2

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@article{d87d90685f864e768a4abc312ddc473c,

title = "Ultrafast heterodyne detected infrared multidimensional vibrational stimulated echo studies of hydrogen bond dynamics",

abstract = "Multidimensional vibrational stimulated echo correlation spectra with full phase information are presented for the broad hydroxyl stretch band of methanol-OD oligomers in CCl4 using ultrashort (<50 fs) infrared pulses. Hydrogen bond breaking permits data to be acquired for times much greater than the vibrational lifetime. The data indicates that vibrational relaxation leads to preferential hydrogen bond breaking for oligomers on the red side of the spectrum. An off diagonal peak in the correlation spectrum that appears at long time (>1 ps) shows that there is frequency correlation between the initially excited hydroxyl stretch and the frequency shifted hydroxyl stretch formed by hydrogen bond breaking.",

author = "Asbury, {John B.} and Tobias Steinel and C. Stromberg and Gaffney, {K. J.} and Piletic, {I. R.} and Alexi Goun and Fayer, {M. D.}",

note = "Funding Information: This work was supported by the AFOSR (Grant No. F49620-01-1-0018), the National Institutes of Health (IR01-GM61137), the National Science Foundation (DMR-0088942), and the Department of Energy (Grant DE-FG03-84ER132SI). TS would like to thank the Alexander von Humboldt Foundation for partial support.",

year = "2003",

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doi = "10.1016/S0009-2614(03)00643-2",

language = "English (US)",

volume = "374",

pages = "362--371",

journal = "Chemical Physics Letters",

issn = "0009-2614",

publisher = "Elsevier",

number = "3-4",

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TY - JOUR

T1 - Ultrafast heterodyne detected infrared multidimensional vibrational stimulated echo studies of hydrogen bond dynamics

AU - Asbury, John B.

AU - Steinel, Tobias

AU - Stromberg, C.

AU - Gaffney, K. J.

AU - Piletic, I. R.

AU - Goun, Alexi

AU - Fayer, M. D.

N1 - Funding Information: This work was supported by the AFOSR (Grant No. F49620-01-1-0018), the National Institutes of Health (IR01-GM61137), the National Science Foundation (DMR-0088942), and the Department of Energy (Grant DE-FG03-84ER132SI). TS would like to thank the Alexander von Humboldt Foundation for partial support.

PY - 2003/6/11

Y1 - 2003/6/11

N2 - Multidimensional vibrational stimulated echo correlation spectra with full phase information are presented for the broad hydroxyl stretch band of methanol-OD oligomers in CCl4 using ultrashort (<50 fs) infrared pulses. Hydrogen bond breaking permits data to be acquired for times much greater than the vibrational lifetime. The data indicates that vibrational relaxation leads to preferential hydrogen bond breaking for oligomers on the red side of the spectrum. An off diagonal peak in the correlation spectrum that appears at long time (>1 ps) shows that there is frequency correlation between the initially excited hydroxyl stretch and the frequency shifted hydroxyl stretch formed by hydrogen bond breaking.

AB - Multidimensional vibrational stimulated echo correlation spectra with full phase information are presented for the broad hydroxyl stretch band of methanol-OD oligomers in CCl4 using ultrashort (<50 fs) infrared pulses. Hydrogen bond breaking permits data to be acquired for times much greater than the vibrational lifetime. The data indicates that vibrational relaxation leads to preferential hydrogen bond breaking for oligomers on the red side of the spectrum. An off diagonal peak in the correlation spectrum that appears at long time (>1 ps) shows that there is frequency correlation between the initially excited hydroxyl stretch and the frequency shifted hydroxyl stretch formed by hydrogen bond breaking.

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U2 - 10.1016/S0009-2614(03)00643-2

DO - 10.1016/S0009-2614(03)00643-2

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VL - 374

SP - 362

EP - 371

JO - Chemical Physics Letters

JF - Chemical Physics Letters

IS - 3-4

ER -

Ultrafast heterodyne detected infrared multidimensional vibrational stimulated echo studies of hydrogen bond dynamics

Abstract

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