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

Asbury, John B.; Steinel, Tobias; Stromberg, Christopher J.; Gaffney, Kelly J.; Piletic, Ivan R.; Goun, Alexei; Fayer, M. D.

doi:10.1016/s0009-2614(03)00643-2

Cited by 75 publications

(122 citation statements)

References 31 publications

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“…By adding the Fourier transforms of the interferograms from the two pathways, the dispersive component can be substantially cancelled leaving only the absorptive component. 26,44 Following a phasing procedure 44,45 based on the projection slice theorem, 26,44,46 the 2D vibrational echo spectra are constructed by plotting the amplitude of the absorptive part of spectrum (see below).…”

Section: The 2d Vibrational Echo Methodsmentioning

confidence: 99%

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Finkelstein

Zheng

Ishikawa

et al. 2007

Phys. Chem. Chem. Phys.

148

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Ultrafast 2D IR vibrational echo spectroscopy is described and a number of experimental examples are given. Details of the experimental method including the pulse sequence, heterodyne detection, and determination of the absorptive component of the 2D spectrum are outlined. As an initial example, the 2D spectrum of the stretching mode of CO bound to the protein myoglobin (MbCO) is presented. The time dependence of the 2D spectrum of MbCO, which is caused by protein structural evolution, is presented and its relationship to the frequency-frequency correlation function is described and used to make protein structural assignments based on comparisons to molecular dynamics simulations. The 2D vibrational echo experiments on the protein horseradish peroxidase are presented. The time dependence of the 2D spectra of the enzyme in the free form and with a substrate bound at the active site are compared and used to examine the influence of substrate binding on the protein's structural dynamics. The application of 2D vibrational echo spectroscopy to the study of chemical exchange under thermal equilibrium conditions is described. 2D vibrational echo chemical exchange spectroscopy is applied to the study of formation and dissociation of organic solute-solvent complexes and to the isomerization around a carbon-carbon single bond of an ethane derivative.

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Section: The 2d Vibrational Echo Methodsmentioning

confidence: 99%

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Finkelstein

Zheng

Ishikawa

et al. 2007

Phys. Chem. Chem. Phys.

148

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“…49 Here, we present a detailed account of the vibrational echo experiments on AOT reverse micelles that have been reported previously, 49 including new frequency-dependent data, as well as vibrational pump-probe experiments that examine the population dynamics of the hydroxyl stretch. Vibrational echo spectroscopy [16][17][18]20,[50][51][52][53][54][55][56] is uniquely capable of determining system dynamics by removing the inhomogeneous broadening contribution from the line shape 16,[56][57][58][59][60][61][62] and tracking the underlying dynamics. 63, 64 The properties of hydrogen-bond networks can be studied using IR spectroscopy of the hydroxyl stretching mode, because of the strong influence of the number and strength of hydrogen bonds on the hydroxyl stretch frequency.…”

Section: Introductionmentioning

confidence: 99%

Dynamics of Nanoscopic Water: Vibrational Echo and Infrared Pump−Probe Studies of Reverse Micelles

2005

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The dynamics of water in nanoscopic pools 1.7-4.0 nm in diameter in AOT reverse micelles were studied with ultrafast infrared spectrally resolved stimulated vibrational echo and pump-probe spectroscopies. The experiments were conducted on the OD hydroxyl stretch of low-concentration HOD in the H 2 O, providing a direct examination of the hydrogen-bond network dynamics. Pump-probe experiments show that the vibrational lifetime of the OD stretch mode increases as the size of the reverse micelle decreases. These experiments are also sensitive to hydrogen-bond dissociation and reformation dynamics, which are observed to change with reverse micelle size. Spectrally resolved vibrational echo data were obtained at several frequencies. The vibrational echo data are compared to data taken on bulk water and on a 6 M NaCl solution, which is used to examine the role of ionic strength on the water dynamics in reverse micelles. Two types of vibrational echo measurements are presented: the vibrational echo decays and the vibrational echo peak shifts. As the water nanopool size decreases, the vibrational echo decays become slower. Even the largest nanopool (4 nm, ∼1000 water molecules) has dynamics that are substantially slower than bulk water. It is demonstrated that the slow dynamics in the reverse micelle water nanopools are a result of confinement rather than ionic strength. The data are fit using time-dependent diagrammatic perturbation theory to obtain the frequency-frequency correlation function (FFCF) for each reverse micelle. The results are compared to the FFCF of water and show that the largest differences are in the slowest time scale dynamics. In bulk water, the slowest time scale dynamics are caused by hydrogen-bond network equilibration, i.e., the making and breaking of hydrogen bonds. For the smallest nanopools, the longest time scale component of the water dynamics is ∼10 times longer than the dynamics in bulk water. The vibrational echo data for the smallest reverse micelle displays a dependence on the detection wavelength, which may indicate that multiple ensembles of water molecules are being observed.

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“…The vibrational properties of liquid water have received considerable attention. [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22]31,[43][44][45] Much experimental [9][10][11][12][13][14][15][16][17] and theoretical [18][19][20][21]43,44 effort has focused on the OH stretch of HOD in D 2 O. This is a simpler system than neat water since that mode is spectrally isolated so that the rapid resonant intermolecular vibrational energy transfer 46 is eliminated.…”

Section: Introductionmentioning

confidence: 99%

Collective Solvent Coordinates for the Infrared Spectrum of HOD in D₂O Based on an ab Initio Electrostatic Map

et al. 2004

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An ab initio MP2 vibrational Hamiltonian of HOD in an external electrostatic potential parametrized by the electric field and its gradient-tensor is constructed. By combining it with the fluctuating electric field induced by the D 2 O solvent obtained from molecular dynamics simulations, we calculate the infrared absorption of the O-H stretch. The resulting solvent shift and infrared line shape for three force fields (TIP4P, SPC/E, and SW) are in good agreement with the experiment. A collective coordinate response for the solvent effect is constructed by identifying the main electrostatic field and gradient components contributing to the line shape. This allows a realistic stochastic Liouville equation simulation of the line shapes which is not restricted to Gaussian frequency fluctuations.

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

Cited by 75 publications

References 31 publications

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Dynamics of Nanoscopic Water: Vibrational Echo and Infrared Pump−Probe Studies of Reverse Micelles

Collective Solvent Coordinates for the Infrared Spectrum of HOD in D₂O Based on an ab Initio Electrostatic Map

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

Cited by 75 publications

References 31 publications

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

Dynamics of Nanoscopic Water: Vibrational Echo and Infrared Pump−Probe Studies of Reverse Micelles

Collective Solvent Coordinates for the Infrared Spectrum of HOD in D2O Based on an ab Initio Electrostatic Map

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Collective Solvent Coordinates for the Infrared Spectrum of HOD in D₂O Based on an ab Initio Electrostatic Map