Picosecond infrared vibrational photon echoes in a liquid and glass using a free electron laser

Zimdars, David; Tokmakoff, Andrei; Chen, S.; Greenfield, Scott R.; Fayer, M. D.; Smith, T. I.; Schwettman, H. A.

doi:10.1103/physrevlett.70.2718

Cited by 205 publications

(149 citation statements)

References 14 publications

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“…[20][21][22][23][24] These first one-dimensional two-pulse vibrational echo experiments were conducted with an IR free electron laser. 20 However, rapid advances in laser technology now make it possible to conduct far more sophisticated vibrational echo experiments, particularly two-dimensional (2D) vibrational echoes, using table top laser systems.…”

Section: Introductionmentioning

confidence: 99%

“…2D IR vibrational echo experiments have been successfully applied to study fast chemical exchange reactions and solution dynamics, 29,31,36 water dynamics, 37,38 hydrogen network evolution, 28 intramolecular vibrational energy relaxations, 34 protein structures and dynamics, 30,39,40 and mixed chemicals analysis. 41 Since the first fast condensed matter vibrational echo experiments in 1993, 20 the field has advanced a great deal. The first experiments were 1D with a time resolution of B1 ps.…”

Section: Introductionmentioning

confidence: 99%

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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: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

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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“…15 In 1995 an Accounts of Chemical Research article was published 22 summarizing recent fast condensed phase vibrational echo experiments. 1,23,24 The experiments were 1D with a time resolution of ∼1 ps. Since those first experiments, the field has advanced greatly.…”

Section: Introductionmentioning

confidence: 99%

“…Ultrafast 2D IR vibrational echo spectroscopy [1][2][3][4][5][6][7][8][9][10][11] is an ultrafast IR analog of 2D NMR 12 that directly probes the structural degrees of freedom of molecules. 13 The 2D IR vibrational echo technique involves a three-pulse sequence that induces and then probes the coherent evolution of excitations (vibrations) of a molecular system.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast 2D IR Vibrational Echo Spectroscopy

2007

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The experimental technique and applications of ultrafast twodimensional infrared (2D IR) vibrational echo spectroscopy are presented. Using ultrashort infrared pulses and optical heterodyne detection to provide phase information, unique information can be obtained about the dynamics, interactions, and structures of molecular systems. The form and time evolution of the 2D IR spectrum permits examination of processes that cannot be studied with linear infrared absorption experiments. Three examples are given: organic solute-solvent complex chemical exchange, dynamics of the hydrogen-bond network of water, and assigning peaks in an IR spectrum of a mixture of species.

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Picosecond infrared vibrational photon echoes in a liquid and glass using a free electron laser

Cited by 205 publications

References 14 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

Ultrafast 2D IR Vibrational Echo Spectroscopy

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