No data available.
Please log in to see this content.
You have no subscription access to this content.
No metrics data to plot.
The attempt to load metrics for this article has failed.
The attempt to plot a graph for these metrics has failed.
Three-dimensional infrared spectroscopy of isotope-diluted ice Ih
13. M. L. Cowan, B. D. Bruner, N. Huse, J. R. Dwyer, B. Chugh, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Nature (London) 434, 199–202 (2005).
14. D. Kraemer, M. L. Cowan, A. Paarmann, N. Huse, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller, Proc. Natl. Acad. Sci. U.S.A. 105(2), 437–442 (2008).
18. J. B. Asbury, T. Steinel, K. Kwak, S. A. Corcelli, C. P. Lawrence, J. L. Skinner, and M. D. Fayer, J. Chem. Phys. 121, 12431–12446 (2004).
28. T. Loerting, K. Winkel, M. Seidl, M. Bauer, C. Mitterdorfer, P. H. Handle, C. G. Salzmann, E. Mayer, J. L. Finney, and D. T. Bowron, Phys. Chem. Chem. Phys. 13, 8783–8794 (2011).
29. P. V. Hobbs, Ice Physics (Oxford University Press, Oxford, 1974).
43. P. Hamm and M. T. Zanni, Concepts and Methods of 2D Infrared Spectroscopy (Cambridge University Press, Cambridge, 2011).
57. P. M. Donaldson, R. Guo, F. Fournier, E. M. Gardner, L. M. C. Barter, C. J. Barnett, I. R. Gould, D. R. Klug, D. J. Palmer, and K. R. Willison, J. Chem. Phys. 127(11), 114513 (2007).
65. M. J. Frisch, G. W. Trucks, H. B. Schlegel et al., GAUSSIAN 09, Revision A.1, Gaussian Inc., Wallingford, CT, 2009.
69. A. R. Leach, Molecular Modelling, Principles and Applications (Pearson Education Limited, Essex, England, 2001).
71. S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford University Press, Oxford, 1995).
Article metrics loading...
Using three-dimensional infrared (3D-IR) spectroscopy, we investigate the vibrational dynamics of isotope-diluted ice Ih. By probing the OD stretch mode of HOD in H2O, we observe an extremely rapid decay (≈200 fs) of the population from the second vibrational excited state. Quantum simulations based on a two-dimensional Lippincott-Schroeder potential agree nearly quantitatively with the experimental 3D-IR lineshapes and dynamics. The model suggests that energy dissipation is enhanced due to nonadiabatic effects between vibrational states, which arise from strong mode-mixing between the OD stretch mode with lattice degrees of freedom. Furthermore, we compare the simulation results to ab initio based potentials, in which the hydrogen bond anharmonicity is too small to reproduce the experimental 3D-IR spectra. We thus conclude that the Lippincott-Schroeder potential effectively coalesces many degrees of freedom of the crystal into one intermolecular coordinate.
Full text loading...
Most read this month