Permanent URL to this publication: http://dx.doi.org/10.5167/uzh-64719
Hamm, Peter; Savolainen, Janne; Ono, Junichi; Tanimura, Yoshitaka (2012). Note: Inverted time-ordering in two-dimensional-Raman-terahertz spectroscopy of water. Journal of Chemical Physics, 136(23):236101.
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In a previous paper [P. Hamm and J. Savolainen, J. Chem. Phys. 136, 094516 (2012)]10.1063/1.3691601, we have studied the 2D-Raman-THz response of liquid water, based on an all-atom molecular dynamics simulation. In the pulse sequence we investigated a near-infraredlaser pulse excites a vibrational coherence through a Raman process that switches it into another coherence by a THz pulse after some time, and finally read out by the emission of a THz field.In the present note, we explore the inverted time-ordered pulse sequence, in which the first coherence is generated by a direct THz excitation, while the switching of coherences is achieved by a Raman interaction. Since the dependence of the polarizibility on the nuclear coordinates is more nonlinear compared to that of the dipole moment, this pulse sequence reveals more of the couplings and correlations between the various degrees of freedom of water. Compared to 2D-Raman spectroscopy and the original pulse sequence, this pulse sequence reveals the clearest signature of a photon echo.
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|Item Type:||Journal Article, refereed, original work|
|Communities & Collections:||07 Faculty of Science > Department of Chemistry|
|Deposited On:||20 Sep 2012 11:47|
|Last Modified:||23 Jun 2014 13:32|
|Publisher:||American Institute of Physics|
|Funders:||Swiss National Science Foundation (SNF) through the National Center of Competence and Research (NCCR) MUST|
|Additional Information:||© 2012 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in J. Chem. Phys. 136, 236101 (2012), and may be found at http://jcp.aip.org/resource/1/jcpsa6/v136/i23/p236101_s1|
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