Note

Inverted time-ordering in two-dimensional-Raman-terahertz spectroscopy of water

Peter Hamm, Janne Savolainen, Junichi Ono, Yoshitaka Tanimura

Research output: Contribution to journalShort survey

22 Citations (Scopus)

Abstract

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, was studied. The dependence of the polarizibility on the nuclear coordinates is expected to be more nonlinear compared to that of the dipole moment. The hybrid equilibrium-non-equilibrium approach introduced by Tanimura and co-workers is used to compute this response function from an all-atom MD simulation. An echo arises when a coherence dephases very quickly, and then rephases upon a second perturbation. Traces of a photon echo appear in simulations of 2D-Raman spectroscopy, but only when approximating the signal with instantaneous or quenched normal modes. It is concluded that indeed the inverted pulse sequence more sensitively measures the coupling between the various degrees of freedom of water.

Original languageEnglish
Article number236101
JournalJournal of Chemical Physics
Volume136
Issue number23
DOIs
Publication statusPublished - 2012 Jun 21
Externally publishedYes

Fingerprint

Terahertz spectroscopy
Raman spectroscopy
Water
echoes
water
Dipole moment
pulses
Laser pulses
dipole moments
Photons
simulation
degrees of freedom
perturbation
Atoms
photons
excitation
atoms
interactions

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Note : Inverted time-ordering in two-dimensional-Raman-terahertz spectroscopy of water. / Hamm, Peter; Savolainen, Janne; Ono, Junichi; Tanimura, Yoshitaka.

In: Journal of Chemical Physics, Vol. 136, No. 23, 236101, 21.06.2012.

Research output: Contribution to journalShort survey

Hamm, Peter ; Savolainen, Janne ; Ono, Junichi ; Tanimura, Yoshitaka. / Note : Inverted time-ordering in two-dimensional-Raman-terahertz spectroscopy of water. In: Journal of Chemical Physics. 2012 ; Vol. 136, No. 23.
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