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Title: Line-space description of resonant four-wave mixing: Theory for isotropic molecular states

Based on the quantum Liouville formalism, a theory of the two-color, triply resonant four-wave mixing is developed for molecules with isotropically oriented angular momenta. The approach allows to strictly incorporate the relaxation matrices Γ{sup (r)} (r = 0, 1, 2) into the third-order susceptibility χ{sup (3)} whose expression acquires therewith the form of a scalar product in the line space. Thanks to this representation, isolation of all resonance terms from χ{sup (3)} becomes a routine task. Some of these terms correspond to the case when a molecule initially interacts with two pump photons of the same frequency. Such interactions give rise to the grating line-space vectors which have the same (zero) eigenfrequency. Due to this degeneracy, the latter are easily mixed by rotationally inelastic collisions which shows up in a state-resolved coherence transfer. The satellite signals induced thereby provide a great scope to study the state-to-state inelastic rates in situ by purely optical means. If the diagonal form of Γ is assumed, the satellites become forbidden and our results reduce to conventional expressions for the main resonances. Polarization configurations are designed for direct measurements of the population (r = 0), orientation (r = 1), and alignment (r = 2) contributionsmore » to χ{sup (3)}. Finally, depending on the photon-molecule interaction sequence, the resonance terms of χ{sup (3)} are shown to be differently affected by velocity averaging, the effect which conspicuously manifests itself when Doppler broadening becomes paramount.« less
Authors:
 [1] ;  [2]
  1. Department of Physics, Saint-Petersburg State University, Ulyanovskaya str. 3, Peterhof, Saint-Petersburg 198504 (Russian Federation)
  2. Paul Scherrer Institute, CH-5232 Villigen (Switzerland)
Publication Date:
OSTI Identifier:
22254870
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 19; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; EIGENFREQUENCY; FREQUENCY MIXING; INTERACTIONS; PHOTONS; POLARIZATION