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

A. Kouzov, P. Radi

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4 Scopus citations


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 (r)(r=0, 1, 2) into the third-order susceptibility χ(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(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 ratesin situby purely optical means. If the diagonal form of is assumed,
Original languageEnglish
Pages (from-to)194302_1-13
JournalJournal of Chemical Physics
Issue number19
StatePublished - 2014


  • четырехволновое резонансное смешение
  • столкновения и релаксация в молекулярных газах

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