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Study and characterization of new resonances in the frequency space in a two-level system with non-zero permanent dipole moments

Abstract:

Properties of the resonance peaks associated with the non-degenerate four-wave mixing signal in a two-level molecular system with non-zero permanent dipole moments are studied in the space defined by the pump (ω1) and probe (ω2) frequencies. An analytical expression for the Fourier components of the nonlinear homogeneous macroscopic polarization are obtained, where the terms responsible for the oscillation (at frequency ω3 — ω1- ω2) of the populations and coherences are also identified, Topological properties of the resulting nonlinear spectra are studied in frequency space using three-dimensional curves and contour plots. We have additionally identified the dominant contributions of the coherence and/or population that determine the intensity and the spectral linewidth. The critical quantities for the present analysis are the transition and permanent dipole moments when the rotating-wave approximation (rwa) is not considered. © 1995 IOP Publishing Ltd.