Spatially dependent Rabi oscillations: An approach to sub-diffraction-limited coherent anti-Stokes Raman-scattering microscopy

We present a theoretical investigation of coherent anti-Stokes Raman scattering (CARS) that is modulated by periodically depleting the ground-state population through Rabi oscillations driven by an additional control laser. We find that such a process generates optical sidebands in the CARS spectrum and that the frequency of the sidebands depends on the intensity of the control laser light field. We show that analyzing the sideband frequency upon scanning the beams across the sample allows one to spatially resolve emitter positions where a spatial resolution of 65 nm, which is well below the diffraction limit, can be obtained.