We theoretically investigate ground-state depletion for subdiffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. We propose a scheme based on ground-state depopulation, which is achieved via a control laser light field incident prior to the CARS excitation light fields. This ground-state depopulation results in a reduced CARS signal generation. With an appropriate choice of spatial beam profiles, the scheme can be used to increase the spatial resolution. Based on the density matrix formalism we calculate the CARS signal generation and find a CARS signal suppression by 75
due to ground-state depletion with a single control light field and by using two control light fields the CARS signal suppression can be enhanced to 94
. Additional control light fields will enhance the CARS suppression even further. In case of a single control light field we calculate resulting CARS images using a computer-generated test image including quantum and detector noise and show that the background from the limited CARS suppression can be removed by calculating difference images, yielding subdiffraction-limited resolution where the resolution achievable depends only on the intensity used.
The non-classical effects of squeezing of light in coherent anti-Stokes Raman scattering (CARS) and coherent anti-Stokes hyper-Raman scattering (CAHRS) are investigated under the short-time approximation based on a fully quantum mechanical approach. In an idealized model CARS, the interaction is looked upon as a process involving absorption of a pump photon and emission of a Stokes photon, which is followed by absorption of a pump photon and subsequently emission of an anti-Stokes photon at a different frequency, whereas CAHRS is looked upon as a process involving absorption of two pump photons and emission of a Stokes photon, which is followed by absorption of two more pump photons and subsequent emission of an anti-Stokes photon at a different frequency. The coupled Heisenberg equations of motion involving real and imaginary parts of the quadrature operators are established. It is shown that squeezing in the Stokes and anti-Stokes mode in CARS is found to be dependent on amplitude-squared squeezing of the initial pump field while, in CAHRS, it is dependent on the fourth-order amplitude squeezing of the initial pump field. Higher-order squeezing can be converted to linear squeezing through these processes. It is also shown that squeezing is greater in CAHRS than the corresponding squeezing in CARS.