Whispering gallery mode resonators (WGMR) show two unique properties, a long photon lifetime and small mode volume that allow the reduction of the threshold of nonlinear phenomena1-3. Whispering gallery modes are optical modes that are confined at the dielectric air interface by total internal reflection. The small mode volume is due to the high spatial confinement whereas the temporal confinement is related to the quality factor Q of the cavity. WGMR can have different geometries and there are different fabrication techniques suitable for obtaining high Q resonators4-6 Surface tension cavities such as silica microspheres exhibit near atomic scale roughness, which translates in high quality factors. Both types of confinement significantly reduce the threshold for nonlinear effects due to the strong energy buildup inside the WGMR. It also allows continuous wave (CW) nonlinear optics.
WGMR can be described using the quantum numbers n, l, m and their polarization state, in a strong analogy with the hydrogen atom7. The spherical symmetry allows the separation in radial and angular dependencies. The radial solution is given by Bessel functions, the angular ones by the spherical harmonics8.
Silica glass is centrosymmetric and, therefore, second order phenomena related to Χ(2) interactions are forbidden. At the surface of the microsphere, the inversion of symmetry is broken and Χ(2) phenomena can be observed1. However, phase matching conditions for second-order frequency generation are more problematic than the equivalent in third order frequency generation, especially because the wavelengths involved are quite different and the role of dispersion can be quite important. The second order interactions are extremely weak. The generated power scales with Q3 whereas for a third order interaction the generated power scales with Q4.9 For that reason, the focus of this work is third order optical non-linear susceptibility Χ(3) interactions such as Stimulated Raman Scattering (SRS) and Stimulated Antistokes Raman Scattering (SARS), being SARS the less explored interaction10,11. Chang12 and Campillo13 pioneered the studies of nonlinear phenomena using droplets of highly nonlinear materials as WGMR but the pump laser was pulsed instead of CW. Silica microspheres14,10 and microtoroids15 provided more stable and robust platforms compared to the micro-droplets, gaining much of the attention in the last decades. Particularly, silica microspheres are very easy to fabricate and handle.
SRS is a pure gain process that can be easily achieved in silica WGMR14,15, since reaching a threshold is enough. In this case, the high circulating intensity inside the WGMR guarantees Raman lasing, but for parametric oscillations is not sufficient. In these cases, efficient oscillations require phase and mode matching, energy and momentum conservation law and a good spatial overlap of all resonant modes to be fulfilled16-18. This is the case for SARS and FWM in general.