Generation of femtosecond optical vortices by molecular modulation in a Raman-active crystal

We have generated multi-color optical vortices in a Raman-active crystal PbWO4 using two-color Fourier-transform limited femtosecond laser pulses. This setup overcomes some of the limitation of our previous research by allowing for the production of subcycle femtosecond optical vortices without the need for compensating for added chirp. In addition, the use of an OPA allows for greater flexibility in exciting different Raman modes. We verified the topological charges using two different methods. These diagnostic experiments verify not only theoretically predicted OAM algebra but demonstrated instabilities in high-order OVs. We have also studied factors which affect the high-order vortex sidebands such as the diameter and intensity of the input beams.