Langevin analysis of fundamental noise limits in coherent anti-Stokes Raman spectroscopy

We use a Langevin approach to analyze the quantum noise in coherent anti-Stokes Raman spectroscopy in several experimental scenarios: with continuous-wave input fields acting simultaneously and with fast sequential pulsed lasers where one field scatters off the coherence generated by other fields and for interactions within a cavity and in free space. In all cases, the signal and quantum noise due to spontaneous decay and decoherence in the medium are shown to be described by the same general expression. Our theory in particular shows that for short interaction times, the medium noise is not important and the efficiency is limited only by the intrinsic quantum nature of the photon. We obtain fully analytic results without making an adiabatic approximation; the fluctuations of the medium and the fields are solved self-consistently.