Noise autocorrelation spectroscopy with coherent Raman scattering

Coherent anti-Stokes Raman scattering (CARS) with femtosecond laser pulses has become a widespread method in nonlinear optical spectroscopy and microscopy(1,2). As a third-order nonlinear process, femtosecond CARS exhibits high efficiency at low average laser power. High sensitivity to molecular structure enables detection of small quantities of complex molecules(3,4) and non-invasive biological imaging(5). Temporal and spectral resolution of CARS is typically limited by the duration of the excitation pulses and their frequency bandwidth, respectively. Broadband femtosecond pulses are advantageous for time-resolved CARS spectroscopy(6,7), but offer poor spectral resolution. The latter can be improved by invoking optical(8,9) or quantum(10,11) interference at the expense of increasing complexity of instrumentation and susceptibility to noise. Here, we present a new approach to coherent Raman spectroscopy in which high resolution is achieved by means of deliberately introduced noise. The proposed method combines the efficiency of a coherent process with the robustness of incoherent light. It does require averaging over different noise realizations, but no temporal scanning or spectral pulse shaping as commonly used by frequency-resolved spectroscopic methods with ultrashort pulses.