  The success of non-linear optics relies largely on pulse-to-pulse
consistency. In contrast, covariance based techniques used in photoionization
electron spectroscopy and mass spectrometry have shown that wealth of
information can be extracted from noise that is lost when averaging multiple
measurements. Here, we apply covariance based detection to nonlinear optical
spectroscopy, and show that noise in a femtosecond laser is not necessarily a
liability to be mitigated, but can act as a unique and powerful asset. As a
proof of principle we apply this approach to the process of stimulated Raman
scattering in alpha-quartz. Our results demonstrate how nonlinear processes in
the sample can encode correlations between the spectral components of
ultrashort pulses with uncorrelated stochastic fluctuations. This in turn
provides richer information compared to the standard non-linear optics
techniques that are based on averages over many repetitions with well-behaved
laser pulses. These proof-of-principle results suggest that covariance based
nonlinear spectroscopy will improve the applicability of fs non-linear
spectroscopy in wavelength ranges where stable, transform limited pulses are
not available such as, for example, x-ray free electron lasers which naturally
have spectrally noisy pulses ideally suited for this approach.
