Author: ["Xiaoji G. Xu","Stanislav O. Konorov","John W. Hepburn","Valery Milner"]
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Abstract
Coherent anti-Stokes Raman scattering (CARS) with femtosecond laser pulses has become a widespread method in nonlinear optical spectroscopy and microscopy1,2. 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 molecules3,4 and non-invasive biological imaging5. 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 spectroscopy6,7, but offer poor spectral resolution. The latter can be improved by invoking optical8,9 or quantum10,11 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.Cite this article
Xu, X., Konorov, S., Hepburn, J. et al. Noise autocorrelation spectroscopy with coherent Raman scattering. Nature Phys 4, 125–129 (2008). https://doi.org/10.1038/nphys809 