2 research outputs found
Noise auto-correlation spectroscopy with coherent Raman scattering
Ultrafast lasers have become one of the most powerful tools in coherent
nonlinear optical spectroscopy. Short pulses enable direct observation of fast
molecular dynamics, whereas broad spectral bandwidth offers ways of controlling
nonlinear optical processes by means of quantum interferences. Special care is
usually taken to preserve the coherence of laser pulses as it determines the
accuracy of a spectroscopic measurement. Here we present a new approach to
coherent Raman spectroscopy based on deliberately introduced noise, which
increases the spectral resolution, robustness and efficiency. We probe laser
induced molecular vibrations using a broadband laser pulse with intentionally
randomized amplitude and phase. The vibrational resonances result in and are
identified through the appearance of intensity correlations in the noisy
spectrum of coherently scattered photons. Spectral resolution is neither
limited by the pulse bandwidth, nor sensitive to the quality of the temporal
and spectral profile of the pulses. This is particularly attractive for the
applications in microscopy, biological imaging and remote sensing, where
dispersion and scattering properties of the medium often undermine the
applicability of ultrafast lasers. The proposed method combines the efficiency
and resolution of a coherent process with the robustness of incoherent light.
As we demonstrate here, it can be implemented by simply destroying the
coherence of a laser pulse, and without any elaborate temporal scanning or
spectral shaping commonly required by the frequency-resolved spectroscopic
methods with ultrashort pulses.Comment: To appear in Nature Physic