Lawrence Berkeley National Laboratory

In coherent anti-Stokes Raman scattering spectroscopy (CARS) experiments, usually the amplitude of the signal is measured and the phase information is lost. With a polarization- and phase-controlled pulse shaping technique, the relative phase between the resonant and non-resonant CARS signals is controlled, and spectral interferometry is performed without an interferometer. Both the real and imaginary parts of the background-free resonant CARS spectrum are measured via spectral interferometry between the resonant and non-resonant signals from the same sample. The resonant signal is amplified significantly by homodyne mixing with the non-resonant signal as a local oscillator, greatly improving the detection limit.