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A time-resolved coherent anti-Stokes Raman scattering (CARS) microscope allows three-dimensional imaging based on Raman free induction decay of molecular vibration with no requirement for labeling of the sample with natural or artificial fluorophores. A major benefit of the technique is the capability to completely remove nonresonant coherent background signal from the sample and the solvent, and thus increasing the detection sensitivity of CARS microscopy significantly. © 2002 American Institute of Physics.