Abstract

We report all-UV coherent anti-Stokes Raman scattering (CARS) in calcite with $250–280\mathrm{nm}$ pump, Stokes, probe, and anti-Stokes light. UV CARS efficiency is $\sim 7\times$ higher than for comparable scattering in the visible, $480–540\mathrm{nm}$. Time-resolved UV CARS reveals lengthening of the dephasing time of $1086{\mathrm{cm}}^{-1}$ $\mathrm{C}\mathrm{O}_3{}^{2-}$ internal vibrations from $4\text{to}7\mathrm{ps}$ with increasing vibrational excitation, consistent with a phonon depletion model.

© 2006 Optical Society of America

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