Stimulated Raman scattering in micrometer-sized droplets:time-resolved measurements

Time-resolved measurements of elastic scattering and stimulated Raman scattering (SRS) in micrometer-sized water and carbon tetrachloride droplets irradiated with a pulsed, frequency-doubled Nd:YAG laser (pulse width 8 nsec, λ = 532 nm, peak intensity ~1 GW cm−2) are reported. Elastic scattering of light is instantaneous within our measurement error, estimated to be <±3 nsec. On the other hand, the first Stokes shift in water and multiple-order (through ninth-order) Stokes shifts in carbon tetrachloride are delayed from the elastically scattered light by 5–7 nsec. The delay in SRS is apparently a consequence of structure resonances within the droplet, which acts as an optical cavity with relatively high Q. Quasi-periodic peaks in SRS spectra of water droplets are shown to be associated with elastic-scattering structure resonances having the same mode order.