Random occurrence of stimulated Raman scattering emission from liquid water microdroplets

Stimulated Raman scattering (SRS) spectra from micrometer-sized water droplets have been obtained in the range 2100 < Δν < 5100 cm-(1). A number of Raman bands have been individually identified (to our knowledge, for the first time), corresponding to fundamental OH- and OD-stretching vibrations and to vibrations of hydrogen-bonded molecular complexes. All bands exhibit the intense morphologydependent resonance features that are characteristic of SRS emission from microdroplets. SRS emission is apparently random from all bands; however, the frequency of occurrence varies widely, from bands where emission is seen on practically every laser shot to bands where emission is seen only once in > 10(4) laser shots. Possible causes of these noteworthy emission features are discussed, including the difficulty of coupling weak spontaneous Raman emission to both the intense pump beam and the morphologydependent resonances within the droplet.