When dye-doped ethanol droplets are irradiated with an intense pulsed laser beam, the resulting laser emission from individual droplets highlights the liquid-air interface. Photographs of the lasing droplets in the micrometer size range taken in a single 10-nanosecond laser pulse clearly show the dynamic changes in droplet size, shape, and orientation.

Stimulated Raman scattering (SRS) from an individual liquid droplet (~30-microm radius) has been observed for H(2)O, D(2)O, and ethanol. The occurrence of a series of spectrally narrow peaks that are regularly spaced in wavelength is consistent with morphology-dependent resonances of the droplet, which acts as an optical resonator. The input intensity required to achieve the SRS threshold for the droplet is considerably less than that for the liquid in an optical cell.

The coherent Raman mixing spectra from individual micrometer-sized droplets of ethanol and of water consist of regularly spaced peaks that correspond to the morphology-dependent resonances of a spherical droplet. In contrast, the coherent anti-Stokes Raman scattering spectra from droplets exhibit no morphology-dependent peaks. Both results are explained by the spatial overlap of the matching conditions associated with the droplet.

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The vibronic intensity distribution at room temperature and 77 °K of the 1 1Ag→1 1Bu transition for the series of linear polyenes with two through six conjugated double bonds has been measured and analyzed. These inhomogeneously broadened solution spectra can be described reasonably using only two harmonic normal modes of vibration: single and double bond stretches at ∼1200 and ∼1600 cm−1, respectively. Excited state normal coordinate displacements were determined by a least-squares fitting procedure. For both the double and single bond modes the estimated change in bond length upon excitation decreases as the length of the polyene chain increases. The bandwidth of these spectra decreases with increasing polyene length. This is well described by assuming that in solution a range of conformations differing by very small torsions about the terminal single bonds has been frozen in. The Franck–Condon analysis indicates that under these conditions all of the polyenes are approximately planar in the 1Bu state, ruling out the argument that the lack of fluorescence in butadiene and hexatriene is due to the polyene framework being significantly twisted in the lowest energy 1Bu state.