A novel nonlinear Raman spectroscopic technique, which can be used to monitor the chemical composition of an aerosol particle interface, is described. The technique is called morphology-dependent stimulated Raman scattering (MDSRS). Experimental results show that there is a quantifiable relation between MDSRS signal size and the concentration of species being probed. We outline the analytic form of the nonlinear gain equation and prove its reliability by modeling MDSRS signal strengths.
Experimental confirmation that morphology-dependent stimulated Raman scattering can be used as an optical imaging technique is given. The water structure variations present at a charged water/air interface have been mapped. The measured structure variations track precisely that given by the Gouy–Chapman theory. We present, to our knowledge, the first experimental investigations of water solvent response in the diffuse part of the electric double layer. Imaging experiments on droplets charged to both positive and negative values have enabled us to determine the neutral water/air interface potential.
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