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We report ionic strength-dependent phase shifts in second harmonic generation (SHG) signals from charged interfaces that verify a recent model in which dispersion between the fundamental and second harmonic beams modulates observed signal intensities. We show how phase information can be used to unambiguously separate the chi(2) and interfacial potential-dependent chi(3) terms that contribute to the total signal and provide a path to test primitive ion models and mean field theories for the electrical double layer with experiments to which theory must conform. Finally, we demonstrate the new method on supported lipid bilayers and comment on the ability of our new instrument to identify hyper-Rayleigh scattering contributions to common homodyne SHG measurements in reflection geometries.
Ion specific outcomes at aqueous interfaces remain among the most enigmatic phenomena in interfacial chemistry. Here, charged fused silica/water interfaces have been probed by homodyne- and heterodyne-detected (HD) second harmonic generation (SHG) sp
Piezoresponse Force Microscopy (PFM), as a powerful nanoscale characterization technique, has been extensively utilized to elucidate diverse underlying physics of ferroelectricity. However, the intensive study of conventional PFM has revealed a growi
Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic con
Silica-based optical fibers are a workhorse of nonlinear optics. They have been used to demonstrate nonlinear phenomena such as solitons and self-phase modulation. Since the introduction of the photonic crystal fiber, they have found many exciting ap
Light with light control of surface plasmon polaritons is theoretically demonstrated. A barely simple and compact source of these waves consists in a finite number of slits (evenly spaced) perforating a metal film. The system scatters electromagnetic