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Register a new userBeyond the Gouy-Chapman Model with Heterodyne-Detected Second Harmonic Generation
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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.
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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) spectroscopy at pH 7 and pH 5.8 and for concentrations of LiCl, NaCl, NaBr, NaI, KCl, RbCl, and CsCl ranging from 10 mc microM to several 100 mM. For ionic strengths around 0.1 mM to 1 mM, SHG intensities increase reversibly by up to 15% compared to the condition of zero added salt because of optical phase matching and electrical double layer. For ionic strengths above 1 mM, use of any combination of cations and anions produces decreases in SHG response by as much as 50%, trending with ion softness when compared to the condition of zero added salt. Gouy- Chapman model fits to homodyned SHG intensities for the alkali halides studied here show charge densities increase significantly with decreasing cation size. HD-SHG measurements indicate diffuse layer properties probed by the SHG process are invariant with ion identity, while Stern layer properties, as reported by chi(2), are subject to ion specificity for the ions surveyed in this work in the order of chi(2)RbCl = 1/2 chi(2)NaCl = 1/4 chi(2)NaI .
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 growing number of concerns and limitations which are largely challenging its validity and application. Herein, we developed a new advanced PFM technique, named Heterodyne Megasonic Piezoresponse Force Microscopy (HM-PFM), which uniquely uses 106 to 108 Hz high-frequency excitation and heterodyne method to measure the piezoelectric strain at nanoscale. We report that HM-PFM can unambiguously provide standard ferroelectric domain and hysteresis loop measurements, and an effective domain characterization with excitation frequency up to ~110 MHz has been realized. Most importantly, owing to the high-frequency and heterodyne scheme, the contributions from both electrostatic force and electrochemical strain can be significantly minimized in HM-PFM. Furthermore, a special difference-frequency piezoresponse frequency spectrum (DFPFS) measurement is developed on HM-PFM and a distinct DFPFS characteristic is observed on the materials with piezoelectricity. It is believed that HM-PFM can be an excellent candidate for the piezoelectric or ferroelectric studies where the conventional PFM results are highly controversial.
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 conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast pump is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an an even-order nonlinear optical response. The temporal evolution of the plasmonic near-field is characterized with ~100as resolution using a novel nonlinear interferometric technique. The ability to manipulate nonlinear signals in a metamaterial geometry as demonstrated here is indispensable both to understanding the ultrafast nonlinear response of nanoscale materials, and to producing active, optically reconfigurable plasmonic devices
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 applications, such as supercontinuum white light sources and third-harmonic generation, among others. They stand out by their low loss, large interaction length, and the ability to engineer its dispersive properties, which compensate for the small chi(3) nonlinear coefficient. However, they have one fundamental limitation: due to the amorphous nature of silica, they do not exhibit second-order nonlinearity, except for minor contributions from surfaces. Here, we demonstrate significant second-harmonic generation in functionalized optical fibers with a monolayer of highly nonlinear MoS2 deposited on the fiber guiding core. The demonstration is carried out in a 3.5 mm short piece of exposed core fiber, which was functionalized in a scalable process CVD-based process, without a manual transfer step. This approach is scalable and can be generalized to other transition metal dichalcogenides and other waveguide systems. We achieve an enhancement of more than 1000x over a reference sample of equal length. Our simple proof-of-principle demonstration does not rely on either phase matching to fundamental modes, or ordered growth of monolayer crystals, suggesting that pathways for further improvement are within reach. Our results do not just demonstrate a new path towards efficient in-fiber SHG-sources, instead, they establish a platform with a new route to chi(2)-based nonlinear fiber optics, optoelectronics, and photonics platforms, integrated optical architectures, and active fiber networks.
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 fields in one side of the metal film when it is illuminated from the opposite side by a polarized light source. High intensity light sources moreover efficiently generate light at second harmonic and higher frequencies in the metal led by optical nonlinearities. It is shown how the mixing of fields scattered by the slits from a weak beam at $lambda$ wavelength, with the second harmonic fields generated by a high intensity $2 lambda$ beam, creates a destructive interference of surface plasmons in one of the two possible directions of emission from the slits, while these are enhanced along the opposite direction. The unidirectional launching of surface plasmons is due to the different properties of symmetry at $lambda$ whether they are linearly or nonlinearly generated. It is envisaged a nanodevice which might allow sending digital information codified in the surface plasmon field or be used to build ultra-narrow bandwidth surface plasmon frequency combs.
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