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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…
Non-resonant second harmonic generation phase and amplitude measurements obtained from the silica:water interface at varying pH and 0.5 M ionic strength point to the existence of a nonlinear susceptibility term, which we call chi(3)X, that…
Second harmonic generation (SHG) is forbidden in centrosymmetric molecular materials. However, a signal is frequently observed from interfaces where the symmetry is broken. Whereas the effect can be phenomenologically accommodated, an ab…
We investigate optical second-harmonic generation (SHG) from metasurfaces where noncentrosymmetric V-shaped gold nanoparticles are ordered into regular array configurations. In contrast to expectations, a substantial enhancement of the SHG…
Graphite is a ubiquitous electrode material with particular promise for use in e.g., energy storage and desalination devices, but very little is known about the properties of the graphite-electrolyte double layer at technologically relevant…
Second-harmonic generation (SHG) is a second-order nonlinear optical process that is not allowed in media with inversion sym-metry. However, due to the broken symmetry at the surface, surface SHG still occurs, but is generally small. We…
We examine an electric double layer containing an antagonistic salt in an aqueous mixture, where the cations are small and hydrophilic but the anions are large and hydrophobic. In this situation, a strong coupling arises between the charge…
We report optical second-harmonic generation (SHG) in reflection from GaSe crystals of 1 to more than 100 layers using a fundamental picosecond pulsed pump at 1.58 eV and a supercontinuum white light pulsed laser with energies ranging from…
Recent experiments and calculations in topological semimetals have observed anomalously strong second-order optical nonlinearity, but yet whether the enhancement also occurs at surfaces of topological semimetals in general remains an open…
Here we report the polarization dependent non-resonant second harmonic generation (SHG) measurement of the interfacial water molecules at the aqueous solution of the following salts: NaF, NaCl, NaBr, KF, KCl, and KBr. Through quantitative…
The surface sensitivity and probe depth in the x-ray regime of diamond for second harmonic generation (SHG) was investigated both analytically and computationally with velocity gauge real-time time-dependent density functional theory…
The dielectric permittivity of salt water decreases on dissolving more salt. For nearly a century, this phenomenon has been explained by invoking saturation in the dielectric response of the solvent water molecules. Herein, we employ an…
The spatial structure of the transition region between an insulator and an electrolyte solution was studied with x-ray scattering.The electron density profile across the n-hexane/silica sol interface (solutions with 5-nm, 7-nm, and 12-nm…
Surfaces of metal oxides at working conditions are usually electrified due to the acid-base chemistry. The charged interface compensated with counterions forms the so-called electric double layer. The coupling of surface chemistry and…
Polarized and azimuthal dependencies of optical second harmonics generation (SHG) at the surface of noncentrosymmetric semiconductor crystals have been measured on polished surfaces of ZnSe(100), using a fundamental wavelength of 1.06$\mu…
Light and heat drive interfacial chemistry at solid-liquid interfaces, underpinning processes central to sustainable energy conversion, including photoelectrochemical and hydrovoltaic systems. Yet, non-invasive probing of light-induced…
Second-harmonic generation (SHG) is a direct measure of the strength of second-order nonlinear optical effects, which also include frequency mixing and parametric oscillations. Natural and artificial materials with broken…
The forces of electrical imaging strongly polarize the surface of colloidal silica. I used X-ray scattering to study the adsorbed 2-nm-thick compact layer of alkali ions at the surface of concentrated solutions of 5-nm, 7-nm, and 22-nm…
Second harmonic generation (SHG) is a fundamental nonlinear optical phenomenon widely used both for experimental probes of materials and for application to optical devices. Even-order nonlinear optical responses including SHG generally…
We present an analytical theory of second harmonic generation (SHG) in hybrid structures combining a nonlinear 2D crystal with a dielectric metasurface waveguide. The theory describes the excitation spectrum and enhancement of SHG at both…