Related papers: A New Imaginary Term in the 2nd Order Nonlinear Su…
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…
We explore by means of modeling how absorptive-dispersive mixing between the second- and third-order terms modify the imaginary chi(2)total responses from air/water interfaces under conditions of varying charge densities and ionic strength.…
Using Time Independent Density Functional Theory (TIDFT) it is shown that the 2nd order optical susceptibilities of narrow (1nm-2nm) Silicon Nanowires (SiNW) are enhanced due to surface termination. The value of $\chi^{(2)}$ is enhanced up…
Probing the polarization of water molecules at charged interfaces by second harmonic generation spectroscopy has been heretofore limited to isotropic materials. Here, we report non-resonant nonlinear optical measurements at the interface of…
Second harmonic generation (SHG) spectroscopy has been applied to probe the fused silica/water interface at pH 7 and the uncharged 11bar02 sapphire/water interface at pH 5.2 in contact with aqueous solutions of NaCl, NaBr, NaI, KCl, RbCl,…
Second-order nonlinear spectroscopy has proven to be a powerful tool in elucidating key chemical and structural characteristics at a variety of interfaces. However, the presence of interfacial potentials may lead to complications regarding…
The second order para-ferromagnetic phase transition in a series of amorphous alloys (Fe{_5}Co{_{50}}Ni{_{17-x}}Cr{_x}B{_{16}}Si{_{12}}) is investigated using nonlinear susceptibility. A simple molecular field treatment for the critical…
Second harmonic generation amplitude and phase measurements are acquired in real time from fused silica:water interfaces that are subjected to ionic strength transitions conducted at pH 5.8. In conjunction with atomistic modeling, we…
Optical nonlinear processes are indispensable in a wide range of applications including ultrafast laser sources, microscopy, metrology, and quantum information technologies. Combinations of the diverse nonlinear processes should further…
A possibility of tuning the phase of the third-order Kerr-type nonlinear susceptibility in a system consisting of two interacting metal nanospheres and a nonlinearly polarizable molecule is investigated theoretically and numerically. It is…
Implicit summation is a technique for the conversion of sums over intermediate states in multiphoton absorption and the high-order susceptibility in hydrogen into simple integrals. Here, we derive the equivalent technique for hydrogenic…
We compute from first principles the infrared dispersion of the nonlinear susceptibility $\chi^{(2)}$ in zincblende semiconductors. At terahertz frequencies the nonlinear susceptibility depends not only on the purely electronic response…
We present experimental results on the observation of a bulk second-order nonlinear susceptibility derived from both free-space and integrated measurements in silicon nitride. Phase-matching is achieved through dispersion engineering of the…
The recent, rapid advances in nonlinear chipscale nanophotonics in the visible and near-infrared have been largely driven by manipulating the local dielectric environment proximate to decades-old workhorse bulk nonlinear optical materials,…
State-of-the-art experiments employ strong ultrafast optical fields to study the nonlinear response of electrons in solids on an attosecond time-scale. Notably, a recent experiment retrieved a 3rd order nonlinear susceptibility by comparing…
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…
We report second- and third-harmonic generation in monolayer MoS$_\mathrm{2}$ as a tool for imaging and accurately characterizing the material's nonlinear optical properties under 1560 nm excitation. Using a surface nonlinear optics…
The interface between two different semiconductors is crucial in determining the electronic properties at the heterojunction, therefore novel techniques that can probe these regions are of particular interest. Recently it has been shown…
We report about the experimental observation and characterization of nonlinear optical properties of individual silicon nanowires of different dimensions. Our results show that the nonlinear light has different components, one of them…
We develop and verify a phase-sensitive second harmonic generation spectroscopic scheme that allows for direct determination of the absolute surface charge density and surface potential of a water interface without need of prior interfacial…