Reliable Nanofabrication of Single-Crystal Diamond Photonic Nanostructures for Nanoscale Sensing.

In this manuscript, we outline a reliable procedure to manufacture photonic nanostructures from single-crystal diamond (SCD). Photonic nanostructures, in our case SCD nanopillars on thin (<1 µ m) platforms, are highly relevant for nanoscale sensing. The presented top-down procedure includes electron beam lithography (EBL) as well as reactive ion etching (RIE). Our method introduces a novel type of inter-layer, namely silicon, that significantly enhances the adhesion of hydrogen silsesquioxane (HSQ) electron beam resist to SCD and avoids sample charging during EBL. In contrast to previously used adhesion layers, our silicon layer can be removed using a highly-selective RIE step, which is not damaging HSQ mask structures. We thus refine published nanofabrication processes to ease a higher process reliability especially in the light of the advancing commercialization of SCD sensor devices.

Bulk second-harmonic generation from thermally evaporated indium selenide thin films.

We investigate bulk second-order nonlinear optical properties of amorphous indium selenide thin films fabricated by thermal evaporation. Such films are shown to exhibit strong and photostable second-harmonic generation (SHG). We report strong thickness dependence of the second-harmonic signals as characterized by the Maker-fringe method. The absolute value of the nonlinear susceptibility tensor of the film is addressed by analyzing the interference of SHG signals from the film and the glass substrate. The value of the joint non-diagonal component of the susceptibility is found to be 4 pm/V, which is comparable to that of widely used second-order nonlinear materials.

Fabrication of Ion-Shaped Anisotropic Nanoparticles and their Orientational Imaging by Second-Harmonic Generation Microscopy.

Ion beam shaping is a novel and powerful tool to engineer nanocomposites with effective three-dimensional (3D) architectures. In particular, this technique offers the possibility to precisely control the size, shape and 3D orientation of metallic nanoparticles at the nanometer scale while keeping the particle volume constant. Here, we use swift heavy ions of xenon for irradiation in order to successfully fabricate nanocomposites consisting of anisotropic gold nanoparticle that are oriented in 3D and embedded in silica matrix. Furthermore, we investigate individual nanorods using a nonlinear optical microscope based on second-harmonic generation (SHG). A tightly focused linearly or radially-polarized laser beam is used to excite nanorods with different orientations. We demonstrate high sensitivity of the SHG response for these polarizations to the orientation of the nanorods. The SHG measurements are in excellent agreement with the results of numerical modeling based on the boundary element method.

Single KTP nanocrystals as second-harmonic generation biolabels in cortical neurons.

We report an efficient colloidal synthesis of KTiOPO4 (KTP) nanocrystals with excellent crystallinity and the direct observation of optical second-harmonic generation (SHG) from discrete KTP nanocrystals in neurons cultured from mammalian brain cortex. Direct internalization and monitoring of these nanoparticles was successfully achieved without limitations from cytotoxicity, bleaching and blinking emission.

Coherent nonlinear emission from a single KTP nanoparticle with broadband femtosecond pulses.

We demonstrate that the intensity of the second harmonic (SH) generated in KTiOPO(4) nanoparticles excited with femtosecond laser pulses increases with decreasing duration of the infrared pump pulses. The SH intensity scales, approximately, as the inverse of the laser pulse duration ranging between 13 fs and 200 fs. The SH intensity enhancement requires careful compensation of the high-order spectral phase, being achieved with a genetic algorithm. Using ultrashort laser pulses improves the signal-to-noise ratio and will allow the detection of 10-nm size particles. Finally, we demonstrate that the spectrum of broadband (100 nm) pulses can be shaped to generate non-degenerate sum-frequency mixing. This opens up access to the polarization degrees of freedom of this second-order nonlinear process at the nanoscale.