Alternative materials for plasmonic devices have garnered much recent interest. A promising candidate material is titanium nitride. Although there is a substantial body of work on the formation of this material, its use for plasmonic applications requires a more systematic and detailed optical analysis than has previously been carried out. This paper describes an initial optimization of sputtered TiN thin films for plasmonic performance from visible into near-IR wavelengths. The metallic behavior of TiN films exhibits a sensitive dependence on the substrate and deposition details. We explored reactive and non-reactive sputter deposition of TiN onto various substrates at both room temperature and 600°C. Metallic character was compared for films grown under different conditions via spectroscopic ellipsometry and correlated with compositional and structural measurements via x-ray photoelectron spectroscopy (XPS), x-ray diffraction (XRD), and scanning transmission electron microscopy (STEM).
Titanium nitride (TiN) is a novel refractory plasmonic material which can sustain high temperatures and exhibits large optical nonlinearities, potentially opening the door for high-power nonlinear plasmonic applications. We fabricate TiN nanoantenna arrays with plasmonic resonances tunable in the range of about 950-1050 nm by changing the antenna length. We present second-harmonic (SH) spectroscopy of TiN nanoantenna arrays, which is analyzed using a nonlinear oscillator model with a wavelength-dependent second-order response from the material itself. Furthermore, characterization of the robustness upon strong laser illumination confirms that the TiN antennas are able to endure laser irradiation with high peak intensity up to 15 GW/cm(2) without changing their optical properties and their physical appearance. They outperform gold antennas by one order of magnitude regarding laser power sustainability. Thus, TiN nanoantennas could serve as promising candidates for high-power/high-temperature applications such as coherent nonlinear converters and local heat sources on the nanoscale.
Robust plasmonic nanoantennas at mid-infrared wavelengths are essential components for a variety of nanophotonic applications ranging from thermography to energy conversion. Titanium nitride (TiN) is a promising candidate for such cases due to its high thermal stability and metallic character. Here, we employ direct laser writing as well as interference lithography to fabricate large-area nanoantenna arrays of TiN on sapphire and silicon substrates. Our lithographic tools allow for fast and homogeneous preparation of nanoantenna geometries on a polymer layer, which is then selectively transferred to TiN by subsequent argon ion beam etching followed by a chemical wet etching process. The antennas are protected by an additional Al 2 O 3 layer which allows for high-temperature annealing in argon flow without loss of the plasmonic properties. Tailoring of the TiN antenna geometry enables precise tuning of the plasmon resonances from the near to the mid-infrared spectral range. Due to the advantageous properties of TiN combined with our versatile large-area and low-cost fabrication process, such refractory nanoantennas will enable a multitude of high-temperature plasmonic applications such as thermophotovoltaics in the future.
The authors used depth-resolved cathodoluminescence spectroscopy and current-voltage measurements to probe the temperature-dependent formation of native point defects and reaction layers at metal-ZnO interfaces and their effect on transport properties. These results identify characteristic defect emissions corresponding to metal-Zn alloy versus oxide formation. Au alloys with Zn above its eutectic temperature, while Ta forms oxide blocking layers that reduce current by orders of magnitude at intermediate temperatures. Defects generated at higher temperatures and/or with higher initial defect densities for all interfaces produce Ohmic contacts. These reactions and defect formation with annealing reveal a thermodynamic control of blocking versus Ohmic contacts.
Titanium nitride (TiN) has been identified as a promising refractory material for high temperature plasmonic applications such as surface plasmon polaritons (SPPs) waveguides, lasers and light sources, and near field optics. Such SPPs are sensitive not only to the highly metallic nature of the TiN, but also to its low loss. We have formed highly metallic, low-loss TiN thin films on MgO substrates to create SPPs with resonances between 775-825 nm. Scanning near-field optical microscopy (SNOM) allowed imaging of the SPP fringes, the accurate determination of the effective wavelength of the SPP modes, and propagation lengths greater than 10 microns. Further, we show the engineering of the band structure of the plasmonic modes in TiN in the mid-IR regime and experimentally demonstrate, for the first time, the ability of TiN to support Spoof Surface Plasmon Polaritons in the mid-IR (6 microns wavelength).
The delivery of biomolecules into cells relies on porating the plasma membrane to allow exterior molecules to enter the cell via diffusion. Various established delivery methods, including electroporation and viral techniques, come with drawbacks such as low viability or immunotoxicity, respectively. An optics-based delivery method that uses laser pulses to excite plasmonic titanium nitride (TiN) micropyramids presents an opportunity to overcome these shortcomings. This laser excitation generates localized nano-scale heating effects and bubbles, which produce transient pores in the cell membrane for payload entry. TiN is a promising plasmonic material due to its high hardness and thermal stability. In this study, two designs of TiN micropyramid arrays are constructed and tested. These designs include inverted and upright pyramid structures, each coated with a 50-nm layer of TiN. Simulation software shows that the inverted and upright designs reach temperatures of 875 °C and 307 °C, respectively, upon laser irradiation. Collectively, experimental results show that these reusable designs achieve maximum cell poration efficiency greater than 80% and viability greater than 90% when delivering calcein dye to target cells. Overall, we demonstrate that TiN microstructures are strong candidates for future use in biomedical devices for intracellular delivery and regenerative medicine.
The authors used a complement of depth-resolved cathodoluminescence spectroscopy (DRCLS), atomic force microscopy (AFM), and Kelvin probe force microscopy (KPFM) to correlate the formation of native point defects with interface chemical reactions as well as surface morphology. A wide array of ZnO crystals grown by both melt and hydrothermal growth methods display orders-of-magnitude variation in 2.1, 2.5, and 3.0eV native point defect optical transitions at their free surface and as a function of depth on a nanometer scale. AFM surface morphology scans taken simultaneously with KPFM potential maps reveal large variations in surface morphology related to the growth method and subsequent processing. Notably, when DRCLS defect emissions are low, the surface roughness is low and the morphology matches its respective KPFM potential map. When DRCLS emissions vary with depth, the morphology and potential maps do not correlate. Indeed, the latter can vary by hundreds of meV across micron square areas. These subsurface electrical changes are consistent with DRCLS features and emphasize the contribution of surface morphology to electrically active interface defects. The relative strength of near band edge to deep level defect emissions exhibit a threshold dependence on surface roughness.
Van der Waals layered GeTe/Sb2Te3 chalcogenide superlattices have demonstrated outstanding performance for use in dynamic resistive memories in what is known as interfacial phase change memory devices due to their low power requirement and fast switching. These devices are made from the periodic stacking of nanometer thick crystalline layers of chalcogenide phase change materials. The mechanism for this transition is still debated, though it varies from that of traditional phase change melt-quench transition observed in singular layers of GeTe and Sb2Te3. In order to better understand the mechanism and behavior of this transition, a thorough study on each constituent layer and the parameters for growth via molecular beam epitaxy was performed. In this work, the authors show the effect of tellurium overpressure and substrate temperature on the growth of thin film GeTe and Sb2Te3 on (100) GaAs. The authors demonstrate the significant role during growth that tellurium overpressure plays in the transport properties of both GeTe and Sb2Te3, as well as the negligible impact this has on both the structural and optical properties. The highest mobility recorded was 466 cm2/V s with a p-type bulk carrier concentration of 1.5 × 1019 cm−3 in Sb2Te3. For GeTe, the highest achieved was 55 cm2/V s at a p-type bulk carrier concentration of 8.6 × 1020 cm−3. The authors discuss transport properties, orientation, and crystal structure and the parameters needed to achieve high mobility chalcogenide thin films.
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