High Sensitivity Plasmonic Sensing of Hydrogen over a Broad Dynamic Range Using Catalytic Au-CeO2 Thin Film Nanocomposites.

Next-generation gas-sensor technologies are needed for diverse applications including environmental surveillance, occupational safety, and industrial process control. However, the dynamic range using existing sensors is often too narrow to meet demands. In this work, plasmonic films of Au-CeO2 that detect hydrogen with 0.38% and 60% lower and upper detection limits in an oxygen-free atmosphere experiment are demonstrated. The observed 15 nm peak shift was 4 times stronger versus other plasmonic H2 sensors. The proposed sensing mechanism that involves H2 dissociation by Auδ+ nanoparticles was validated using XPS, kinetics, and Arrhenius studies. Our understanding of this remarkable sensing behavior in oxygen-free conditions opens new horizons for packaging, art conservation, industrial process control, and other applications where conventional oxygen-dependent sensors lack broad dynamic range.

Thermal energy harvesting near-infrared radiation and accessing low temperatures with plasmonic sensors.

Near-infrared (NIR) thermal energy harvesting has been demonstrated for gold nanorods (AuNRs), allowing concentration dependent, ppm-level, gas detection of H2, CO, and NO2 at 500 °C without using a white light source. Part-per-million detection capabilities of the gold nanorods are demonstrated with a factor of 11 reduction in collection times in the NIR as compared to measurements made in the visible light region. Decreased collection times are enabled by an increase in S : N ratio, which allowed a demonstration of selectivity through the use of both full spectral and a reduced spectral-based principal component analysis. Furthermore, low temperature thermal imaging spectra have been obtained at sample temperatures ranging from 275-500 °C, showing the possibility of energy harvested gas sensing at lower temperatures. These findings are promising in the area of miniaturizing plasmonic gas sensing technology and integration in areas such as gas turbines.

Thermal energy harvesting plasmonic based chemical sensors.

Detection of gases such as H2, CO, and NO2 at 500 °C or greater requires materials with thermal stability and reliability. One of the major barriers toward integration of plasmonic-based chemical sensors is the requirement of multiple components such as light sources and spectrometers. In this work, plasmonic sensing results are presented where thermal energy is harvested using lithographically patterned Au nanorods, replacing the need for an external incident light source. Gas sensing results using the harvested thermal energy are in good agreement with sensing experiments, which used an external incident light source. Principal Component Analysis (PCA) was used to reduce the wavelength parameter space from 665 variables down to 4 variables with similar levels of demonstrated selectivity. The combination of a plasmonic-based energy harvesting sensing paradigm with PCA analysis offers a novel path toward simplification and integration of plasmonic-based sensing methods.

Assessing clinical prospects of silicon quantum dots: studies in mice and monkeys.

Silicon nanocrystals can provide the outstanding imaging capabilities of toxic heavy-metal-based quantum dots without employing heavy metals and have potential for rapid progression to the clinic. Understanding the toxicity of silicon quantum dots (SiQDs) is essential to realizing this potential. However, existing studies of SiQD biocompatibility are limited, with no systematic progression from small-animal to large-animal studies that are more clinically relevant. Here, we test the response of both mice and monkeys to high intravenous doses of a nanoconstruct created using only SiQDs and FDA-approved materials. We show that (1) neither mice nor monkeys show overt signs of toxicity reflected in their behavior, body mass, or blood chemistry, even at a dose of 200 mg/kg. (2) This formulation did not biodegrade as expected. Elevated levels of silicon were present in the liver and spleen of mice three months post-treatment. (3) Histopathology three months after treatment showed adverse effects of the nanoformulation in the livers of mice, but showed no such effects in monkeys. This investigation reveals that the systemic reactions of the two animal models may have some differences and there are no signs of toxicity clearly attributable to silicon quantum dots.