A hydrogen sensor based on plasmonic metasurfaces is demonstrated to exhibit the industry-required 10 s reaction time and sensitivity. It consists of a layer of either Y or WO 3 sandwiched between a top Pd nanodisk and a Au mirror at the base. The phase change layer (Y, WO 3 ) reacts with hydrogen, and the corresponding change of the refractive index (permittivity) is detected by the spectral shift of the resonance dip in reflectance at the IR spectral window. This direct reflectance readout of the permittivity change due to hydrogen uptake is fast and is facilitated by radiation field enhancement extending into the phase change volume. Numerical modeling was used to elucidate the effects that real and imaginary parts of the refractive index exert on the spectral shifts of resonance. The mechanism of sensor performance is outlined, and a possibility to tune its spectral range of operation by the diameter of the Pd nanodisk and thickness of the phase change material makes this design applicable to other molecular detection applications including surfaceenhanced IR absorption.

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Formation of metal hydrides is a signature chemical property of hydrogen and it can be leveraged to enact both storage and detection of this technologically important yet extremely volatile gas. Palladium shows particular promise as a hydrogen storage medium as well as a platform for creating rapid and reliable H 2 optical sensor devices. Furthermore, alloying Pd with other noble metals provides a technologically simple yet powerful way of enacting control over the structural and catalytic properties of the resultant material. Similarly, in addition to alloying, different top-down and bottom-up Pd nanostructuring methods have been proposed and investigated specifically for creating optical H 2 sensors. In this work it was determined that the hydrogen sensing ability of a series of Pd-Au alloy films could be improved by way of a hydrogen over exposure (HOE) treatment. Structural investigation showed that the HOE treatment, in addition to irreversibly altering the film morphology, results in a 1 to 2% expansion in the lattice constant of the metal. By combining a cyclic HOE treatment and alloy aging through annealing, the hydrogen detection sensitivity and response rates of Pd-Au films could be stabilized so that their performance would no longer be appreciably affected by repeated hydrogen uptake and release cycles. This work takes a further step towards routine all-optical detection of part-per-million level hydrogen gas concentrations in Pd-Au alloy films and discussion of ways to enhance response rates is provided.

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