Theoretical Design of Composite Stratified Nanohole Arrays for High-Figure-of-Merit Plasmonic Hydrogen Sensors

Fast, spark-free detection of hydrogen leaks is indispensable for large-scale hydrogen deployment, yet electronic sensors remain power-intensive and prone to cross-talk. Optical schemes based on surface plasmons enable remote read-out, but single-metal devices offer either weak H2 affinity or poor plasmonic quality. Here we employ full-wave finite-difference time-domain (FDTD) simulations to map the hydrogen response of nanohole arrays (NAs) that can be mass-produced by colloidal lithography. Square lattices of 200 nm holes etched into 100 nm films of Pd, Mg, Ti, V, or Zr expose an intrinsic trade-off: Pd maintains sharp extraordinary optical transmission modes but shifts by only 28 nm upon hydriding, whereas Mg undergoes a large dielectric transition that extinguishes its resonance. Vertical pairing of a hydride-forming layer with a noble metal plasmonic cap overcomes this limitation. A Mg/Pd bilayer preserves all modes and red-shifts by 94 nm, while the predicted optimum Ag (60 nm)/Mg (40 nm) stack delivers a 163 nm shift with an 83 nm linewidth, yielding a figure of merit of 1.96—surpassing the best plasmonic hydrogen sensors reported to date. Continuous-film geometry suppresses mechanical degradation, and the design rules—noble-metal plasmon generator, buried hydride layer, and thickness tuning—are general. This study charts a scalable route to remote, sub-ppm, optical hydrogen sensors compatible with a carbon-neutral energy infrastructure.