Publications

We present an approach for rational design and optimization of plasmonic arrays for ultrasensitive surface enhanced infrared absorption (SEIRA) spectroscopy of specific protein analytes. Motivated by our previous work that demonstrated sub-attomole detection of surface-bound silk fibroin [Proc. Natl. Acad. Sci. U.S.A. 106, 19227 (2009)], we introduce here a general framework that allows for the numerical optimization of metamaterial sensor designs in order to maximize the absorbance signal. A critical feature of our method is the explicit compensation for the perturbative effects of the analyte's refractive index which alters the resonance frequency and line-shape of the metamaterial response, thereby leading to spectral distortion in SEIRA signatures. As an example, we leverage our method to optimize the geometry of periodic arrays of plasmonic nanoparticles on both Si and CaF2 substrates. The optimal geometries result in a three-order of magnitude absorbance enhancement compared to an unstructured Au layer, with the CaF2 substrate offering an additional factor of three enhancement in absorbance over a traditional Si substrate. The latter improvement arises from increase of near-field intensity over the Au nanobar surface for the lower index substrate. Finally, we perform sensitivity analysis for our optimized arrays to predict the effects of fabrication imperfections. We find that

Our recent work has showed that diffractively coupled nanoplasmonic arrays for Fourier transform infrared (FTIR) microspectroscopy can enhance the Amide I protein vibrational stretch by up to 105 times as compared to plain substrates. In this work we consider computationally the impact of a microscope objective illumination cone on array performance. We derive an approach for computing angular- and spatially-averaged reflectance for various numerical aperture (NA) objectives. We then use this approach to show that arrays that are perfectly optimized for normal incidence undergo significant response degradation even at modest NAs, whereas arrays that are slightly detuned from the perfect grating condition at normal incidence irradiation exhibit only a slight drop in performance when analyzed with a microscope objective. Our simulation results are in good agreement with microscope measurements of experimentally optimized periodic nanoplasmonic arrays.