Wavelength-multiplexed hook nanoantennas for machine learning enabled mid-infrared spectroscopy

Infrared spectroscopy with plasmonic nanoantennas is limited by small overlap between molecules and hot spots, and sharp resonance peaks. The authors demonstrate spectral multiplexing of hook nanoantennas with gradient dimensions as ultrasensitive vibrational probes in a continuous ultra-broadband region and utilize machine learning for enhanced sensing performance. Infrared (IR) plasmonic nanoantennas (PNAs) are powerful tools to identify molecules by the IR fingerprint absorption from plasmon-molecules interaction. However, the sensitivity and bandwidth of PNAs are limited by the small overlap between molecules and sensing hotspots and the sharp plasmonic resonance peaks. In addition to intuitive methods like enhancement of electric field of PNAs and enrichment of molecules on PNAs surfaces, we propose a loss engineering method to optimize damping rate by reducing radiative loss using hook nanoantennas (HNAs). Furthermore, with the spectral multiplexing of the HNAs from gradient dimension, the wavelength-multiplexed HNAs (WMHNAs) serve as ultrasensitive vibrational probes in a continuous ultra-broadband region (wavelengths from 6 mu m to 9 mu m). Leveraging the multi-dimensional features captured by WMHNA, we develop a machine learning method to extract complementary physical and chemical information from molecules. The proof-of-concept demonstration of molecular recognition from mixed alcohols (methanol, ethanol, and isopropanol) shows 100% identification accuracy from the microfluidic integrated WMHNAs. Our work brings another degree of freedom to optimize PNAs towards small-volume, real-time, label-free molecular recognition from various species in low concentrations for chemical and biological diagnostics.

Automated summary

This article introduces a spectral multiplexing method using hook nanoantennas for infrared spectroscopy, which can achieve ultrasensitive vibrational probes in a continuous ultra-broadband region and utilize machine learning for enhanced sensing performance. By optimizing the damping rate and reducing radiative loss, the sensitivity and bandwidth of the hook nanoantennas are improved. The gradient dimension of the hook nanoantennas enables wavelength-multiplexing and serves as ultrasensitive vibrational probes, and machine learning is used to extract complementary information from molecules.