Dual-Gradient Plasmonic qBIC Metasurface for Time-Resolved In Situ Optimization of Molecular Vibrational Sensing in Water

Abstract

Metaphotonic platforms based on quasi-bound states in the continuum (qBICs), harnessing strong near-field enhancement and deeply subwavelength field confinement, provide a versatile framework for surface-enhanced infrared absorption (SEIRA) spectroscopy. However, real-time molecular sensing in water using qBIC metasurfaces remains challenging. First, strong water absorption in the mid-infrared region damps qBICs and obscures weak analyte signals. Second, conventional metasurfaces rely on discrete arrays targeting individual wavelengths and coupling conditions, increasing the device footprint and fabrication effort required to match the qBIC to the molecular vibrational resonance. Here, we present a dual-gradient plasmonic qBIC metasurface with diamond-shaped resonators for in situ molecular vibrational sensing in water, where spatially encoded gradients in the scaling factor and asymmetry parameter independently control the qBIC spectral positions and radiative rates, respectively, across a 1000 um x 700 um footprint. Building on this capability, we experimentally monitor lipid vesicle dynamics in real time and resolve the carbonyl vibrational signature despite the unavoidable water absorption. We then directly identify the optimal sensing condition and track its evolution across the spatially encoded parameter space. The results establish a compact single-chip strategy that combines adsorption-kinetics monitoring, vibrational fingerprint detection, and on-chip optimization, opening opportunities for investigating biological dynamics under aqueous conditions.