Plasmonic Colloidosomes as Three‐Dimensional SERS Platforms with Enhanced Surface Area for Multiphase Sub‐Microliter Toxin Sensing

Colloidosomes are robust microcapsules attractive for molecular sensing because of their characteristic micron size, large specific surface area, and dual‐phase stability. However, current colloidosome sensors are limited to qualitative fluorogenic receptor‐based detection, which restrict their applicability to a narrow range of molecules. Here, we introduce plasmonic colloidosome constructed from Ag nanocubes as an emulsion‐based 3D SERS platform. The colloidosomes exhibit excellent mechanical robustness, flexible size tunability, versatility to merge, and ultrasensitivity in SERS quantitation of food/industrial toxins down to sub‐femtomole levels. Using just 0.5 μL of sample volumes, our plasmonic colloidosomes exhibit >3000‐fold higher SERS sensitivity over conventional suspension platform. Notably, we demonstrate the first high‐throughput multiplex molecular sensing across multiple liquid phases.