Ultrasensitive Molecular Detection at Subpicomolar Concentrations by the Diffraction Pattern Imaging with Plasmonic Metasurfaces and Convex Holographic Gratings

Compact and cost‐effective optical devices for highly sensitive detection of trace molecules are significant in many applications, including healthcare, pollutant monitoring and explosive detection. Nanophotonic metasurface‐based sensors have been intensively attracting attentions for molecular detection. However, conventional methods often involve spectroscopic characterizations that require bulky, expensive and sophisticated spectrometers. Here, a novel ultrasensitive sensor of plasmonic metasurfaces is designed and fabricated for the detection of trace molecules. The sensor features a convex holographic grating, of which the first‐order diffraction pattern of a disposable metasurface is recorded by a monochrome camera.The diffraction pattern changes with the molecules attached to the metasurface, realizing label‐free and spectrometer‐free molecular detection by imaging and analyzing of the diffraction pattern. By integrating the sensor with a microfluidic setup, the quantitative characterization of rabbit anti‐human Immunoglobulin G (IgG) and human IgG biomolecular interactions is demonstrated with an excellent limit of detection (LOD) of 0.6 pm. Moreover, both the metasurface and holographic grating are obtained through vacuum‐free solution‐processed fabrications, minimizing the manufacturing cost of the sensor. A prototype of the imaging‐based sensor, consisting of a white light‐emitting diode (LED) and a consumer‐level imaging sensor is achieved to demonstrate the potential for on‐site detection. A novel imaging‐based molecular detection platform is reported that integrates solution‐processed disposable metasurfaces with convex holographic gratings for trace amounts of molecule detection. The limit of detection (LOD) for the human Immunoglobulin G (IgG)IgG/anti‐IgG immune complex formation assay of the proposed sensor is 0.6 pm. This image‐based detection method is expected to be a promising technique for point‐of‐care and on‐site detection.