Emerging as substantial concerns in the ecosystem, submicron plastics have attracted much attention for their considerable hazards. However, their effect and even amount in the environment remain unclear. Establishing a substantive analytic platform is essential to expand the understanding of nanoplastics. However, the issues of diffusion and detection limit that arise from ultradiluted concentration and extremely small scales of nanoplastics leave significant technical hurdles to analyze the nanoplastic pollutants. In this study, we obtain effective Raman signals in real time from underwater nanoplastics with ultralow concentrations via AC electro-osmotic flows and dielectrophoretic tweezing. This enables the field-induced active collection of nanoplastics toward the optical sensing area from remote areas in a rapid manner, integrating conventional technical skills of preconcentration, separation, and identification in a single process. A step further, synergetic combination with plasmonic nanorods, accomplishes the highest on-site detection performance so far.
Obtaining single–molecular–level fingerprints of biomolecules and electron–transfer dynamic imaging in living cells are critically demanded in postgenomic life sciences and medicine. However, the possible solution called plasmonic resonance energy transfer (PRET) spectroscopy remains challenging due to the fixed scattering spectrum of a plasmonic nanoparticle and limited multiplexing. Here, multiplexed metasurfaces‐driven PRET hyperspectral imaging, to probe biological light–matter interactions, is reported. Pixelated metasurfaces with engineered scattering spectra are first designed over the entire visible range by the precision nanoengineering of gap plasmon and grating effects of metasurface clusters. Pixelated metasurfaces are created and their full dark‐field coloration is optically characterized with visible color palettes and high‐resolution color printings of the art pieces. Furthermore, three different biomolecules (i.e., chlorophyll a, chlorophyll b, and cytochrome c) are applied on metasurfaces for color palettes to obtain selective molecular fingerprint imaging due to the unique biological light–matter interactions with application‐specific biomedical metasurfaces. This metasurface‐driven PRET hyperspectral imaging will open up a new path for multiplexed real‐time molecular sensing and imaging methods.
The assembly of metal nanoparticles and targets to be detected in a small light probe volume is essential for achieving sensitive in‐solution surface‐enhanced Raman spectroscopy (SERS). Such assemblies generally require either chemical linkers or templates to overcome the random diffusion of the colloids unless the aqueous sample is dried. Here, a facile method is reported to produce 3D multiscale assemblies of various colloids ranging from molecules and nanoparticles to microparticles for sensitive in‐solution SERS detection without chemical linkers and templates by exploiting photothermally driven convective flow. The simulations suggest that colloids sub 100 nm in diameter can be assembled by photothermally driven convective flow regardless of density; the assembly of larger colloids up to several micrometers by convective flow is significant only if their density is close to that of water. Consistent with the simulation results, the authors confirm that the photothermally driven convective flow is mainly responsible for the observed coassembly of plasmonic gold nanorods with either smaller molecules or larger microparticles. It is further found that the coassembly with the plasmonic nanoantennae leads to dramatic Raman enhancements of molecules, microplastics, and microbes by up to fivefold of magnitude compared to those measured in solution without the coassembly.
Plasmonic nanocavities have been used as a novel platform for studying strong light−matter coupling, opening access to quantum chemistry, material science, and enhanced sensing. However, the biomolecular study of cavity quantum electrodynamics (QED) is lacking. Here, we report the quantum electrodynamic behavior of chlorophyll-a in a plasmonic nanocavity. We construct an extreme plasmonic nanocavity using Au nanocages with various linker molecules and Au mirrors to obtain a strong coupling regime. Plasmon resonance energy transfer (PRET)-based hyperspectral imaging is applied to study the electrodynamic behaviors of chlorophyll-a in the nanocavity. Furthermore, we observe the energy level splitting of chlorophyll-a, similar to the cavity QED effects due to the light− matter interactions in the cavity. Our study will provide insight for further studies in quantum biological electron or energy transfer, electrodynamics, the electron transport chain of mitochondria, and energy harvesting, sensing, and conversion in both biological and biophysical systems.
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