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Jazlynn C. Sikes, Kevin Wonner, Aaron Nicholson, Paolo Cignoni, Ingrid Fritsch, Kristina Tschulik

• Redox magnetohydrodynamics (RMHD) microfluidics is coupled with dark-field microscopy (DFM) to offer high-throughput single-nanoparticle (NP) differentiation \(\textit {in situ}\) and \(\it operando\) in a flowing mixture by localized surface plasmon resonance (LSPR) and tracking of NPs. The color of the scattered light allows visualization of the NPs below the diffraction limit. Their Brownian motion in 1-D superimposed on and perpendicular to the RMHD trajectory yields their diffusion coefficients. LSPR and diffusion coefficients provide two orthogonal modalities for characterization where each depends on a particle’s material composition, shape, size, and interactions with the surrounding medium. RMHD coupled with DFM was demonstrated on a mixture of 82 \(\pm\) 9 nm silver and 140 \(\pm\) 10 nm gold-coated silica nanospheres. The two populations of NPs in the mixture were identified by blue/green and orange/red LSPR and their scattering intensity, respectively, and their sizes were further evaluated based on their diffusion coefficients. RMHD microfluidics facilitates high-throughput analysis by moving the sample solution across the wide field of view absent of physical vibrations within the experimental cell. The well-controlled pumping allows for a continuous, reversible, and uniform flow for precise and simultaneous NP tracking of the Brownian motion. Additionally, the amounts of nanomaterials required for the analysis are minimized due to the elimination of an inlet and outlet. Several hundred individual NPs were differentiated from each other in the mixture flowing in forward and reverse directions. The ability to immediately reverse the flow direction also facilitates re-analysis of the NPs, enabling more precise sizing.