We report on label-free imaging, detection, and mass/size measurement of single viral particles in solution by high-resolution surface plasmon resonance microscopy. Diffraction of propagating plasmon waves along a metal surface by the viral particles creates images of the individual particles, which allow us to detect the binding of the viral particles to surfaces functionalized with and without antibodies. We show that the intensity of the particle image is related to the mass of the particle, from which we determine the mass and mass distribution of influenza viral particles with a mass detection limit of approximately 1 ag (or 0.2 fg∕mm 2 ). This work demonstrates a multiplexed method to measure the masses of individual viral particles and to study the binding activity of the viral particles.influenza virus | human cytomegalovirus | silica nanoparticles | real time detection | solution phase measurement
We demonstrated an electrochemical microscopy technique based on the detection of variations in local electrochemical current from optical signals arising from surface plasmon resonance. It enables local electrochemical measurements (such as voltammetry and amperometry) with high spatial resolution and sensitivity, because the signal varies with current density rather than current. The imaging technique is noninvasive, scanning-free, and fast, and it constitutes a powerful tool for studying heterogeneous surface reactions and for analyzing trace chemicals.
The electrocatalytic properties of nanoparticles depend on their size, shape and composition. These properties are typically probed by measuring the total electrocatalytic reaction current of a large number of nanoparticles, but this approach is time-consuming and can only measure the average catalytic activity of the nanoparticles under study. However, the identification of new catalysts requires the ability to rapidly measure the properties of nanoparticles synthesized under various conditions and, ideally, to measure the electrocatalytic activity of individual nanoparticles. Here, we show that a plasmonic-based electrochemical current-imaging technique can simultaneously image and quantify the electrocatalytic reactions of an array of 1.6 × 10(5) platinum nanoparticles printed on an electrode surface, which could facilitate high-throughput screening of the catalytic activities of nanoparticles. We also show that the approach can be used to image the electrocatalytic reaction current and measure the cyclic voltammograms of single nanoparticles.
We report an electrochemical impedance microscope (EIM) based on surface plasmon resonance. The new EIM can resolve local impedance with sub-micron spatial resolution, and monitor dynamics of various processes, such as apoptosis and electroporation of individual cells with millisecond time resolution. The high spatial and temporal resolution images make it possible to not only study individual cells, but also resolve the sub-cellular structures and processes without labels. The detection sensitivity achieved with the current setup is ~2 pS, which is excellent considering the conductance of a single ion channel is in the range of 5–400 pS. We describe also a model that simulates the EIM images of cells based on local dielectric constant and conductivity.
Metal anode instability, including dendrite growth, metal corrosion, and hetero-ions interference, occurring at the electrolyte/electrode interface of aqueous batteries, are among the most critical issues hindering their widespread use in energy storage. Herein, a universal strategy is proposed to overcome the anode instability issues by rationally designing alloyed materials, using Zn-M alloys as model systems (M = Mn and other transition metals). An in-situ optical visualization coupled with finite element analysis is utilized to mimic actual electrochemical environments analogous to the actual aqueous batteries and analyze the complex electrochemical behaviors. The Zn-Mn alloy anodes achieved stability over thousands of cycles even under harsh electrochemical conditions, including testing in seawater-based aqueous electrolytes and using a high current density of 80 mA cm−2. The proposed design strategy and the in-situ visualization protocol for the observation of dendrite growth set up a new milestone in developing durable electrodes for aqueous batteries and beyond.
We demonstrate here a surface impedance imaging technique based on sensitive dependence of surface plasmon resonance (SPR) on local surface charge density. By applying a potential modulation to a sensor surface, we are able to simultaneously obtain three images: the dc component and the amplitude and phase of the ac component. The dc image measures local molecular binding activity on the surface, as found in the conventional SPR imaging technique, and the ac images are directly related to the local impedance of the surface. Our experimental data can be analyzed quantitatively in terms of the simple free electron gas model for the sensor surface and the Randles equivalent circuit model for interfacial impedance.
Measuring electrochemical activities of nanomaterials is critical for creating novel catalysts, for developing ultrasensitive sensors, and for understanding fundamental nanoelectrochemistry. However, traditional electrochemical methods measure a large number of nanoparticles, which wash out the properties of individual nanoparticles. We report here a study of transient electrochemical oxidation of single Ag nanoparticles during collision with an electrode and voltammetry of single nanoparticles immobilized on the electrode using a plasmonic-based electrochemical current microscopy. This technique images both electrochemical reaction and size of the same individual nanoparticle, enabling quantitative examination of size-dependent electrochemical activities at single nanoparticle level. The imaging capability further allows detection of the reaction kinetics of each individual nanoparticle and analysis of the average behaviors of multiple nanoparticles. The average kinetics and size dependence can be accurately described by the Tafel equation, but there is a large variability between different nanoparticles, which underscores the importance of single nanoparticle analysis.
Surface plasmon resonance (SPR) has become an indispensable tool for label-free detection and quantification of molecular binding. Traditionally, the principle of SPR biosensors is described with a stratified medium model, in which discrete molecules are approximated with a uniform thin film. With the recent technical advances, SPR can now detect extremely low coverage of molecules, which raises the question of the validity of the traditional model. Here, we present combined theoretical, numerical and experimental analysis of SPR detection principle by considering the discrete nature of the molecules (particles). Our results show that the stratified medium model can provide reasonable description of SPR biosensors for relatively high coverage and weakly scattering samples. However, interference between the SPR images of individual particles needs to be considered for high spatial resolution images and for strong scattering samples at certain incident angles of light.
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