High-Throughput Identification of Single Nanoparticles via Electrochemically Assisted High-Resolution Plasmonic Scattering Interferometric Microscopy.

The identification of nanoparticles within heterogeneous mixtures poses significant challenges due to the similarity in physical properties among different nanomaterials. Here, we present electrochemically assisted high-resolution plasmonic scattering interferometric microscopy (HR-PSIM). This technique allows for the high-throughput identification of nanoparticles by accurately measuring the refractive index of individual nanoparticles without interference from background signals. Through elimination of parabolic scattering interference and employing electrochemical modulation, HR-PSIM demonstrates high spatial resolution and stability against background noise, enabling the differentiation of nanoparticles with closely matched refractive indices, such as Au and Ag nanoparticles. The efficacy of this method is demonstrated through its application in real-time, label-free imaging of nanoparticle electrochemical activity, providing a platform for the precise and high-throughput characterization of nanomaterials. The robustness of our approach against electrochemical interference and its high spatial resolution mark a significant advancement in the field of nanomaterial analysis, promising wide-ranging applications in nanoparticle research and beyond.

Label-Free Optical Imaging of the Electron Transfer in Single Live Microbial Cells.

Measurement of electron transfer at the single-particle or -cell level is crucial to the in situ study of basic chemical and biological processes. However, it remains challenging to directly probe the microbial extracellular electron transfer process due to the weakness of signals and the lack of techniques. Here, we present a label-free and noninvasive imaging method that is able to measure the electron transfer in microbial cells. We measured the extracellular electron transfer processes by imaging the redox reaction of c-type outer membrane cytochromes in microbial cells using a plasmonic imaging technique, and obtained the electrochemical activity parameters (formal potential and number of electrons transferred) of multiple individual microbial cells, allowing for unveiling ample heterogeneities in electron transfer at the single-cell level. We anticipate that this method will contribute to the study of electron transfer in various biological and chemical processes.

Plasmonic Probing of Deoxyribonucleic Acid Hybridization at the Single Base Pair Resolution.

Partial DNA duplex formation greatly impacts the quality of DNA hybridization and has been extensively studied due to its significance in many biological processes. However, traditional DNA sensing methods suffer from time-consuming amplification steps and hinder the acquisition of information about single-molecule behavior. In this work, we developed a plasmonic method to probe the hybridization process at a single base pair resolution and study the relationship between the complementarity of DNA analytes and DNA hybridization behaviors. We measured single-molecule hybridization events with Au NP-modified ssDNA probes in real time and found two hybridization adsorption events: stable and transient adsorption. The ratio of these two hybridization adsorption events was correlated with the length of the complementary sequences, distinguishing DNA analytes from different complementary sequences. By using dual incident angle excitation, we recognized different single-base complementary sequences. These results demonstrated that the plasmonic method can be applied to study partial DNA hybridization behavior and has the potential to be incorporated into the identification of similar DNA sequences, providing a sensitive and quantitative tool for DNA analysis.

High-Resolution, High-Throughput Plasmonic Imaging of Nanomaterials.

Label-free imaging of nanoscale targets with intrinsic properties is crucial for chemistry, physics, and life science to unveil the underlying mechanisms. Plasmonic imaging techniques are particularly attractive because they allow real-time imaging, providing insights into nanoscale detection and nanocatalysis. Here, we present a high-resolution plasmonic imaging method that is capable of imaging nanomaterials with high morphological fidelity and high throughput. We demonstrate that this approach allows for high-resolution plasmonic imaging of various nanomaterials ranging from nanoparticles and nanowires to two-dimensional nanomaterials and accurate tracking of the interfacial dynamics of nanoparticles. Given the experimental simplicity and capacity for label-free and real-time imaging of nanomaterials with high spatial resolution and high throughput, this approach can serve as a promising platform for characterizing nanomaterials at the single-particle level.

Plasmonic probing of the adhesion strength of single microbial cells.

Probing the binding between a microbe and surface is critical for understanding biofilm formation processes, developing biosensors, and designing biomaterials, but it remains a challenge. Here, we demonstrate a method to measure the interfacial forces of bacteria attached to the surface. We tracked the intrinsic fluctuations of individual bacterial cells using an interferometric plasmonic imaging technique. Unlike the existing methods, this approach determined the potential energy profile and quantified the adhesion strength of single cells by analyzing the fluctuations. This method provides insights into biofilm formation and can also serve as a promising platform for investigating biological entity/surface interactions, such as pathogenicity, microbial cell capture and detection, and antimicrobial interface screening.

Real-Time Plasmonic Imaging of the Compositional Evolution of Single Nanoparticles in Electrochemical Reactions.

Real-time probing of the compositional evolution of single nanoparticles during an electrochemical reaction is crucial for understanding the structure-performance relationship and rationally designing nanomaterials for desirable applications; however, it is consistently challenging to achieve high-throughput real-time tracking. Here, we present an optical imaging method, termed plasmonic scattering interferometry microscopy (PSIM), which is capable of imaging the compositional evolution of single nanoparticles during an aqueous electrochemical reaction in real time. By quantifying the plasmonic scattering interferometric pattern of nanoparticles, we establish the relationship between the pattern and composition of single nanoparticles. Using PSIM, we have successfully probed the compositional transformation dynamics of multiple individual nanoparticles during electrochemical reactions. PSIM could be used as a universal platform for exploring the compositional evolution of nanomaterials at the single-nanoparticle level and offers great potentials for addressing the extensive fundamental questions in nanoscience and nanotechnology.

Optical Tracking of Surfactant-Tuned Bacterial Adhesion: a Single-Cell Imaging Study.

Probing the interfacial dynamics of single bacterial cells in complex environments is crucial for understanding the microbial biofilm formation process and developing antifouling materials, but it remains a challenge. Here, we studied single bacterial interfacial behaviors modulated by surfactants via a plasmonic imaging technique. We quantified the adhesion strength of single bacterial cells by plasmonic measurement of potential energy profiles and dissected the mechanism of surfactant-tuned single bacterial adhesion. The presence of surfactant tuned single bacterial adhesion by increasing the thickness of extracellular polymeric substances (EPS) and reducing the degree of EPS cross-linking. The adhesion kinetics and equilibrium state of bacteria attached to the surface confirmed the decrease in adhesion strength tuned by surfactants. The information obtained is valuable for understanding the interaction mechanism between a single bacterial cell and surface, developing new biofilm control strategies, and designing anticontamination materials. IMPORTANCE Studying the interfacial dynamic of single bacteria in complex environments is crucial for understanding the microbial biofilm formation process and developing antifouling materials. However, quantifying the interactions between microorganisms and surfaces in the presence of pollution at the single-cell level remains a great challenge. This paper presents the analysis of single bacterial interfacial behaviors modulated by surfactants and quantification of the adhesion strength via a plasmonic imaging technique. Our study provided insights into the mechanism of initial bacterial adhesion, facilitating our understanding of the adhesion process at the microscopic scale, and is of great value for controlling membrane fouling biofilm formation.

Label-Free Probing of Molecule Binding Kinetics Using Single-Particle Interferometric Imaging.

Probing molecular interactions is critical for screening drugs, detecting pollutants, and understanding biological processes at the molecular level, but these interactions are difficult to detect, especially for small molecules. A label-free optical imaging technology that can detect molecule binding kinetics is presented, in which free-moving particles are driven into oscillations with an alternating electrical field and the interferometric scattering patterns of the particles are imaged via an optical imaging method. By tracking the charge-sensitive variations in the oscillation amplitude with sub-nanometer precision, the small molecules and metal ions binding to the surface as well as protein-protein binding kinetics were measured. The capability of the label-free measurement of molecular interactions can provide a promising platform for screening small-molecule drugs, probing conformational changes in proteins, and detecting environmental pollutants.

Optical Tracking of the Interfacial Dynamics of Single SARS-CoV-2 Pseudoviruses.

The frequent detection of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA in healthcare environments, accommodations, and wastewater has attracted great attention to the risk of viral transmission by environmental fomites. However, the process of SARS-CoV-2 adsorption to exposed surfaces in high-risk environments remains unclear. In this study, we investigated the interfacial dynamics of single SARS-CoV-2 pseudoviruses with plasmonic imaging technology. Through the use of this technique, which has high spatial and temporal resolution, we tracked the collision of viruses at a surface and differentiated their stable adsorption and transient adsorption. We determined the effect of the electrostatic force on virus adhesion by correlating the solution and surface chemistry with the interfacial diffusion velocity and equilibrium position. Viral adsorption was found to be enhanced in real scenarios, such as in simulated saliva. This work not only describes a plasmonic imaging method to examine the interfacial dynamics of a single virus but also provides direct measurements of the factors that regulate the interfacial adsorption of SARS-CoV-2 pseudovirus. Such information is valuable for understanding virus transport and environmental transmission and even for designing anticontamination surfaces.

Rapid Assessment of Water Toxicity by Plasmonic Nanomechanical Sensing.

The ability to rapidly and accurately detect water toxicity is crucial for monitoring water quality and assessing toxic risk, but such detection remains a great challenge. Here, we present a plasmonic nanomechanical sensing (PNMS) system for the rapid assessment of water toxicity. This technique is based on the plasmonic sensing of the nanomechanical movement of single bacterial cells, which could be inhibited upon exposure to potential toxicants. By correlating the amplitude of nanomechanical movement with bacterial activity, we detected a variety of toxic substances in water. The direct readout of bacterial activity via PNMS allowed for a high sensitivity to toxicants in water, thereby enabling us to evaluate the acute toxicological effect of chemical compounds rapidly. The PNMS method is promising for online alerts of water quality safety and for assessing chemical hazards. We anticipate that PNMS is also suitable for a wide range of other applications, including bacterial detection and high-throughput screening of antibacterial materials.

Tracking Interfacial Dynamics of a Single Nanoparticle Using Plasmonic Scattering Interferometry.

The ability to track interfacial dynamics of a single nanoparticle at the solution-solid interface is crucial for understanding physical, chemical, and biological processes, but it remains a challenge. Here, we demonstrated a plasmonic imaging technique that can track unlabeled nanoparticles at the solution-solid interface with high spatial and temporal resolutions. This technique is based on particle-induced interferometric scattering of a surface plasmonic wave, which results in a high vertical sensitivity. Using this ability, we tracked the trajectories of a single nanoparticle interacting with a surface, measured the hydrodynamically hindered diffusion of nanoparticles, and revealed the surface chemistry-dependent behavior of nanoparticles at the interface. The application for tracking formation of membranes from a lipid vesicle was demonstrated, indicating the potential for investigating a broad range of nano-objects at interfaces in a complex environment.

Surface Plasmon Resonance Microscopy: From Single-Molecule Sensing to Single-Cell Imaging.

Surface plasmon resonance microscopy (SPRM) is a versatile platform for chemical and biological sensing and imaging. Great progress in exploring its applications, ranging from single-molecule sensing to single-cell imaging, has been made. In this Minireview, we introduce the principles and instrumentation of SPRM. We also summarize the broad and exciting applications of SPRM to the analysis of single entities. Finally, we discuss the challenges and limitations associated with SPRM and potential solutions.

Identification of Nanoparticles via Plasmonic Scattering Interferometry.

The development of optical imaging techniques has led to significant advancements in single-nanoparticle tracking and analysis, but these techniques are incapable of label-free selective nanoparticle recognition. A label-free plasmonic imaging technology that is able to identify different kinds of nanoparticles in water is now presented. It quantifies the plasmonic interferometric scattering patterns of nanoparticles and establishes relationships among the refractive index, particle size, and pattern both numerically and experimentally. Using this approach, metallic and metallic oxide particles with different radii were distinguished without any calibration. The ability to optically identify and size different kinds of nanoparticles can provide a promising platform for investigating nanoparticles in complex environments to facilitate nanoscience studies, such as single-nanoparticle catalysis and nanoparticle-based drug delivery.

Plasmonic-Based Electrochemical Impedance Imaging of Electrical Activities in Single Cells.

Studying electrical activities in cells, such as action potential and its propagation in neurons, requires a sensitive and non-invasive analytical tool that can image local electrical signals with high spatial and temporal resolutions. Here we report a plasmonic-based electrochemical impedance imaging technique to study transient electrical activities in single cells. The technique is based on the conversion of the electrical signal into a plasmonic signal, which is imaged optically without labels. We demonstrate imaging of the fast initiation and propagation of action potential within single neurons, and validate the imaging technique with the traditional patch clamp technique. We anticipate that the plasmonic imaging technique will contribute to the study of electrical activities in various cellular processes.

Production of human blood group B antigen epitope conjugated protein in Escherichia coli and utilization of the adsorption blood group B antibody.

BACKGROUND: In the process of ABO-incompatible (ABOi) organ transplantation, removal of anti-A and/or B antibodies from blood plasma is a promising method to overcome hyperacute rejection and allograft loss caused by the immune response between anti-A and/or B antibodies and the A and/or B antigens in the recipient. Although there are commercial columns to do this work, the application is still limited because of the high production cost. RESULTS: In this study, the PglB glycosylation pathway from Campylobacter jejuni was exploited to produce glycoprotein conjugated with Escherichia coli O86:B7 O-antigen, which bears the blood group B antigen epitope to absorb blood group B antibody in blood. The titers of blood group B antibody were reduced to a safe level without changing the clotting function of plasma after glycoprotein absorption of B antibodies in the plasma. CONCLUSIONS: We developed a feasible strategy for the specific adsorption/removal of blood group antibodies. This method will be useful in ABOi organ transplantation and universal blood transfusion.

Application of a weak magnetic field to improve microbial fuel cell performance.

Microbial fuel cells (MFCs) have emerged as a promising technology for wastewater treatment with concomitant energy production but the performance is usually limited by low microbial activities. This has spurred intensive research interest for microbial enhancement. This study demonstrated an interesting stimulation effect of a static magnetic field (MF) on sludge-inoculated MFCs and explored into the mechanisms. The implementation of a 100-mT MF accelerated the reactor startup and led to increased electricity generation. Under the MF exposure, the activation loss of the MFC was decreased, but there was no increased secretion of redox mediators. Thus, the MF effect was mainly due to enhanced bioelectrochemical activities of anodic microorganisms, which are likely attributed to the oxidative stress and magnetohydrodynamic effects under an MF exposure. This work implies that weak MF may be applied as a simple and effective approach to stimulate microbial activities for various bioelectrochemical energy production and decontamination applications.

Cathodic catalysts in bioelectrochemical systems for energy recovery from wastewater.

Bioelectrochemical systems (BESs), in which microorganisms are utilized as a self-regenerable catalyst at the anode of an electrochemical cell to directly extract electrical energy from organic matter, have been widely recognized as a promising technology for energy-efficient wastewater treatment or even for net energy generation. However, currently BES performance is constrained by poor cathode reaction kinetics. Thus, there is a strong impetus to improve the cathodic catalysis performance through proper selection and design of catalysts. This review introduces the fundamentals and current development status of various cathodic catalysts (including electrocatalysts, photoelectrocatalysts and bioelectrocatalysts) in BES, identifies their limitations and influential factors, compares their catalytic performances in terms of catalytic efficiency, stability, selectivity, etc., and discusses the possible optimization strategies and future research directions. Special focus is given on the analysis of how the catalytic performance of different catalysts can be improved by fine tuning their physicochemical or physiological properties.

Nanoscale Spatiotemporal Dynamics of Microbial Adhesion: Unveiling Stepwise Transitions with Plasmonic Imaging.

Understanding bacterial adhesion at the nanoscale is crucial for elucidating biofilm formation, enhancing biosensor performance, and designing advanced biomaterials. However, the dynamics of the critical transition from reversible to irreversible adhesion has remained elusive due to analytical constraints. Here, we probed this adhesion transition, unveiling nanoscale, step-like bacterial approaches to substrates using a plasmonic imaging technique. This method reveals the discontinuous nature of adhesion, emphasizing the complex interplay between bacterial extracellular polymeric substances (EPS) and substrates. Our findings not only deepen our understanding of bacterial adhesion but also have significant implications for the development of theoretical models for biofilm management. By elucidating these nanoscale step-like adhesion processes, our work provides avenues for the application of nanotechnology in biosensing, biofilm control, and the creation of biomimetic materials.

Microbiome-functionality in anaerobic digesters: A critical review.

Microbially driven anaerobic digestion (AD) processes are of immense interest due to their role in the biovalorization of biowastes into renewable energy resources. The function-versatile microbiome, interspecies syntrophic interactions, and trophic-level metabolic pathways are important microbial components of AD. However, the lack of a comprehensive understanding of the process hampers efforts to improve AD efficiency. This study presents a holistic review of research on the microbial and metabolic "black box" of AD processes. Recent research on microbiology, functional traits, and metabolic pathways in AD, as well as the responses of functional microbiota and metabolic capabilities to optimization strategies are reviewed. The diverse ecophysiological traits and cooperation/competition interactions of the functional guilds and the biomanipulation of microbial ecology to generate valuable products other than methane during AD are outlined. The results show that AD communities prioritize cooperation to improve functional redundancy, and the dominance of specific microbes can be explained by thermodynamics, resource allocation models, and metabolic division of labor during cross-feeding. In addition, the multi-omics approaches used to decipher the ecological principles of AD consortia are summarized in detail. Lastly, future microbial research and engineering applications of AD are proposed. This review presents an in-depth understanding of microbiome-functionality mechanisms of AD and provides critical guidance for the directional and efficient bioconversion of biowastes into methane and other valuable products.

Deep-Learning Driven, High-Precision Plasmonic Scattering Interferometry for Single-Particle Identification.

Label-free probing of the material composition of (bio)nano-objects directly in solution at the single-particle level is crucial in various fields, including colloid analysis and medical diagnostics. However, it remains challenging to decipher the constituents of heterogeneous mixtures of nano-objects with high sensitivity and resolution. Here, we present deep-learning plasmonic scattering interferometric microscopy, which is capable of identifying the composition of nanoparticles automatically with high throughput at the single-particle level. By employing deep learning to decode the quantitative relationship between the interferometric scattering patterns of nanoparticles and their intrinsic material properties, this technique is capable of high-throughput, label-free identification of diverse nanoparticle types. We demonstrate its versatility in analyzing dynamic surface chemical reactions on single nanoparticles, revealing its potential as a universal platform for nanoparticle imaging and reaction analysis. This technique not only streamlines the process of nanoparticle characterization, but also proposes a methodology for a deeper understanding of nanoscale dynamics, holding great potential for addressing extensive fundamental questions in nanoscience and nanotechnology.