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.

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.

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.

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.

Multiple spectroscopic insights into the interaction mechanisms between proteins and humic acid.

Proteins are important constituents of dissolved organic matter (DOM) in aqueous environments, and their interaction with humic acid (HA), another key component of DOM, substantially affects the environmental behaviors of DOM. In this work, the interaction mechanisms between tryptophan-containing proteins and HA were systematically investigated using multiple molecular spectroscopic approaches. The fluorescence quenching tests indicate that bovine serum albumin (BSA) was more readily quenched by HA and the coexisting phenolic, carboxyl, and quinone groups in HA contributed to this process significantly. By comparison, the fluorescence of L-tryptophan (L-Trp) was more stable under the same conditions. Furthermore, with multiple groups in HA, static quenching with the binding constants and the number of sites were calculated in the protein-HA and L-Trp-HA mixtures. In addition, the differential fluorescence spectra, UV‒Vis spectra, and two-dimensional correlation spectroscopy results confirmed that L-tryptophan amino acid could indeed form a complex with HA, while did not lead to fluorescence quenching. Finally, the molecular docking and density functional theory (DFT) simulations highlighted the contribution of multiple residues surrounding the HA groups to their interactions. The direct interaction between the tryptophan residue and HA might not be the prerequisite for the fluorescence response. Therefore, our work provides further insights into protein-HA interactions and implies other reasonable elucidations for further explanation.

Dynamic imaging of interfacial electrochemistry on single Ag nanowires by azimuth-modulated plasmonic scattering interferometry.

Direct visualization of surface chemical dynamics in solution is essential for understanding the mechanisms involved in nanocatalysis and electrochemistry; however, it is challenging to achieve high spatial and temporal resolution. Here, we present an azimuth-modulated plasmonic imaging technique capable of imaging dynamic interfacial changes. The method avoids strong interference from reflected light and consequently eliminates the parabolic-like interferometric patterns in the images, allowing for a 67-fold increase in the spatial resolution of plasmonic imaging. We demonstrate that this optical imaging approach enables comprehensive analyses of surface chemical dynamics and identification of previously unknown surface reaction heterogeneity by investigating electrochemical redox reactions over single silver nanowires as an example. This work provides a general strategy for high-resolution plasmonic imaging of surface electrochemical dynamics and other interfacial chemical reactions, complementing existing surface characterization methods.

Plasmonic Scattering Imaging of Surface-Bonded Nanoparticles at the Solution-Solid Interface.

Imaging nanoscale objects at interfaces is essential for revealing surface-tuned mechanisms in chemistry, physics, and life science. Plasmonic-based imaging, a label-free and surface-sensitive technique, has been widely used for studying the chemical and biological behavior of nanoscale objects at interfaces. However, direct imaging of surface-bonded nanoscale objects remains challenging due to uneven image backgrounds. Here, we present a new surface-bonded nanoscale object detection microscopy that eliminates strong background interference by reconstructing accurate scattering patterns at different positions. Our method effectively functions at low signal-to-background ratios, allowing for optical scattering detection of surface-bonded polystyrene nanoparticles and severe acute respiratory syndrome coronavirus 2 pseudovirus. It is also compatible with other imaging configurations, such as bright-field imaging. This technique complements existing methods for dynamic scattering imaging and broadens the applications of plasmonic imaging techniques for high-throughput sensing of surface-bonded nanoscale objects, enhancing our understanding of the properties, composition, and morphology of nanoparticles and surfaces at the nanoscale.

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.

One-step fluorometric determination of multiple-component dissolved organic matter in aquatic environments.

Dissolved organic matter (DOM) is ubiquitous in aqueous environments and is composed of different components that play different but important roles in the migration and the fate of pollutants, emergence of the disinfect byproduct, thus requiring quantitative characterization. However, until now, simultaneous quantification of the main contents in DOM, i.e., saccharides, proteins, and humic substances, has been difficult, impeding us from understanding and predicting the environmental behaviors of typical pollutants. In this work, a fluorescence approach based on the excitation emission matrix (EEM), combined with a new algorithm, denoted matrix reconstruction coupled with prior linear decomposition (MR-PLD), was developed to quantify multiple DOM simultaneously. First, a set of simulated water samples consisting of glucose, tryptones, and humic acid (HA) were analyzed using MR-PLD to validate the feasibility of the method. The DOM components could be reliably determined with a higher accuracy than parallel factor analysis (PARAFAC) and Parallel Factor Framework-Linear Regression (PFFLR), also with a more convenient procedure than conventional PLD. Second, both actual simulated and experimental methods were performed to test the anti-interference performance of MR-PLD, indicating that the quantification of DOM would not be significantly impacted by other fluorophores. Finally, several actual water samples from natural waters and wastewater treatment plants were also analyzed to confirm the robustness of this method in actual aqueous environments. This study provides a new approach to characterize DOM with EEM, contributing to its convenient concentration monitoring and the further exploration of the environmental impacts.

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 imaging of the layer-dependent electrocatalytic activity of two-dimensional catalysts.

Studying the localized electrocatalytic activity of heterogeneous electrocatalysts is crucial for understanding electrocatalytic reactions and further improving their performance. However, correlating the electrocatalytic activity with the microscopic structure of two-dimensional (2D) electrocatalysts remains a great challenge due to the lack of in situ imaging techniques and methods of tuning structures with atomic precision. Here, we present a general method of probing the layer-dependent electrocatalytic activity of 2D materials in situ using a plasmonic imaging technique. Unlike the existing methods, this approach was used to visualize the surface charge density and electrocatalytic activity of single 2D MoS2 nanosheets, enabling the correlation of layer-dependent electrocatalytic activity with the surface charge density of single MoS2 nanosheets. This work provides insights into the electrocatalytic mechanisms of 2D transition metal dichalcogenides, and our approach can serve as a promising platform for investigating electrocatalytic reactions at the heterogeneous interface, thus guiding the rational design of high-performance electrocatalysts.

T1 rectal mucinous adenocarcinoma with bilateral enlarged lateral lymph nodes and unilateral metastasis: A case report.

BACKGROUND: There are a few cases of lateral lymph node (LLN) metastasis (LLNM) of T1 rectal cancer. Moreover, LLNM is easily missed, especially in patients with early-stage rectal cancer. To our knowledge, the possibility of bilateral LLNM before surgery has not been reported in previous studies. CASE SUMMARY: A 36-year-old woman underwent endoscopic submucosal dissection at a local hospital owing to a clinical diagnosis of a rectal polyp. The pathology report showed a diagnosis of T1 rectal mucinous adenocarcinoma. She was considered to have bilateral LLNM after the examination at our hospital. Laparoscopic total mesorectal excision plus bilateral LLN dissection was performed and the pathological outcomes indicated unilateral LLNM. The patient received long-course adjuvant chemoradiotherapy with no recurrence or metastasis observed during the 1-year follow-up period. CONCLUSION: T1 rectal cancer could lead to LLNM and possibly, bilateral LLNM. Therefore, adequate clinical evaluation is essential for these patients.

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.

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.

Simultaneous nanocatalytic surface activation of pollutants and oxidants for highly efficient water decontamination.

Removal of organic micropollutants from water through advanced oxidation processes (AOPs) is hampered by the excessive input of energy and/or chemicals as well as the large amounts of residuals resulting from incomplete mineralization. Herein, we report a new water purification paradigm, the direct oxidative transfer process (DOTP), which enables complete, highly efficient decontamination at very low dosage of oxidants. DOTP differs fundamentally from AOPs and adsorption in its pollutant removal behavior and mechanisms. In DOTP, the nanocatalyst can interact with persulfate to activate the pollutants by lowering their reductive potential energy, which triggers a non-decomposing oxidative transfer of pollutants from the bulk solution to the nanocatalyst surface. By leveraging the activation, stabilization, and accumulation functions of the heterogeneous catalyst, the DOTP can occur spontaneously on the nanocatalyst surface to enable complete removal of pollutants. The process is found to occur for diverse pollutants, oxidants, and nanocatalysts, including various low-cost catalysts. Significantly, DOTP requires no external energy input, has low oxidant consumption, produces no residual byproducts, and performs robustly in real environmental matrices. These favorable features render DOTP an extremely promising nanotechnology platform for water purification.

Single-Particle Electrochemical Imaging Provides Insights into Silver Nanoparticle Dissolution at the Solution-Solid Interface.

Dissolution of nanoparticles is an environmental interfacial process that affects the transformation of nanoparticles. Understanding the dissolution processes of nanoparticles is important to predict their fate in the aquatic environment. However, studying nanoparticle dissolution kinetics is still challenging since dissolution is usually coupled with nanoparticle aggregation. Here, we probed the dissolution process of Ag nanoparticles at the single-particle level by surface plasmon resonance microscopy. The single-particle imaging capability enabled us to classify Ag nanoparticles, measure the dissolution dynamics of single nanoparticles, and correlate the aggregation size with oxidation activity. Moreover, we studied the dual effect of natural organic matter on the dissolution of Ag nanoparticles and validated this result with real natural freshwater. Our study provides new insights into the dissolution of Ag nanoparticles, and this technique can be extended for other nanomaterials to evaluate their fate in aquatic environments.

Notes on the genus Gryllacris Audinet-Serville (Orthoptera: Gryllacrididae) with description of a new species from China.

In this work we briefly reviewed the genus Gryllacris with some notes on taxonomic issues, note the taxa that have been described in and transferred to the genus and describe a new taxon, Gryllacris (Gryllacris) stylommatoprocera, from Yunnan, China. Materials are deposited in Shanghai Entomological Museum, Chinese Academy of Sciences.

The ATP Level in the Medial Prefrontal Cortex Regulates Depressive-like Behavior via the Medial Prefrontal Cortex-Lateral Habenula Pathway.

BACKGROUND: Depression is the most common mental illness. Mounting evidence suggests that dysregulation of extracellular ATP (adenosine triphosphate) is involved in the pathophysiology of depression. However, the cellular and neural circuit mechanisms through which ATP modulates depressive-like behavior remain elusive. METHODS: By use of ex vivo slice electrophysiology, chemogenetic manipulations, RNA interference, gene knockout, behavioral testing, and two depression mouse models, one induced by chronic social defeat stress and one caused by a IP3R2-null mutation, we systematically investigated the cellular and neural circuit mechanisms underlying ATP deficiency-induced depressive-like behavior. RESULTS: Deficiency of extracellular ATP in both defeated susceptible mice and IP3R2-null mutation mice led to reduced GABAergic (gamma-aminobutyric acidergic) inhibition and elevated excitability in lateral habenula-projecting, but not dorsal raphe-projecting, medial prefrontal cortex (mPFC) neurons. Furthermore, the P2X2 receptor in GABAergic interneurons mediated ATP modulation of lateral habenula-projecting mPFC neurons and depressive-like behavior. Remarkably, chemogenetic activation of the mPFC-lateral habenula pathway induced depressive-like behavior in C57BL/6J mice, while inhibition of this pathway was sufficient to alleviate the behavioral impairment in both defeated susceptible and IP3R2-null mutant mice. CONCLUSIONS: Overall, our study provides compelling evidence that ATP level in the mPFC is critically involved in regulating depressive-like behavior in a pathway-specific manner. These results shed new light on the mechanisms underlying depression and the antidepressant effect of ATP.

Renewable fatty acid ester production in Clostridium.

Bioproduction of renewable chemicals is considered as an urgent solution for fossil energy crisis. However, despite tremendous efforts, it is still challenging to generate microbial strains that can produce target biochemical to high levels. Here, we report an example of biosynthesis of high-value and easy-recoverable derivatives built upon natural microbial pathways, leading to improvement in bioproduction efficiency. By leveraging pathways in solventogenic clostridia for co-producing acyl-CoAs, acids and alcohols as precursors, through rational screening for host strains and enzymes, systematic metabolic engineering-including elimination of putative prophages, we develop strains that can produce 20.3 g/L butyl acetate and 1.6 g/L butyl butyrate. Techno-economic analysis results suggest the economic competitiveness of our developed bioprocess. Our principles of selecting the most appropriate host for specific bioproduction and engineering microbial chassis to produce high-value and easy-separable end products may be applicable to other bioprocesses.

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.