A novel dual-activatable ultrasensitive chemiluminescent probe for mercury (II) monitoring: From rational design to multiple application.

Real-time optical sensing of mercury has been developed rapidly in recent years but remains challenging such as bearing background interference. Herein, a Hg2+ and base dual-activatable ultrasensitive chemiluminescent probe CL-Hg based on benzothiazole-phenoxyl-dioxetane with profits of excitation light-free and minimal interference is presented. The photophysical properties study and sensing performance verified CL-Hg is coupled with unique advantages of long-term detection (more than 400 min), ultrahigh sensitivity (LOD = 0.52 nM), and high specificity to Hg2+, and visualization detection by the paper-based test strips. More importantly, CL-Hg showed the qualitative and quantitative detection capability for Hg2+ with great recyclability in real samples of water, seafood, and beverages, holding great potential for on-site monitoring of Hg2+ levels in the actual samples. To our knowledge, this is the first work achieving the detection of Hg2+ by chemiluminescence. Overall, the Hg2+-activated visualization platform offers a practical method for detecting Hg2+ in various application scenarios.

Fidelity-oriented fluorescence imaging probes for beta-galactosidase: From accurate diagnosis to precise treatment.

Beta-galactosidase (ß-gal), a typical glycosidase catalyzing the hydrolysis of glycosidic bonds, is regarded as a vital biomarker for cell senescence and cancer occurrence. Given the advantages of high spatiotemporal resolution, high sensitivity, non-invasiveness, and being free of ionizing radiations, fluorescent imaging technology provides an excellent choice for in vivo imaging of ß-gal. In this review, we detail the representative biotech advances of fluorescence imaging probes for ß-gal bearing diverse fidelity-oriented improvements to elucidate their future potential in preclinical research and clinical application. Next, we propose the comprehensive design strategies of imaging probes for ß-gal with respect of high fidelity. Considering the systematic implementation approaches, a range of high-fidelity imaging-guided theragnostic are adopted for the individual ß-gal-associated biological scenarios. Finally, current challenges and future trends are proposed to promote the next development of imaging agents for individual and specific application scenarios.

Effect of depositional evolution on phosphorus enrichment in aquifer sediments of alluvial-lacustrine plain.

Groundwater with high geogenic phosphorus (P) is increasingly concerned as a potential risk to surface water eutrophication. Although hydrogeochemical processes responsible for P mobilization in groundwater systems have been studied, the burial characteristics of P and the effect of depositional evolution on P enrichment in aquifer sediments remain unclear. In this study, aquifer sediments were collected from the Dongting Lake Plain (DTP) within the central Yangtze River Basin, a high P groundwater area, and the effect of depositional evolution on P enrichment was elucidated by comprehensively analyzing the lithology, grain size, geochronology, and geochemistry of the sediments, coupled with groundwater chemistry and sediment incubation experiments. The results showed that the contents of total organic carbon (TOC), iron (Fe), and P (the relative content of bioavailable phosphorus (BAP)) were higher in lacustrine sediments deposited under a warm-wet climate, but lower in fluvial sediments deposited under a cold-dry climate. During depositional evolution, the sedimentary facies mainly controlled the content of organic phosphorus (OP), while the paleo-climate controlled the content of both OP and Fe-bound inorganic P (FeP), which jointly affected total P content in aquifer sediments. Under the interaction of groundwater and sediment, the reductive dissolution of P-rich Fe (oxyhydr)oxides and the mineralization of OP in sediment continuously release P into groundwater. Notably, the rapid accumulation of alluvial sediments after the Last Glacial Maximum in the DTP and rapid evolution of Dongting Lake during the Holocene led to a large amount of organic matter (OM) and P buried in sediments, providing materials for P release in aquifers, which seriously threatens groundwater quality. This exploration can provide a new understanding of the enrichment of geogenic P in groundwater from the perspective of depositional evolution.

A Rapid Nucleic Acid Visualization Assay for Infectious Bovine Rhinotracheitis Virus That Targets the TK Gene.

Infectious bovine rhinotracheitis virus (IBRV) can cause various degrees of symptoms in the respiratory system, reproductive system, and whole body of cattle. It also can lead to persistent and latent infection in cattle, posing a challenge to timely control of infectious bovine rhinotracheitis (IBR) in farms and causing large financial losses in the global cattle industry. Therefore, the goal of this study was to establish a rapid, simple, and accurate method that can detect IBRV in order to facilitate the control and eradication of IBR in cattle. We combined recombinant polymerase amplification (RPA) with a closed vertical flow visualization strip (VF) and established an RPA-VF assay that targets the thymidine kinase (TK) gene to rapidly detect IBRV. This method (reaction at 42°C for 25 min) was able to detect a minimum of 3.8 × 101 copies/µL of positive plasmid and 1.09 × 101 50% tissue culture infective dose (TCID50) of the IBRV. This assay has high specificity for IBRV and does not cross-react with other respiratory pathogens in cattle. The concordance between the RPA-VF assay and the gold standard was 100%. In addition, this assay was also suitable for the detection of DNA from clinical samples extracted by a simple method (heating at 95°C for 5 min), which can achieve the rapid detection of clinical samples in the field. Overall, the present sensitivity, specificity, and clinical applicability assessments indicated that the RPA-VF assay we developed can be utilized as a quick and accurate on-site test for IBRV detection in farms. IMPORTANCE IBRV causes different degrees of clinical symptoms in cattle and poses a great threat to the cattle industry. The infection is persistent and latent, and the elimination of IBRV in infected herds is difficult. A rapid, simple, and accurate method to detect IBRV is therefore vital to control and eradicate IBR. Combining RPA with an VF, we established an RPA-VF assay for the rapid detection of IBRV, which can complete the test of clinical samples in 35 min. The assay shows good sensitivity, specificity, and clinical applicability and can be used as an on-site test for IBRV in farms.

Characteristics and Factors Associated with Ability of Caregivers to Care for Hemodialysis Patients.

BACKGROUND The care ability of caregivers markedly impacts the patient' s quality of life and such ability may be influenced by various factors. This study aimed to explore the factors affected the care ability of caregivers for hemodialysis patients. MATERIAL AND METHODS This cross-sectional study involved 271 caregivers of hemodialysis patients. Various basic sociodemographic data of patients and caregivers were collected using questionnaires. The care abilities of caregivers were evaluated by the Caregiver Task Inventory (CTI). Univariate and multivariate linear regression analyses were used to identify the independent factors associated with the care ability of caregiver. The independent samples t test was used to further explore the impact of the independent factors on caregiver's care ability. RESULTS The mean age was 54.88±10.73 years for the patients and 44.68±15.22 years for the caregivers. Among the 271 hemodialysis patients, 59.04% were male. Multivariate regression analysis showed that female caregivers (standardized ß=-0.140, P=0.002), lived with patients (standardized ß=-0.381, P<0.001), high annual income of caregivers (standardized ß=-0.281, P<0.001), receiving caregiving training (standardized ß=-0.183, P<0.001), and patients without other chronic diseases (standardized ß=0.200, P<0.001) were associated with better care abilities of caregivers. CONCLUSIONS The gender and annual income of caregivers, receiving caregiving training, cohabitation with patient, and other concurrent chronic diseases of patients were the independent influencing factors for the care ability of caregivers for hemodialysis patients. Our study emphasized the necessity of implementing comprehensive socioeconomic and educational support to improve the care ability of caregivers.

A molecular descriptor of intramolecular noncovalent interaction for regulating optoelectronic properties of organic semiconductors.

In recent years, intramolecular noncovalent interaction has become an important means to modulate the optoelectronic performances of organic/polymeric semiconductors. However, it lacks a deep understanding and a direct quantitative relationship among the molecular geometric structure, strength of noncovalent interaction, and optoelectronic properties in organic/polymeric semiconductors. Herein, upon systematical theoretical calculations on 56 molecules with and without noncovalent interactions (X···Y, X = O, S, Se, Te; Y = C, F, O, S, Cl), we reveal the essence of the interactions and the dependence of its strength on the molecular geometry. Importantly, a descriptor S is established as a function of several basic geometric parameters to well characterize the noncovalent interaction energy, which exhibits a good inverse correlation with the reorganization energies of the photo-excited states or electron-pumped charged states in organic/polymeric semiconductors. In particular, the experimental 1H, 77Se, and 125Te NMR, the optical absorption and emission spectra, and single crystal structures of eight compounds fully confirm the theoretical predictions. This work provides a simple descriptor to characterize the strength of noncovalent intramolecular interactions, which is significant for molecular design and property prediction.

Ellagic acid from pomegranate peel: Consecutive countercurrent chromatographic separation and antioxidant effect.

Ellagic acid is one of the most representative natural antioxidants, and is rich in pomegranate peel. In this study, a consecutive countercurrent chromatographic (CCC) separation method was established to improve the preparative efficiency of ellagic acid from pomegranate peel. By optimizing the solvent system, sample size and flow rate, 280 mg of ellagic acid was obtained from 5 g of crude sample from pomegranate peel by CCC after six consecutive injections. Moreover, the values of EC50 for ellagic acid in scavenging ABTS·+ and DPPH· were 4.59 ± 0.07 and 10.54 ± 0.07 µg/ml, respectively, indicating a strong antioxidant activity. This study not only established a high-throughput method for the preparation of ellagic acid, but also provided a successful example for the development of and research on other natural antioxidants.

Modulating Triplet Excited States of Organic Semiconductors via Tuning Molecular Conformation for Dual-ratiometric Thermometers.

The dual-ratiometric thermometry is one of highly accurate methods for microscopic thermal measurement in biological systems. Herein, a series of chromone derivatives with noncovalently intramolecular interactions (NIIs) were designed and synthesized for ratiometric thermometers. The triplet states of these organic compounds were systematically tuned upon regulating the conformation with NIIs to yield efficient room temperature phosphorescence and large wavelength difference between fluorescence and phosphorescence simultaneously. As a result, an unprecedent organic 3D dual-ratiometric thermometer was established based on the intensity ratio and lifetime ratio of fluorescence/phosphorescence vs temperature, which was used for in vitro and in vivo bio-thermometry with high accuracy. This work provides a novel method to achieve organic dual ratiometric thermometers via tuning the triplet excited states.

Multiple Perspectives with Online EFL Practicum Technology Learning: Case Study on a Cloud.

This yearlong study describes multiple stakeholders' perspectives of 20 preservice English as Foreign Language (EFL) teachers, 43 elementary school students, 2 online mentors, and a teacher-researcher during a technology professional development practicum on a cloud. The case study provides qualitative and quantitative data from stakeholders concerning technology integration after participating in online project-based EFL instruction. The participating stakeholders encountered affordances and challenges that enhanced their online learning and teaching repertoires and offered nuanced evidence within this online professional development community. The findings call for continuing exploration of online practicums in preservice (language) teacher education and further research documenting complexities of multiple stakeholders' technology professional development.

TMT-based quantitative proteomic and physiological analyses on lotus plumule of artificially aged seed in long-living sacred lotus Nelumbo nucifera.

Seed longevity is important for the maintenance of seed nutritional quality, vigor, and germination potential during storage. Sacred lotus is known as one of the longest living seeds in the world and their ability to maintain longevity has been widely investigated. In this study, a suitable controlled deterioration treatment (CDT) method was first established to evaluate the vigor loss of lotus plumule (LP), and then the Tandem Mass Tags (TMT)-based proteomic analysis was performed on LP from the CDT-treated seed to quantitatively and qualitatively analyze the protein profile dynamic. In total, 4002 proteins were successfully quantified, of them, 558 differently accumulated proteins (DAPs) were identified. Protein processing and RNA-related proteins were found more easily to be affected by CDT, which may directly result in seed vigor loss. Meanwhile, CDT resulted in remarkable up-regulation of numerous proteins related to antioxidation, photosynthesis, RNA and DNA stability, starch and sucrose mobilization, and cell membrane and wall stability, which potentially played key roles in maintaining the lotus seed vigor under CDT. Histological and physiological analyses were also performed to verify some proteome results. This study provided both fundamental data and new insights to further uncover the secret of lotus seed longevity. SIGNIFICANCE: Seed aging affects the seed quality and can result in direct economic losses. The exceptional longevity of sacred lotus seed has attracted extensive attention. In this study, an optimized CDT method was used to mimic the natural aging process of sacred lotus seed, and based on TMT-based quantitative proteomic analysis on the LP profile of CDT-treated seeds, a series of differentially accumulation of specific proteins (DEPs) were revealed related to CDT resistance. Correspondingly, the physiological state and histological structure of the LP along with the CDT were detected to verify the proteome data. This study provided comprehensive information for the molecular basis of lotus seed aging analysis and facilitate to screen seed longevity related proteins for other plant species.

Breaching Bacterial Biofilm Barriers: Efficient Combinatorial Theranostics for Multidrug-Resistant Bacterial Biofilms with a Novel Penetration-Enhanced AIEgen Probe.

The formation of microbial biofilms is acknowledged as a major virulence factor in a range of persistent local infections. Failures to remove biofilms with antibiotics foster the emergence of antibiotic-resistant bacteria and result in chronic infections. As a result, the construction of effective biofilm-inhibiting and biofilm-eradicating chemicals is urgently required. Herein, we designed a water-soluble probe APDIS for membrane-active fluorescence and broad-spectrum antimicrobial actions, particularly against methicillin-resistant Staphylococcus aureus (MRSA), which shows multidrug resistance. In vitro and in vivo experiments demonstrate its high antibacterial effects comparable to vancomycin. Furthermore, it inhibits biofilm formation by effectively killing planktonic bacteria at low inhibitory concentrations, without toxicity to mammalian cells. More importantly, this probe can efficiently penetrate through biofilm barriers and exterminate bacteria that are enclosed within biofilms and startle existing biofilms. In the mouse model of implant-related biofilm infections, this probe exhibits strong antibiofilm activity against MRSA biofilms, thus providing a novel theranostic strategy to disrupt biofilms in vivo effectively. Our results indicate that this probe has the potential to be used for the development of a combinatorial theranostic platform with synergistic enhanced effects for the treatment of multidrug-resistant bacterial infections and antibiofilm medications.

High-Performance Organic Laser Semiconductor Enabling Efficient Light-Emitting Transistors and Low-Threshold Microcavity Lasers.

An organic light-emitting transistor (OLET) is a candidate device architecture for developing electrically pumped organic solid-state lasers, but it remains a critical challenge because of the lack of organic semiconductors that simultaneously possess a high solid-state emission efficiency (Φs), a high and balanced ambipolar mobility (µh,e), and a large stimulated emission cross-section. Here, we designed a molecule of 4,4'-bis(2-dibenzothiophenyl-vinyl)-biphenyl (DBTVB) and prepared its ultrathin single-crystal microplates with herringbone packing arrangements, which achieve balanced mobilities of µh = 3.55 ± 0.5 and µe = 2.37 ± 0.5 cm2 V-1 s-1, a high Φs of 85 ± 3%, and striking low-threshold laser characteristics. Theoretical and experimental investigations reveal that a strong electronic coupling and a small reorganization energy ensure efficient charge transport; meanwhile, the exciton-vibration effect and negligible π-π orbital overlap give rise to highly emissive H-aggregates and facilitate laser emission. Furthermore, OLET-based DBTVB crystals offer an internal quantum efficiency approaching 100% and a record-high electroluminescence external quantum efficiency of 4.03%.

Mesityl-Functionalized Multi-Resonance Organoboron Delayed Fluorescent Frameworks with Wide-Range Color Tunability for Narrowband OLEDs.

Polycyclo-heteraborin multi-resonance (MR) emitters are promising for high color-purity organic light-emitting diodes (OLEDs). Here, unlike the most common heteroatom ternary-doped (X/B/N) frameworks, a binary-doped (B/N) skeleton is reported with a large energy band for wide-range color tunability. Based on this parent-segment, a "one-pot" catalyst-free borylation method is developed which generates deep blue to pure green MR emitters from readily available starting materials, with peaks at 426-532 nm and full-width-at-half-maxima of 27-38 nm. Impressively, a maximum external quantum efficiency of nearly 40 % is recorded for the corresponding device with Commission Internationale de l'Eclairage coordinates of (0.14, 0.16), representing the state-of-the-art performances. This work presents a new paradigm and synthesis of B/N-doped MR emitters and will motivate the study of other novel frameworks.

Excitation-Wavelength-Dependent Organic Long-Persistent Luminescence Originating from Excited-State Long-Range Proton Transfer.

Stimuli-responsive functional luminescent materials with tunable color and long-persistent emission have emerged as a powerful tool in information encryption, anticounterfeiting, and bioelectronics. Herein, we prove a novel strategy for manipulating the proton transfer pathways in the salicylaldehyde derivative EQCN solutions/powder to produce excitation wavelength-dependent (Ex-De) performances with switchable emissions (blue-sky, green, and orange). The experiments and theoretical results demonstrated that the different luminous colors are originated from enol (E) form (blue-sky), Keto-1 (K1) form (orange) through the excited-state intramolecular proton transfer (ESIPT) process, and Keto-2 (K2) form (green) through the excited-state long-range proton transfer (ESLRPT) process. We leverage synergistic effects between the dopant and matrix (dimethyl terephthalate, DTT) to manipulate the excited-state proton transfer pathway in EQCN@DTT mixture powders to generate Ex-De long-persistent luminescence (Ex-De-LPL), which can be well applied in multilevel information encryption. This strategy not only paves an intriguing way for the construction and preparation of pure organic Ex-De materials but also offers a guideline for developing LPL materials based on ESLRPT processes.

Extending the π-Skeleton of Multi-Resonance TADF Materials towards High-Efficiency Narrowband Deep-Blue Emission.

Multi-resonance TADF (MR-TADF) emitters are promising for high-resolution OLEDs, but the concurrent optimization of excited-state dynamics and color purity remains a tough challenge. Herein, three deep-blue MR-TADF compounds (BN1-BN3) featuring gradually enlarged ring-fused structures and increased rigidity are accessed by lithium-free borylation in high yields from the same precursor, with all the emitters possessing CIEy coordinates below 0.08. Structure-property investigations demonstrate a strategic improvement of the oscillator strength (fosc ) and acceleration of the reverse intersystem crossing (RISC) process by extending the π-skeleton, where BN3 realizes a maximum external quantum efficiency (EQE) of 37.6 % and reduced roll-off, thus showing the best efficiency reported for deep-blue TADF OLEDs. The internal regulation of the efficiency and color purity of these compounds validate the general effectiveness to achieve advanced deep-blue narrowband emitters with higher-order boron/nitrogen-based MR motifs.

Preclinical detection of lysophosphatidic acid: A new window for ovarian cancer diagnostics.

Ovarian cancer, a highly metastatic disease characterized by widespread peritoneal and ascites dissemination, is the leading cause of death from gynecological malignancies and poses a serious threat to women's lives. Biomarkers detection for the early diagnosis is crucial to ameliorate the dismal survival rate. Currently, there is much interest in lysophosphatidic acid (LPA), with evidences shown that the elevated LPA level in plasma could serve as an effective biomarker for ovarian cancer. Thus the mastery of LPA measurement techniques is conducive to providing a new diagnostic or prognostic platform for ovarian cancer. In this tutorial review, with a brief discussion on the sample pre-treatment protocols, we summarize various methods for LPA detection with emphasis on the advances in universal mass spectrometry-based technologies and emerging optical sensor strategies. Meanwhile, other methods such as enzymatic method, capillary electrophoresis, dot immunogold filtration assay and bioassay are also included. Eventually, we outlook the potential clinical value of LPA detection, and anticipate the future improvements of these methodologies to make them truly useful for ovarian cancer diagnosis.

Profile-based intensity and frequency corrections for single-snapshot spatial frequency domain imaging.

We have proposed the profile-based intensity and frequency corrections for single-snapshot spatial frequency domain (SFD) imaging to mitigate surface profile effects on the measured intensity and spatial frequency in extracting the optical properties. In the scheme, the spatially modulated frequency of the projected sinusoidal pattern is adaptively adjusted according to the sample surface profile, reducing distortions of the modulation amplitude in the single-snapshot demodulation and errors in the optical property extraction. The profile effects on both the measured intensities of light incident onto and reflected from the sample are then compensated using Minnaert's correction to obtain the true diffuse reflectance of the sample. We have validated the method by phantom experiments using a highly sensitive SFD imaging system based on the single-pixel photon-counting detection and assessed error reductions in extracting the absorption and reduced scattering coefficients by an average of 40% and 10%, respectively. Further, an in vivo topography experiment of the opisthenar vessels has demonstrated its clinical feasibility.

Organic Nanoparticles-Assisted Low-Power STED Nanoscopy.

Stimulated emission depletion (STED) nanoscopy plays a key role in achieving sub-50 nm high spatial resolution for subcellular live-cell imaging. To avoid re-excitation, the STED wavelength has to be tuned at the red tail of the emission spectrum of fluorescent probes, leading to high depletion laser power that might damage the cell viability and functionality. Herein, with the highly emissive silica-coated core-shell organic nanoparticles (CSONPs) enabling a giant Stokes shift of 150 nm, ultralow power STED is achieved by shifting the STED wavelength to the emission maximum at 660 nm. The stimulated emission cross section is increased by ∼20-fold compared to that at the emission red tail. The measured saturation intensity and lateral resolution of our CSONP are 0.0085 MW cm-2 and 25 nm, respectively. More importantly, long-term (>3 min) dynamic super-resolution imaging of the lysosomal fusion-fission processes in living cells is performed with a resolution of 37 nm.

Molecular Design Strategy for Simultaneously Strong Luminescence and High Mobility: Multichannel CH-π Interaction.

It is a big challenge to achieve high-performance organic semiconductor materials integrating both high luminescence efficiency and carrier mobility, because they are commonly regarded as a pair of contradiction. Here, combining a tight-binding model and density functional theory/time-dependent density functional theory, we propose a theoretical protocol to characterize the luminescence efficiency via an excitonic effective mass and charge transport ability via charge effective mass at the same level. Applying this protocol to a series of organic semiconductor materials, we find that the multichannel CH-π interaction can induce a heavy excitonic effective mass and light charge effective mass, which effectively balance the light-emitting efficiency and carrier mobility. Thus, a practical molecular design strategy is figured out to exploit novel organic semiconductor materials with strong luminescence and fast carrier transport simultaneously.