Computational Discovery of Intermolecular Singlet Fission Materials Using Many-Body Perturbation Theory.

Intermolecular singlet fission (SF) is the conversion of a photogenerated singlet exciton into two triplet excitons residing on different molecules. SF has the potential to enhance the conversion efficiency of solar cells by harvesting two charge carriers from one high-energy photon, whose surplus energy would otherwise be lost to heat. The development of commercial SF-augmented modules is hindered by the limited selection of molecular crystals that exhibit intermolecular SF in the solid state. Computational exploration may accelerate the discovery of new SF materials. The GW approximation and Bethe-Salpeter equation (GW+BSE) within the framework of many-body perturbation theory is the current state-of-the-art method for calculating the excited-state properties of molecular crystals with periodic boundary conditions. In this Review, we discuss the usage of GW+BSE to assess candidate SF materials as well as its combination with low-cost physical or machine learned models in materials discovery workflows. We demonstrate three successful strategies for the discovery of new SF materials: (i) functionalization of known materials to tune their properties, (ii) finding potential polymorphs with improved crystal packing, and (iii) exploring new classes of materials. In addition, three new candidate SF materials are proposed here, which have not been published previously.

A copper-catalyzed asymmetric Friedel-Crafts hydroxyalkylation of pyrazole-4,5-diones with 5-aminoisoxazoles.

An asymmetric Friedel-Crafts hydroxyalkylation reaction of 5-aminoisoxazoles with pyrazole-4,5-diones was developed under the catalysis of 5% chiral copper complexes. This reaction exhibits functional group tolerance and excellent enantioselectivity. Moreover, the reaction can be scaled up and its mechanism was studied.

A comprehensive evaluation of risk factors for mortality, infection and colonization associated with CRGNB in adult solid organ transplant recipients: a systematic review and meta-analysis.

BACKGROUND: The burden of carbapenem-resistant gram-negative bacteria (CRGNB) among solid organ transplant (SOT) recipients has not been systematically explored. Here, we discern the risk factors associated with CRGNB infection and colonization in SOT recipients. METHODS: This study included observational studies conducted among CRGNB-infected SOT patients, which reported risk factors associated with mortality, infection or colonization. Relevant records will be searched in PubMed, Embase and Web of Science for the period from the time of database construction to 1 March 2023. RESULTS: A total of 23 studies with 13,511 participants were included, enabling the assessment of 27 potential risk factors. The pooled prevalence of 1-year mortality among SOT recipients with CRGNB was 44.5%. Prolonged mechanical ventilation, combined transplantation, reoperation and pre-transplantation CRGNB colonization are salient contributors to the occurrence of CRGNB infections in SOT recipients. Renal replacement therapy, post-LT CRGNB colonization, pre-LT liver disease and model for end-stage liver disease score increased the risk of infection. Re-transplantation, carbapenem use before transplantation and ureteral stent utilization increaesd risk of CRGNB colonization. CONCLUSION: Our study demonstrated that SOT recipients with CRGNB infections had a higher mortality risk. Invasive procedure may be the main factor contribute to CRGNB infection.

Fully integrated and automated centrifugal microfluidic chip for point-of-care multiplexed molecular diagnostics.

Public health events caused by pathogens have imposed significant economic and societal burdens. However, conventional methods still face challenges including complex operations, the need for trained operators, and sophisticated instruments. Here, we proposed a fully integrated and automated centrifugal microfluidic chip, also termed IACMC, for point-of-care multiplexed molecular diagnostics by harnessing the advantages of active and passive valves. The IACMC incorporates multiple essential components including a pneumatic balance module for sequential release of multiple reagents, a pneumatic centrifugation-assisted module for on-demand solution release, an on-chip silicon membrane module for nucleic acid extraction, a Coriolis force-mediated fluid switching module, and an amplification module. Numerical simulation and visual validation were employed to iterate and optimize the chip's structure. Upon sample loading, the chip automatically executes the entire process of bacterial sample lysis, nucleic acid capture, elution quantification, and isothermal LAMP amplification. By optimizing crucial parameters including centrifugation speed, direction of rotation, and silicone membrane thickness, the chip achieves exceptional sensitivity (twenty-five Salmonella or forty Escherichia coli) and specificity in detecting Escherichia coli and Salmonella within 40 min. The development of IACMC will drive advancements in centrifugal microfluidics for point-of-care testing and holds potential for broader applications in precision medicine including high-throughput biochemical analysis immune diagnostics, and drug susceptibility testing.

Rosmarinic Acid Liposomes Downregulate Hepcidin Expression via BMP6-SMAD1/5/8 Pathway in Mice with Iron Overload.

The objective of this study is to examine the potential protective effect of rosmarinic acid (RosA) encapsulated within nanoliposomes (RosA-LIP) on hepatic damage induced by iron overload. The characteristics, stability, and release of RosA-LIP in vitro were identified. The mice were randomly assigned to five groups: Control, Model, Model+DFO (DFO), Model+RosA (RosA), and Model+RosA-LIP (RosA-LIP). The iron overload model was induced by administering iron dextran (i.p.). The DFO, RosA, and RosA-LIP groups received iron dextran and were subsequently treated with DFO, RosA, and RosA-LIP for 14 days. We developed a novel formulation of RosA-LIP that exhibited stability and controlled release properties. Firstly, RosA-LIP improved liver function and ameliorated pathological changes in a mouse model of iron overload. Secondly, RosA-LIP demonstrated the ability to enhance the activities of T-SOD, GSH-Px, and CAT, while reducing the levels of MDA and 4-HNE, thereby effectively mitigating oxidative stress damage induced by iron overload. Thirdly, RosA-LIP reduced hepatic iron levels by downregulating FTL, FTH, and TfR1 levels. Additionally, RosA-LIP exerted a suppressive effect on hepcidin expression through the BMP6-SMAD1/5/8 signaling pathway. Furthermore, RosA-LIP upregulated FPN1 expression in both the liver and duodenum, thereby alleviating iron accumulation in these organs in mice with iron overload. Notably, RosA exhibited a comparable iron chelation effect, and RosA-LIP demonstrated superior efficacy in mitigating liver damage induced by excessive iron overload. RosA-LIP exhibited favorable sustained release properties, targeted delivery, and efficient protection against iron overload-induced liver damage. A schematic representation of the proposed protective mechanism of rosmarinic acid liposome during iron overload. Once RosA-LIP is transported into cells, RosA is released. On the one hand, RosA attenuates the BMP6-SMAD1/5/8-SMAD4 signaling pathway activation, leading to inhibiting hepcidin transcription. Then, the declined hepcidin contacted the inhibitory effect of FPN1 in hepatocytes and duodenum, increasing iron mobilization. On the other hand, RosA inhibits TfR1 and ferritin expression, which decreases excessive iron and oxidative damage.

Rectal culture could predict carbapenem-resistant organism bloodstream infection and reduce the mortality in haematological patients: A retrospective cohort study.

OBJECTIVES: The objective is to explore the correlation between rectal swab culture and the overall 30-d survival of hematologic patients diagnosed with carbapenem-resistant organism (CRO) bloodstream infection. METHODS: A total of 434 haematological patients who were complicated with Gram-negative bacilli (GNB) bloodstream infections (BSIs) caused by Gram-negative bacteria between January 2020 and December 2021 were included in our retrospective study. Based on their drug susceptibility results, we classified patients into CRO BSIs and non-CRO BSIs cases. Through group comparison, to uncover the correlation between the positive screening of rectal swabs and reducing the mortality of CRO BSI in patients with haematological diseases. RESULTS: Among the 434 cases of Gram-negative bacteria bloodstream infection, 96 were identified as carbapenem-resistant bloodstream infection, which consisted of 57 cases of carbapenem-resistant Klebsiella pneumoniae (CR-KP), 19 cases of carbapenem-resistant Pseudomonas aeruginosa (CR-PA), 11 cases of carbapenem-resistant Escherichia coli (CR-CO), 5 cases of carbapenem-resistant Acinetobacter baumannii (CR-AB), and 4 cases of other Enterobacteriaceae. Before the onset of CRO bloodstream infection, rectal swab cultures were conducted on 36 patients, and the positive result rate was 75.0% (27/36), with 20 cases of CR-KP, 6 cases of CR-CO, and one case of carbapenem-resistant Enterobacter cloacae. It was observed that the rectal and blood cultures had matching outcomes in 75.0% of cases. The mortality rate within 30 d for CRO BSIs was 53.1% (51/96), while for carbapenem-resistant Enterobacteriaceae (CRE) BSIs it was 62.5% (45/72). Univariate analysis showed that 30-d mortality was significantly reduced when there were positive rectal culture results preceding bloodstream infection (P < 0.001), as well as preemptive anti-infection treatment (P < 0.001). Multivariate analysis demonstrated that preemptive adjustment to an effective antibiotic regimen, guided by positive rectal culture results, had a significant effect on decreasing 30-d mortality following CRO BSIs (P= 0.002). Furthermore, for the management of CRE BSIs, antibiotic treatments utilising ceftazidime/avibactam (CAV/AVI) may be more beneficial compared to those that use tigecycline (TGC) or polymyxin (PMB). CONCLUSION: CRO BSI, especially CRE BSI, can be life-threatening for those with haematological diseases. Utilising rectal culture can effectively identify CRO strains with high sensitivity and specificity. Adjusting antibiotic treatment based on the preemptive positive rectal culture results may significantly decrease 30-d mortality rates for haematological patients with CRO BSIs.

Reconstruction of degraded image transmitting through ocean turbulence via deep learning.

When a laser carrying image information is transmitted in seawater, the presence of ocean turbulence leads to significant degradation of the received information due to the effect of interference. To address this issue, we propose a deep-learning-based method to retrieve the original information from a degraded pattern. To simulate the propagation of laser beams in ocean turbulence, a model of an ocean turbulence phase screen based on the power spectrum inversion method is used. The degraded images with different turbulence conditions are produced based on the model. A Pix2Pix network architecture is built to acquire the original image information. The results indicate that the network can realize high-fidelity image recovery under various turbulence conditions based on the degraded patterns. However, as turbulence strength and transmission distance increase, the reconstruction accuracy of the Pix2Pix network decreases. To further improve the image reconstruction ability of neural network architectures, we established three networks (U-Net, Pix2Pix, and Deep-Pix2Pix) and compared their performance in retrieving the degraded patterns. Overall, the Pix2Pix network showed the best performance for image reconstruction.

Effects of cattle on vector-borne disease risk to humans: A systematic review.

Vector-borne pathogens (VBPs) causing vector-borne diseases (VBDs) can circulate among humans, domestic animals, and wildlife, with cattle in particular serving as an important source of exposure risk to humans. The close associations between humans and cattle can facilitate the transmission of numerous VBPs, impacting public health and economic security. Published studies demonstrate that cattle can influence human exposure risk positively, negatively, or have no effect. There is a critical need to synthesize the information in the scientific literature on this subject, in order to illuminate the various ecological mechanisms that can affect VBP exposure risk in humans. Therefore, the aim of this systematic review was to review the scientific literature, provide a synthesis of the possible effects of cattle on VBP risk to humans, and propose future directions for research. This study was performed according to the PRISMA 2020 extension guidelines for systematic review. After screening 470 peer-reviewed articles published between 1999-2019 using the databases Web of Science Core Collection, PubMed Central, CABI Global Health, and Google Scholar, and utilizing forward and backward search techniques, we identified 127 papers that met inclusion criteria. Results of the systematic review indicate that cattle can be beneficial or harmful to human health with respect to VBDs depending on vector and pathogen ecology and livestock management practices. Cattle can increase risk of exposure to infections spread by tsetse flies and ticks, followed by sandflies and mosquitoes, through a variety of mechanisms. However, cattle can have a protective effect when the vector prefers to feed on cattle instead of humans and when chemical control measures (e.g., acaricides/insecticides), semio-chemicals, and other integrated vector control measures are utilized in the community. We highlight that further research is needed to determine ways in which these mechanisms may be exploited to reduce VBD risk in humans.

On-Line Dual-Active Valves Based Centrifugal Microfluidic Chip for Fully Automated Point-of-Care Immunoassay.

There remains an unmet need for a fully integrated microfluidic platform that can automatically perform multistep and multireagent immunoassays. Here, we proposed a novel online dual-active valve-based centrifugal microfluidic chip, termed DAVM, for fully automatic point-of-care immunoassay. Practically, the puncture valve, one of the dual active valves, is capable of achieving precise, on-demand, sequential release of prestored reagents, while the other valve-reversible active valve enables controlled retention and drainage of the reaction solutions. Thereby, our technology mitigates the challenges of hydrophilic/hydrophobic modifications and unstable valve control performance commonly observed in passive valve controls. As a proof of concept, the indirect enzymatic immunoblotting technique was employed on DAVM for fully automated immunological analysis of eight targets, yielding outcomes within an hour. Furthermore, we conducted a comparative analysis of 28 clinical samples with autoimmune diseases. According to 224 clinical data, the sample testing concordance rate between DAVM and the traditional instrument was 82%, with a target compliance rate of 97%. Therefore, our DAVM system has powerful potential for fully automated immunoassays.

Construction of chiral N,O-hemiaminals via a copper-catalyzed enantioselective Michael/N-hemiacetalization cascade reaction.

An efficient Michael/N-hemiacetalization cascade reaction of 5-aminoisoxazoles with ß,γ-unsaturated α-ketoesters was developed under the catalysis of a chiral copper complex. A series of optically pure six-membered ring N,O-hemiaminals were obtained with excellent yields (up to 96% yield) and high enantioselectivities (up to 98% ee). The possible transition state was supported by DFT calculations and thereby the corresponding mechanism was proposed.

Inverse Design of Tetracene Polymorphs with Enhanced Singlet Fission Performance by Property-Based Genetic Algorithm Optimization.

The efficiency of solar cells may be improved by using singlet fission (SF), in which one singlet exciton splits into two triplet excitons. SF occurs in molecular crystals. A molecule may crystallize in more than one form, a phenomenon known as polymorphism. Crystal structure may affect SF performance. In the common form of tetracene, SF is experimentally known to be slightly endoergic. A second, metastable polymorph of tetracene has been found to exhibit better SF performance. Here, we conduct inverse design of the crystal packing of tetracene using a genetic algorithm (GA) with a fitness function tailored to simultaneously optimize the SF rate and the lattice energy. The property-based GA successfully generates more structures predicted to have higher SF rates and provides insight into packing motifs associated with improved SF performance. We find a putative polymorph predicted to have superior SF performance to the two forms of tetracene, whose structures have been determined experimentally. The putative structure has a lattice energy within 1.5 kJ/mol of the most stable common form of tetracene.

True molecular conformation and structure determination by three-dimensional electron diffraction of PAH by-products potentially useful for electronic applications.

The true molecular conformation and the crystal structure of benzo[e]dinaphtho[2,3-a;1',2',3',4'-ghi]fluoranthene, 7,14-diphenylnaphtho[1,2,3,4-cde]bisanthene and 7,16-diphenylnaphtho[1,2,3,4-cde]helianthrene were determined ab initio by 3D electron diffraction. All three molecules are remarkable polycyclic aromatic hydrocarbons. The molecular conformation of two of these compounds could not be determined via classical spectroscopic methods due to the large size of the molecule and the occurrence of multiple and reciprocally connected aromatic rings. The molecular structure of the third molecule was previously considered provisional. These compounds were isolated as by-products in the synthesis of similar products and were at the same time nanocrystalline and available only in very limited amounts. 3D electron diffraction data, taken from submicrometric single crystals, allowed for direct ab initio structure solution and the unbiased determination of the internal molecular conformation. Detailed synthetic routes and spectroscopic analyses are also discussed. Based on many-body perturbation theory simulations, benzo[e]dinaphtho[2,3-a;1',2',3',4'-ghi]fluoranthene may be a promising candidate for triplet-triplet annihilation and 7,14-diphenylnaphtho[1,2,3,4-cde]bisanthene may be a promising candidate for intermolecular singlet fission in the solid state.

A self-administered moxibustion-cum-massage intervention for older adults with chronic pain in the community: A randomized controlled trial.

OBJECTIVES: To determine the effectiveness of a simple, self-administrable moxibustion-cum-massage intervention for relieving chronic pain and improving psychological well-being for older adults in the community. DESIGN: A randomized controlled trial. SETTING: Seventy-eight participants with chronic pain were randomly assigned to the intervention and waitlist control groups. INTERVENTIONS: Participants received two moxa sticks a day to use the moxibustion-cum-massage procedure with the help of trained volunteers or caregivers for five consecutive days. MAIN OUTCOME MEASURES: Participates' pain level, sleep quality, depression and subjective well-being were measured before the intervention (T0), immediately after the intervention (T1), and one week after the intervention (T2). RESULTS: Repeated measures ANOVA revealed a significant group × time interaction effect in subjective well-being with a medium effect size. Regarding within-group effects in the intervention group at post-intervention (T1), the subjective pain level was significantly reduced with a small effect size, while sleep quality and depression significantly improved with large effect sizes. The control group showed no significant within-group effects in these variables. Maintenance effects at follow-up (T2) were not significant. CONCLUSION: Despite the short intervention timeframe of five days, the study revealed preliminary evidence that the moxibustion-cum-massage intervention can be an effective, self-administrable pain relief regime for older adults. A longer period of intervention time is suggested for future studies.

Fatal Rickettsia Japonica Infection Complicating Disseminated Intravascular Coagulation in Yichang, China.

Background: Severe complications may cause a fatal or disabling outcome in patients with Rickettsia japonica infection but are poorly understood. Methods: We identified 11 patients with only Rickettsia japonica infection with metagenomics next generation sequencing (mNGS) during April to November 2021 at Yichang Central People's Hospital, China. Clinical data were obtained through review of medical records. Results: Most patients realized that they had symptoms about one or two days after being bitten. Fever (91%), pulmonary effusion (91%), rash or erythema (100%), abnormal urine (100%), neutropenia (100%), lymphopenia (100%), and thrombocytopenia (100%) were the most common clinical signs. Six severely ill patients were admitted to the intensive care unit and five had mild symptoms. Systemic manifestations such as vomiting (83%), neurological manifestations (100%), and disseminated intravascular coagulation (100%) were more frequently observed in the severe cases, 33.3% of whom developed purpura fulminans requiring amputation or skin graft, and 16.6% died two days after admission. Some patients experienced sequelae. Conclusion: Our study found that patients with critical Rickettsia japonica infection complicating disseminated intravascular coagulation had high risk of poor outcome.

A Meta-Analysis of How Nonalcoholic Fatty Liver Disease Affect Antiviral Treatment of Patients with e Antigen-Positive Chronic Hepatitis B.

Background: Nonalcoholic fatty liver disease (NAFLD) and chronic hepatitis B (CHB) are both the most common underlying diseases leading to cirrhosis and hepatocellular carcinoma, and NAFLD and HBV infection are the first and second leading causes of chronic liver disease in China. However, there are still a lot of controversies about whether the combined presence of CHB and NAFLD will affect the course or outcome of liver disease together with HBV, and how the two affect each other. Objective: To investigate the effect of nonalcoholic fatty liver disease (NAFLD) on antiviral therapy in patients with chronic hepatitis B (CHB). Methods: Computer searches of databases such as PubMed, CNKI, VIP.com, and Wanfang Data Knowledge Service Platform were used. The time frame was from the creation of the database to June 2022. The search subject terms were hepatitis B, CHB, or NAFLD. The observation group consisted of patients with e antigen-positive CHB with NAFLD, and the control group consisted of patients with e-antigen + CHB. Extracts including title, name, date of publication, number of samples, antiviral drugs, and outcome indicators were used for Meta-analysis. Funnel plots were drawn to analyze literature bias. Results: Seven papers including 1348 patients with HBeAg + CHB (observation group: n = 547, control group: n = 801) were finally included. Results: Seven papers including 1348 patients with HBeAg + CHB (observation group: n = 547, control group: n = 801) were finally included. Results. Meta-analysis showed that CHB patients with NAFLD had lower efficacy than CHB patients after 48 weeks of antiviral treatment with nucleotide analogs, as measured by three outcome indicators HBV DNA conversion rate, ALT-normalization, and HBeAg conversion rate. Conclusion: NAFLD reduces the effect of antiviral therapy in CHB patients, and the clinicopathological features of patients with NAFLD combined with chronic hepatitis B are different from those of patients with chronic hepatitis B alone, so early diagnosis by liver histological examination should be actively performed and reasonable antiviral therapy should be administered.

Parametarhizium hingganense, a Novel Ectomycorrhizal Fungal Species, Promotes the Growth of Mung Beans and Enhances Resistance to Disease Induced by Rhizoctonia solani.

The mutualistic interactions between mycorrhizae and plants first occurred along with the terrestrialization of plants. The majority of vascular plants are in symbiosis with mycorrhizal fungi. Due to their importance to the economy and ecology, arbuscular mycorrhizal (AM) and ectomycorrhizal (ECM) fungi emerge as the most popular ones. However, the mechanism underlying the beneficial function of ECM fungi is not as clear as AM fungi. Here, the interaction between Parametarhizium hingganense, a novel fungal species isolated from forest litter, and mung bean (Vigna radiata) was studied. P. hingganense demonstrated P solubilization ability in vitro. Treatment of P. hingganense on the seeds resulted in promoted growth with enhanced P content. The hyphae of green fluorescence protein (GFP)-tagged P. hingganense were found to surround the roots and develop between cells, suggesting the establishment of an ectomycorrhizal symbiosis. Upon symbiosis with P. hingganense, the levels of jasmonic acid (JA) and gibberellin (GA1) and total phenolic and flavonoid content elevated. Meanwhile, damping off caused by Rhizoctonia solani in mycorrhizal plants was alleviated. Taken together, the above findings suggested that symbiosis with P. hingganense conferred growth promotion and priming of defense responses to host plants which should be associated with facilitated P uptake and increased JA and GA1 levels.

Tetraphenylethylene sulfonate derivative as turn-on fluorescent sensor for berberine chloride detection in aqueous solution.

A negatively-charged tetraphenylethylene derivative (TPE-SE) was designed and synthesized as turn-on fluorescent sensor for berberine chloride (BBC) detection in aqueous solution. The fluorescent property and detection mechanism were elucidated by UV-vis absorption spectra, photoluminescence spectra, dynamic light scattering experiments. The results reveal that the BBC can lead to aggregation-induced emission of TPE-SE due to the electrostatic interactions, endowing TPE-SE with excellent turn-on detecting ability, high selectivity and sensitivity to BBC. The detection limit is as low as 6.58 × 10-6M. These results should be applicable to fabricate special turn-on fluorescent sensors towards various antibiotics, and it is crucially important for achieving reasonable control and intake of small biomolecules.

Survey of High Expressed Emotions Experienced By Community Mental Health Service Users in Hong Kong During the COVID-19 Pandemic.

Background: High expressed emotion (EE) experienced by people with mental illness is a known risk factor of relapse. With drastically increased time spent at home and limited health and social service provision during the COVID-19 pandemic, patients' experience of high EE warranted attention. Aims and Methods: The study aimed to investigate the experience of high EE among people with mental illness during the COVID-19 pandemic. We surveyed the service users of 2 community mental health centers, including participants with psychotic and nonpsychotic disorders. Results: Valid responses from 303 participants indicated an overall high EE prevalence of 71.62%, much higher than previous findings, which range between 30% and 40%. People with other psychotic and nonpsychotic disorders showed a higher probability of experiencing high EE than people with schizophrenia. Participants reported a higher probability of experiencing high EE as a result of caregiving by other family relatives and friends than by parents. Conclusion: Findings suggest a significantly elevated high EE prevalence among people suffering from mental illness in the community during the COVID-19 pandemic. It is worth further evaluating the long-term effects of high EE beyond the pandemic.

Effects of Acute Moderate- and High-Intensity Aerobic Exercise on Oxygenation in Prefrontal Cortex of Male Methamphetamine-Dependent Patients.

The aim of this study was to explore the influence of different intensities of acute aerobic exercise on brain activation in male methamphetamine (MA)-dependent patients during exercise. Twenty MA-dependent patients were divided randomly into two groups participating in 35 min of either moderate- or high-intensity aerobic exercise. Functional near-infrared spectral imaging (fNIRS) was used to detect hemodynamic changes in prefrontal cortex during the main 25-min exercise stage. The results revealed that high-intensity acute aerobic exercise aroused more cerebral oxygenation changes in the prefrontal cortex and left dorsolateral prefrontal cortex during exercise as compared with moderate-intensity exercise. Furthermore, there was a stronger positive connection observed between orbital frontal cortex and left dorsolateral prefrontal cortex in the high-intensity group than in the moderate-intensity group. Together these results suggest that for submaximal exercise intensities, high-intensity exercise may bring more benefits to male MA-dependent patients than moderate-intensity.