Harnessing Brightness in Naphthalene Diimides Maniam, Subashani; Higginbotham, Heather F.; Bell, Toby D. M. ...
Chemistry : a European journal,
May 23, 2019, Volume:
25, Issue:
29
Journal Article
Peer reviewed
The development of brightly emissive compounds is of great research and commercial interest, with established and emerging applications across chemistry, biology, physics, medicine and engineering. ...Among the many types of molecules available, naphthalene diimides have been widely used for both fundamental photophysical studies and in practical applications that utilise fluorescence as an information readout. The monomeric naphthalene diimide is weakly fluorescent, however through various methods of core‐derivatisation, it can be developed to be highly fluorescent and further functionalised to add utility. In this review, we highlight recent advances made in naphthalene diimide chemistry that have led to development of molecules with improved optical properties, and the design strategies utilised to produce bright fluorescence emission as small molecules or in supramolecular architectures.
Bright idea: Naphthalene diimides have attracted great scientific interest for their remarkable photophysical and optical tunability. Several key strategies to harness molecular brightness via core‐substitution, shoulder conjugation, self‐assembly and induced transformation approaches are discussed.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
The heart develops from 2 sources of mesoderm progenitors, the first and second heart field (FHF and SHF). Using a single-cell transcriptomic assay combined with genetic lineage tracing and live ...imaging, we find the FHF and SHF are subdivided into distinct pools of progenitors in gastrulating mouse embryos at earlier stages than previously thought. Each subpopulation has a distinct origin in the primitive streak. The first progenitors to leave the primitive streak contribute to the left ventricle, shortly after right ventricle progenitor emigrate, followed by the outflow tract and atrial progenitors. Moreover, a subset of atrial progenitors are gradually incorporated in posterior locations of the FHF. Although cells allocated to the outflow tract and atrium leave the primitive streak at a similar stage, they arise from different regions. Outflow tract cells originate from distal locations in the primitive streak while atrial progenitors are positioned more proximally. Moreover, single-cell RNA sequencing demonstrates that the primitive streak cells contributing to the ventricles have a distinct molecular signature from those forming the outflow tract and atrium. We conclude that cardiac progenitors are prepatterned within the primitive streak and this prefigures their allocation to distinct anatomical structures of the heart. Together, our data provide a new molecular and spatial map of mammalian cardiac progenitors that will support future studies of heart development, function, and disease.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
There is increasing interest in individual differences in animal behaviour. Recent research now suggests that an individual's behaviour, once considered to be plastic, may be more predictable than ...previously thought. Here, we take advantage of the large number of studies that have estimated the repeatability of various behaviours to evaluate whether there is good evidence for consistent individual differences in behaviour and to answer some outstanding questions about possible factors that can influence repeatability. Specifically, we use meta-analysis to ask whether different types of behaviours were more repeatable than others, and if repeatability estimates depended on taxa, sex, age, field versus laboratory, the number of measures and the interval between measures. Some of the overall patterns that were revealed by this analysis were that repeatability estimates were higher in the field compared to the laboratory and repeatability was higher when the interval between observations was short. Mate preference behaviour was one of the best studied but least repeatable behaviours. Our findings prompt new insights into the relative flexibility of different types of behaviour and offer suggestions for the design and analysis of future research.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Per- and polyfluoroalkyl substances (PFAS) are used for their properties such as stain and water resistance. The substances have been associated with adverse health outcomes in both pregnant mothers ...and infants, including pre-eclampsia and low birthweight. A growing body of research suggests that PFAS are transferred from mother to fetus through the placenta, leading to in utero exposure. A systematic review was performed using the PubMed database to search for studies evaluating determinants of PFAS concentrations in blood matrices of pregnant mothers and neonates shortly after birth. Studies were included in this review if an observational study design was utilized, exposure to at least one PFAS analyte was measured, PFAS were measured in maternal or neonatal matrices, at least one determinant of PFAS concentrations was assessed, and results such as beta estimates were provided. We identified 35 studies for inclusion in the review and evaluated the PFAS and determinant relationships among the factors collected in these studies. Parity, breastfeeding history, maternal race and country of origin, and household income had the strongest and most consistent evidence to support their roles as determinants of certain PFAS concentrations in pregnant mothers. Reported study findings on smoking status, alcohol consumption, and pre-pregnancy body mass index (BMI) suggest that these factors are not important determinants of PFAS concentrations in pregnant mothers or neonates. Further study into informative factors such as consumer product use, detailed dietary information, and consumed water sources as potential determinants of maternal or neonatal PFAS concentrations is needed. Research on determinants of maternal or neonatal PFAS concentrations is critical to estimate past PFAS exposure, build improved exposure models, and further our understanding on dose-response relationships, which can influence epidemiological studies and risk assessment evaluations. Given the potential for adverse outcomes in pregnant mothers and neonates exposed to PFAS, it is important to identify and understand determinants of maternal and neonatal PFAS concentrations to better implement public health interventions in these populations.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Interest in the application of biochar (charcoal produced during the pyrolysis of biomass) to agricultural land is increasing across the world, recognised as a potential way to capture and store ...atmospheric carbon. Its interest is heightened by its potential co-benefits for soil quality and fertility. The majority of research has however been undertaken in tropical rather than temperate regions. This study assessed the potential for lump-wood charcoal addition (as a substitute for biochar) to soil types which are typically under arable and forest land-use in North East England. The study was undertaken over a 28
week period and found:
i)
No significant difference in net ecosystem respiration (NER) between soils containing charcoal and those without, other than in week 1 of the trial.
ii)
A significantly higher dissolved organic carbon (DOC) flux from soils containing large amounts of charcoal than from those untreated, when planted with ryegrass.
iii)
That when increased respiration or DOC loss did occur, neither was sufficiently large to alter the carbon sink benefits of charcoal application.
iv)
That charcoal incorporation resulted in a significantly lower nitrate flux in soil leachate from mineral soils.
v)
That charcoal incorporation caused significant increases in soil pH, from 6.98 to 7.22 on bare arable soils when 87,500
kg charcoal/ha was applied.
Consideration of both the carbon sink and environmental benefits observed here suggests that charcoal application to temperate soils typical of North East England should be considered as a method of carbon sequestration. Before large scale land application is encouraged, further large scale trials should be undertaken to confirm the positive results of this research.
► Charcoal was incorporated into mineral and organo-mineral soils in NE England. ► No significant difference in NER was observed other than in week 1 of the trial. ► Higher DOC was lost from vegetated soils containing large amounts of charcoal. ► Charcoal incorporation resulted in a significantly lower nitrate flux in soil leachate. ► Increased NER and DOC did not offset the C sink benefits of charcoal application.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Gut mucosal barrier breakdown and inflammation have been associated with high levels of flagellin, the principal bacterial flagellar protein. Although several gut commensals can produce flagella, ...flagellin levels are low in the healthy gut, suggesting the existence of control mechanisms. We find that mice lacking the flagellin receptor Toll-like receptor 5 (TLR5) exhibit a profound loss of flagellin-specific immunoglobulins (Igs) despite higher total Ig levels in the gut. Ribotyping of IgA-coated cecal microbiota showed Proteobacteria evading antibody coating in the TLR5−/− gut. A diversity of microbiome members overexpressed flagellar genes in the TLR5−/− host. Proteobacteria and Firmicutes penetrated small intestinal villi, and flagellated bacteria breached the colonic mucosal barrier. In vitro, flagellin-specific Ig inhibited bacterial motility and downregulated flagellar gene expression. Thus, innate-immunity-directed development of flagellin-specific adaptive immune responses can modulate the microbiome’s production of flagella in a three-way interaction that helps to maintain mucosal barrier integrity and homeostasis.
•TLR5−/− mice have reduced levels of anti-flagellin antibodies in the gut•Flagella-related genes of commensal microbes are upregulated in TLR5−/− mouse guts•Antibodies against flagellin induce downregulation of flagella genes•Flagellated bacteria penetrate TLR5−/− small intestinal villi and mucosal barrier
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The habitability of the surface of any planet is determined by a complex evolution of its interior, surface, and atmosphere. The electromagnetic and particle radiation of stars drive thermal, ...chemical, and physical alteration of planetary atmospheres, including escape. Many known extrasolar planets experience vastly different stellar environments than those in our solar system: It is crucial to understand the broad range of processes that lead to atmospheric escape and evolution under a wide range of conditions if we are to assess the habitability of worlds around other stars. One problem encountered between the planetary and the astrophysics communities is a lack of common language for describing escape processes. Each community has customary approximations that may be questioned by the other, such as the hypothesis of H‐dominated thermosphere for astrophysicists or the Sun‐like nature of the stars for planetary scientists. Since exoplanets are becoming one of the main targets for the detection of life, a common set of definitions and hypotheses are required. We review the different escape mechanisms proposed for the evolution of planetary and exoplanetary atmospheres. We propose a common definition for the different escape mechanisms, and we show the important parameters to take into account when evaluating the escape at a planet in time. We show that the paradigm of the magnetic field as an atmospheric shield should be changed and that recent work on the history of Xenon in Earth's atmosphere gives an elegant explanation to its enrichment in heavier isotopes: the so‐called Xenon paradox.
Plain Language Summary
In addition to having the right surface temperature, a planet needs an atmosphere to keep surface liquid water stable. Although many planets have been found that may lie in the right temperature range, the existence of an atmosphere is not guaranteed. In particular, for planets that are kept warm by being close to dim stars, there are a number of ways that the star may remove a planetary atmosphere. These atmospheric escape processes depend on the behavior of the star as well as the nature of the planet, including the presence of a planetary magnetic field. Under certain conditions, a magnetic field can protect a planet's atmosphere from the loss due to the direct impact of the stellar wind, but it may actually enhance total atmospheric loss by connecting to the highly variable magnetic field of the stellar wind. These enhancements happen especially for planets close to dim stars. We review the complete range of atmospheric loss processes driven by interaction between a planet and a star to aid in the identification of planets that are both the correct temperature for liquid water and that have a chance of maintaining an atmosphere over long periods of time.
Key Points
The different escape processes at planets and exoplanets are reviewed along with their mathematical formulation
The major parameters for each escape processes are described; some escape processes negligible in the solar system may be major source at exoplanets, or for the early solar system
A magnetic field should not be a priori considered as a protection for the atmosphere
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
To assess the safety of intra-articular (IA) autologous tolerogenic dendritic cells (tolDC) in patients with inflammatory arthritis and an inflamed knee; to assess the feasibility and acceptability ...of the approach and to assess potential effects on local and systemic disease activities.
An unblinded, randomised, controlled, dose escalation Phase I trial. TolDC were differentiated from CD14+ monocytes and loaded with autologous synovial fluid as a source of autoantigens. Cohorts of three participants received 1×10
, 3×10
or 10×10
tolDC arthroscopically following saline irrigation of an inflamed (target) knee. Control participants received saline irrigation only. Primary outcome was flare of disease in the target knee within 5 days of treatment. Feasibility was assessed by successful tolDC manufacture and acceptability via patient questionnaire. Potential effects on disease activity were assessed by arthroscopic synovitis score, disease activity score (DAS)28 and Health Assessment Questionnaire (HAQ). Immunomodulatory effects were sought in peripheral blood.
There were no target knee flares within 5 days of treatment. At day 14, arthroscopic synovitis was present in all participants except for one who received 10×10
tolDC; a further participant in this cohort declined day 14 arthroscopy because symptoms had remitted; both remained stable throughout 91 days of observation. There were no trends in DAS28 or HAQ score or consistent immunomodulatory effects in peripheral blood. 9 of 10 manufactured products met quality control release criteria; acceptability of the protocol by participants was high.
IA tolDC therapy appears safe, feasible and acceptable. Knee symptoms stabilised in two patients who received 10×10
tolDC but no systemic clinical or immunomodulatory effects were detectable.
NCT01352858.
Intense demand for water in the Central Valley of California and related increases in groundwater nitrate concentration threaten the sustainability of the groundwater resource. To assess ...contamination risk in the region, we developed a hybrid, non-linear, machine learning model within a statistical learning framework to predict nitrate contamination of groundwater to depths of approximately 500m below ground surface. A database of 145 predictor variables representing well characteristics, historical and current field and landscape-scale nitrogen mass balances, historical and current land use, oxidation/reduction conditions, groundwater flow, climate, soil characteristics, depth to groundwater, and groundwater age were assigned to over 6000 private supply and public supply wells measured previously for nitrate and located throughout the study area. The boosted regression tree (BRT) method was used to screen and rank variables to predict nitrate concentration at the depths of domestic and public well supplies. The novel approach included as predictor variables outputs from existing physically based models of the Central Valley. The top five most important predictor variables included two oxidation/reduction variables (probability of manganese concentration to exceed 50ppb and probability of dissolved oxygen concentration to be below 0.5ppm), field-scale adjusted unsaturated zone nitrogen input for the 1975 time period, average difference between precipitation and evapotranspiration during the years 1971–2000, and 1992 total landscape nitrogen input. Twenty-five variables were selected for the final model for log-transformed nitrate. In general, increasing probability of anoxic conditions and increasing precipitation relative to potential evapotranspiration had a corresponding decrease in nitrate concentration predictions. Conversely, increasing 1975 unsaturated zone nitrogen leaching flux and 1992 total landscape nitrogen input had an increasing relative impact on nitrate predictions. Three-dimensional visualization indicates that nitrate predictions depend on the probability of anoxic conditions and other factors, and that nitrate predictions generally decreased with increasing groundwater age.
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•Boosted regression tree model produced 3D map of nitrate concentration.•Hybrid multi-modeling approach used numerical model outputs as predictors.•Redox characteristics and field scale unsaturated zone N flux were most important.•Nitrate concentrations <2mg/L NO3-N generally conformed to basin subregion.•Nitrate concentrations >10mg/L NO3-N most common in eastern alluvial fans subregion
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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