Soot Superaggregates from Flaming Wildfires and Their Direct Radiative Forcing

Wildfires contribute significantly to global soot emissions, yet their aerosol formation mechanisms and resulting particle properties are poorly understood and parameterized in climate models. The conventional view holds that soot is formed via the cluster-dilute aggregation mechanism in wildfires and emitted as aggregates with fractal dimension D(sub f) approximately equals 1.8 mobility diameter D(sub m) (is) less than or equal to 1 micron, and aerodynamic diameter D(sub a) (is) less than or equal to 300 nm. Here we report the ubiquitous presence of soot superaggregates (SAs) in the outflow from a major wildfire in India. SAs are porous, low-density aggregates of cluster-dilute aggregates with characteristic D(sub f) approximately equals 2.6,D(sub m) (is) greater than 1 micron, and D(sub a) is less than or equal to 300 nm that form via the cluster-dense aggregation mechanism.We present additional observations of soot SAs in wildfire smoke-laden air masses over Northern California, New Mexico, and Mexico City. We estimate that SAs contribute, per unit optical depth, up to 35% less atmospheric warming than freshly-emitted (D(sub f) approximately equals 1.8) aggregates, and approximately equals 90% more warming than the volume-equivalent spherical soot particles simulated in climate models

Trapping and aerogelation of nanoparticles in negative gravity hydrocarbon flames

We report the experimental realization of continuous carbon aerogel production using a flame aerosol reactor by operating it in negative gravity (−g; up-side-down configuration). Buoyancy opposes the fuel and air flow forces in −g, which eliminates convectional outflow of nanoparticles from the flame and traps them in a distinctive non-tipping, flicker-free, cylindrical flame body, where they grow to millimeter-size aerogel particles and gravitationally fall out. Computational fluid dynamics simulations show that a closed-loop recirculation zone is set up in −g flames, which reduces the time to gel for nanoparticles by ≈10[superscript 6] s, compared to positive gravity (upward rising) flames. Our results open up new possibilities of one-step gas-phase synthesis of a wide variety of aerogels on an industrial scale

Interacting networks of resistance, virulence and core machinery genes identified by genome-wide epistasis analysis.

Recent advances in the scale and diversity of population genomic datasets for bacteria now provide the potential for genome-wide patterns of co-evolution to be studied at the resolution of individual bases. Here we describe a new statistical method, genomeDCA, which uses recent advances in computational structural biology to identify the polymorphic loci under the strongest co-evolutionary pressures. We apply genomeDCA to two large population data sets representing the major human pathogens Streptococcus pneumoniae (pneumococcus) and Streptococcus pyogenes (group A Streptococcus). For pneumococcus we identified 5,199 putative epistatic interactions between 1,936 sites. Over three-quarters of the links were between sites within the pbp2x, pbp1a and pbp2b genes, the sequences of which are critical in determining non-susceptibility to beta-lactam antibiotics. A network-based analysis found these genes were also coupled to that encoding dihydrofolate reductase, changes to which underlie trimethoprim resistance. Distinct from these antibiotic resistance genes, a large network component of 384 protein coding sequences encompassed many genes critical in basic cellular functions, while another distinct component included genes associated with virulence. The group A Streptococcus (GAS) data set population represents a clonal population with relatively little genetic variation and a high level of linkage disequilibrium across the genome. Despite this, we were able to pinpoint two RNA pseudouridine synthases, which were each strongly linked to a separate set of loci across the chromosome, representing biologically plausible targets of co-selection. The population genomic analysis method applied here identifies statistically significantly co-evolving locus pairs, potentially arising from fitness selection interdependence reflecting underlying protein-protein interactions, or genes whose product activities contribute to the same phenotype. This discovery approach greatly enhances the future potential of epistasis analysis for systems biology, and can complement genome-wide association studies as a means of formulating hypotheses for targeted experimental work

Horizontal DNA transfer mechanisms of bacteria as weapons of intragenomic conflict

Horizontal DNA transfer (HDT) is a pervasive mechanism of diversification in many microbial species, but its primary evolutionary role remains controversial. Much recent research has emphasised the adaptive benefit of acquiring novel DNA, but here we argue instead that intragenomic conflict provides a coherent framework for understanding the evolutionary origins of HDT. To test this hypothesis, we developed a mathematical model of a clonally descended bacterial population undergoing HDT through transmission of mobile genetic elements (MGEs) and genetic transformation. Including the known bias of transformation toward the acquisition of shorter alleles into the model suggested it could be an effective means of counteracting the spread of MGEs. Both constitutive and transient competence for transformation were found to provide an effective defence against parasitic MGEs; transient competence could also be effective at permitting the selective spread of MGEs conferring a benefit on their host bacterium. The coordination of transient competence with cell-cell killing, observed in multiple species, was found to result in synergistic blocking of MGE transmission through releasing genomic DNA for homologous recombination while simultaneously reducing horizontal MGE spread by lowering the local cell density. To evaluate the feasibility of the functions suggested by the modelling analysis, we analysed genomic data from longitudinal sampling of individuals carrying Streptococcus pneumoniae. This revealed the frequent within-host coexistence of clonally descended cells that differed in their MGE infection status, a necessary condition for the proposed mechanism to operate. Additionally, we found multiple examples of MGEs inhibiting transformation through integrative disruption of genes encoding the competence machinery across many species, providing evidence of an ongoing "arms race." Reduced rates of transformation have also been observed in cells infected by MGEs that reduce the concentration of extracellular DNA through secretion of DNases. Simulations predicted that either mechanism of limiting transformation would benefit individual MGEs, but also that this tactic's effectiveness was limited by competition with other MGEs coinfecting the same cell. A further observed behaviour we hypothesised to reduce elimination by transformation was MGE activation when cells become competent. Our model predicted that this response was effective at counteracting transformation independently of competing MGEs. Therefore, this framework is able to explain both common properties of MGEs, and the seemingly paradoxical bacterial behaviours of transformation and cell-cell killing within clonally related populations, as the consequences of intragenomic conflict between self-replicating chromosomes and parasitic MGEs. The antagonistic nature of the different mechanisms of HDT over short timescales means their contribution to bacterial evolution is likely to be substantially greater than previously appreciated

Mortality from gastrointestinal congenital anomalies at 264 hospitals in 74 low-income, middle-income, and high-income countries: a multicentre, international, prospective cohort study

Summary Background Congenital anomalies are the fifth leading cause of mortality in children younger than 5 years globally. Many gastrointestinal congenital anomalies are fatal without timely access to neonatal surgical care, but few studies have been done on these conditions in low-income and middle-income countries (LMICs). We compared outcomes of the seven most common gastrointestinal congenital anomalies in low-income, middle-income, and high-income countries globally, and identified factors associated with mortality. Methods We did a multicentre, international prospective cohort study of patients younger than 16 years, presenting to hospital for the first time with oesophageal atresia, congenital diaphragmatic hernia, intestinal atresia, gastroschisis, exomphalos, anorectal malformation, and Hirschsprung’s disease. Recruitment was of consecutive patients for a minimum of 1 month between October, 2018, and April, 2019. We collected data on patient demographics, clinical status, interventions, and outcomes using the REDCap platform. Patients were followed up for 30 days after primary intervention, or 30 days after admission if they did not receive an intervention. The primary outcome was all-cause, in-hospital mortality for all conditions combined and each condition individually, stratified by country income status. We did a complete case analysis. Findings We included 3849 patients with 3975 study conditions (560 with oesophageal atresia, 448 with congenital diaphragmatic hernia, 681 with intestinal atresia, 453 with gastroschisis, 325 with exomphalos, 991 with anorectal malformation, and 517 with Hirschsprung’s disease) from 264 hospitals (89 in high-income countries, 166 in middleincome countries, and nine in low-income countries) in 74 countries. Of the 3849 patients, 2231 (58·0%) were male. Median gestational age at birth was 38 weeks (IQR 36–39) and median bodyweight at presentation was 2·8 kg (2·3–3·3). Mortality among all patients was 37 (39·8%) of 93 in low-income countries, 583 (20·4%) of 2860 in middle-income countries, and 50 (5·6%) of 896 in high-income countries (p<0·0001 between all country income groups). Gastroschisis had the greatest difference in mortality between country income strata (nine [90·0%] of ten in lowincome countries, 97 [31·9%] of 304 in middle-income countries, and two [1·4%] of 139 in high-income countries; p≤0·0001 between all country income groups). Factors significantly associated with higher mortality for all patients combined included country income status (low-income vs high-income countries, risk ratio 2·78 [95% CI 1·88–4·11], p<0·0001; middle-income vs high-income countries, 2·11 [1·59–2·79], p<0·0001), sepsis at presentation (1·20 [1·04–1·40], p=0·016), higher American Society of Anesthesiologists (ASA) score at primary intervention (ASA 4–5 vs ASA 1–2, 1·82 [1·40–2·35], p<0·0001; ASA 3 vs ASA 1–2, 1·58, [1·30–1·92], p<0·0001]), surgical safety checklist not used (1·39 [1·02–1·90], p=0·035), and ventilation or parenteral nutrition unavailable when needed (ventilation 1·96, [1·41–2·71], p=0·0001; parenteral nutrition 1·35, [1·05–1·74], p=0·018). Administration of parenteral nutrition (0·61, [0·47–0·79], p=0·0002) and use of a peripherally inserted central catheter (0·65 [0·50–0·86], p=0·0024) or percutaneous central line (0·69 [0·48–1·00], p=0·049) were associated with lower mortality. Interpretation Unacceptable differences in mortality exist for gastrointestinal congenital anomalies between lowincome, middle-income, and high-income countries. Improving access to quality neonatal surgical care in LMICs will be vital to achieve Sustainable Development Goal 3.2 of ending preventable deaths in neonates and children younger than 5 years by 2030

Snow Surface Albedo Sensitivity to Black Carbon: Radiative Transfer Modelling

The broadband surface albedo of snow can greatly be reduced by the deposition of light-absorbing impurities, such as black carbon on or near its surface. Such a reduction increases the absorption of solar radiation and may initiate or accelerate snowmelt and snow albedo feedback. Coincident measurements of both black carbon concentration and broadband snow albedo may be difficult to obtain in field studies; however, using the relationship developed in this simple model sensitivity study, black carbon mass densities deposited can be estimated from changes in measured broadband snow albedo, and vice versa. Here, the relationship between the areal mass density of black carbon found near the snow surface to the amount of albedo reduction was investigated using the popular snow radiative transfer model Snow, Ice, and Aerosol Radiation (SNICAR). We found this relationship to be linear for realistic amounts of black carbon mass concentrations, such as those found in snow at remote locations. We applied this relationship to measurements of broadband albedo in the Chilean Andes to estimate how vehicular emissions contributed to black carbon (BC) deposition that was previously unquantified

Deposition of light-absorbing aerosols on snow: method development and changes to snow optical and radiative properties

Snow and ice cover a significant portion of the Earth’s surface, and not only provide fresh water to billions of people, but also contribute to the Earth’s energy balance through a high surface albedo, reflecting most incident solar radiation back towards space. The surface albedo and reflected radiation can be greatly reduced by small amounts of light-absorbing impurities within the snowpack, such as black carbon (BC), mineral dust aerosol, and microbial growth. A wealth of observations and modelling of snow optical and radiative properties recognize BC and mineral dust aerosol as dominating the reduction of snow albedo after deposition, but growing research into atmospheric, light-absorbing organic carbon (OC) aerosol, known as brown carbon (BrC), encourages a greater understanding of the impacts of this impurity in the snowpack. Little is known about how BrC deposition onto snow surfaces affects the spectral snow albedo and what radiative forcing results from BrC deposition. This is of special importance for areas of the Arctic where wildfires burn fuels, such as peat, that emit BrC aerosol in close proximity to snow and ice. The goal of this dissertation is to explore this snow-BrC aerosol relationship. A simple apparatus was developed to generate and deposit aerosols onto a snow surface to study aerosol deposition and its effect on snow albedo experimentally and to compare with theory. This portable apparatus was used to deposit combustion and mineral dust aerosol – including black carbon, brown carbon, and hematite – in situ onto snow surfaces. Aerosols were generated and continuously transported into a deposition chamber placed on the snow surface, where there were evenly deposited, thereby modifying the snowpack’s optical and radiative properties. Field operation of this apparatus was demonstrated and changes in snow surface reflectivity were monitored by measuring the spectral directional reflectance of the deposited areas and of adjacent natural snowpack. The apparatus was further used for the artificial deposition of emissions from Alaskan peat combustion onto a natural snow surface. This combustion occurs mostly in the smoldering phase, emitting mainly BrC aerosol designated by strongly enhanced light absorption at short-visible and ultraviolet wavelengths. This wavelength dependence was validated by observing a strong reduction in measured spectral snow albedo after deposition, mainly at these same wavelength regions predicted from previous studies of the optical properties of these aerosols generated under similar conditions of combustion. The imaginary refractive index spectrum of deposited BrC was derived from UV-vis absorption spectra of melted snow samples and total organic carbon (TOC) concentrations in the snow before and after deposition, which agreed well with results of other investigations into the refractive indices of smoldering peat combustion emissions. The optical properties of deposited BrC aerosol were calculated with Mie theory and incorporated into a snow/impurity radiative transfer model calculating surface albedo spectra of snow with BrC impurities. Measured and modelled surface albedo spectra were shown to be in good agreement – to within approximately 5% – across the UV-visible wavelength region. Finally, the amount of energy absorbed by the snowpack due to the presence of impurities before deposition to be about 40 W/m2. After depositing BrC, the instantaneous radiative forcing was increased by over 10 W/m2, yielding a direct estimate of the mass weighted radiative forcing, or forcing efficiency, for the conditions during the experiment of 1.2 ± 0.2 W/m2 per ppm of deposited BrC. In addition to estimating the impact from the artificial deposition of BrC, the snow surface spectral albedo, TOC concentration and absorption spectra of melted snow at three depths, and instantaneous radiative forcing was measured for the natural snowpack at the field site in the Sierra Nevada; these results can provide this much needed information for a spatial understanding of snow and impurity properties both locally and worldwide.In summary, this work has developed and characterized a novel apparatus for artificial deposition of aerosols onto snow and has used it, together with other measurements and radiative transfer theory, to determine the changes to snow optical properties and radiative forcing due to the deposition of BrC aerosol produced from smoldering peat combustion

Apparatus for dry deposition of aerosols on snow

Deposition of light-absorbing aerosol on snow can drastically change the albedo of the snow surface and the energy balance of the snowpack. To study these important effects experimentally and to compare them with theory, it is desirable to have an apparatus for such deposition experiments. Here, we describe a simple apparatus to generate and evenly deposit light-absorbing aerosols onto a flat snow surface. Aerosols are produced (combustion aerosols) or entrained (mineral dust aerosols) and continuously transported into a deposition chamber placed on the snow surface where they deposit onto and into the snowpack, thereby modifying its surface reflectance and albedo. We demonstrate field operation of this apparatus by generating black and brown carbon combustion aerosols and entraining hematite mineral dust aerosol and depositing them on the snowpack. Changes in spectral snow reflectance are demonstrated qualitatively through pictures of snow surfaces after aerosol deposition and quantitatively by measuring hemispherical-conical reflectance spectra for the deposited areas and for adjacent snowpack in its natural state. Additional potential applications for this apparatus are mentioned and briefly discussed

Soot superaggregates from flaming wildfires and their direct radiative forcing

Wildfires contribute significantly to global soot emissions, yet their aerosol formation mechanisms and resulting particle properties are poorly understood and parameterized in climate models. The conventional view holds that soot is formed via the cluster-dilute aggregation mechanism in wildfires and emitted as aggregates with fractal dimensionD f ≈1.8 mobility diameterD m ≤1 μm, and aerodynamic diameterD a ≤ 300 nm. Here we report the ubiquitous presence of soot superaggregates (SAs) in the outflow from a major wildfire in India. SAs are porous, low-density aggregates of cluster-dilute aggregates with characteristic D f ≈ 2.6,D m .\u3e 1 μm, andD a ≤300 nmthat form via the cluster-dense aggregation mechanism.Wepresent additional observations of soot SAs in wildfire smoke-laden air masses over Northern California, New Mexico, and Mexico City. We estimate that SAs contribute, per unit optical depth, up to 35% less atmospheric warming than freshly-emitted (D f ≈ 1.8) aggregates, and ≈90% more warming than the volume-equivalent spherical soot particles simulated in climate models