Drivers of ecological assembly in the hindgut of Atlantic Cod fed a macroalgal supplemented diet.

It is difficult to disentangle the many variables (e.g. internal or external cues and random events) that shape the microbiota in the gastrointestinal tract of any living species. Ecological assembly processes applied to microbial communities can elucidate these drivers. In our study, farmed Atlantic cod (Gadus morhua) were fed a diet of 10% macroalgae supplement (Ulva rigida [ULVA] or Ascophyllum nodosum [ASCO] or a non-supplemented control diet [CTRL]) over 12 weeks. We determined the influence of ecological assembly processes using a suite of null-modelling tools. We observed dissimilarity in the abundance of common OTUs over time, which was driven by deterministic assembly. The CTRL samples showed selection as a critical assembly process. While dispersal limitation was a driver of the gut microbiome for fish fed the macroalgae supplemented diet at Week 12 (i.e., ASCO and ULVA). Fish from the ASCO grouping diverged into ASCO_N (normal) and ASCO_LG (lower growth), where ASCO_LG individuals found the diet unpalatable. The recruitment of new taxa overtime was altered in the ASCO_LG fish, with the gut microbiome showing phylogenetic underdispersion (nepotistic species recruitment). Finally, the gut microbiome (CTRL and ULVA) showed increasing robustness to taxonomic disturbance over time and lower functional redundancy. This study advances our understanding of the ecological assembly and succession in the hindgut of juvenile Atlantic cod across dietary treatments. Understanding the processes driving ecological assembly in the gut microbiome, in fish research specifically, could allow us to manipulate the microbiome for improved health or resilience to disease for improved aquaculture welfare and production.

Changes in IPCC Scenario Assessment Emulators Between SR1.5 and AR6 Unraveled.

The IPCC's scientific assessment of the timing of net-zero emissions and 2030 emission reduction targets consistent with limiting warming to 1.5°C or 2°C rests on large scenario databases. Updates to this assessment, such as between the IPCC's Special Report on Global Warming of 1.5°C (SR1.5) of warming and the Sixth Assessment Report (AR6), are the result of intertwined, sometimes opaque, factors. Here we isolate one factor: the Earth System Model emulators used to estimate the global warming implications of scenarios. We show that warming projections using AR6-calibrated emulators are consistent, to within around 0.1°C, with projections made by the emulators used in SR1.5. The consistency is due to two almost compensating changes: the increase in assessed historical warming between SR1.5 (based on AR5) and AR6, and a reduction in projected warming due to improved agreement between the emulators' response to emissions and the assessment to which it is calibrated.

Reduced Complexity Model Intercomparison Project Phase 2: Synthesizing Earth System Knowledge for Probabilistic Climate Projections.

Over the last decades, climate science has evolved rapidly across multiple expert domains. Our best tools to capture state-of-the-art knowledge in an internally self-consistent modeling framework are the increasingly complex fully coupled Earth System Models (ESMs). However, computational limitations and the structural rigidity of ESMs mean that the full range of uncertainties across multiple domains are difficult to capture with ESMs alone. The tools of choice are instead more computationally efficient reduced complexity models (RCMs), which are structurally flexible and can span the response dynamics across a range of domain-specific models and ESM experiments. Here we present Phase 2 of the Reduced Complexity Model Intercomparison Project (RCMIP Phase 2), the first comprehensive intercomparison of RCMs that are probabilistically calibrated with key benchmark ranges from specialized research communities. Unsurprisingly, but crucially, we find that models which have been constrained to reflect the key benchmarks better reflect the key benchmarks. Under the low-emissions SSP1-1.9 scenario, across the RCMs, median peak warming projections range from 1.3 to 1.7°C (relative to 1850-1900, using an observationally based historical warming estimate of 0.8°C between 1850-1900 and 1995-2014). Further developing methodologies to constrain these projection uncertainties seems paramount given the international community's goal to contain warming to below 1.5°C above preindustrial in the long-term. Our findings suggest that users of RCMs should carefully evaluate their RCM, specifically its skill against key benchmarks and consider the need to include projections benchmarks either from ESM results or other assessments to reduce divergence in future projections.

Temporal changes in the gut microbiota in farmed Atlantic cod (Gadus morhua) outweigh the response to diet supplementation with macroalgae.

BACKGROUND: Aquaculture successfully meets global food demands for many fish species. However, aquaculture production of Atlantic cod (Gadus morhua) is just 2.5% of total market production. For cod farming to be a viable economic venture specific challenges on how to increase growth, health and farming productivity need to be addressed. Feed ingredients play a key role here. Macroalgae (seaweeds) have been suggested as a functional feed supplement with both health and economic benefits for terrestrial farmed animals and fish. The impact of such dietary supplements to cod gut integrity and microbiota, which contribute to overall fish robustness is unknown. The objective of this study was to supplement the diet of juvenile Atlantic cod with macroalgae and determine the impacts on fish condition and growth, gut morphology and hindgut microbiota composition (16S rRNA amplicon sequencing). Fish were fed one of three diets: control (no macroalgal inclusion), 10% inclusion of either egg wrack (Ascophyllum nodosum) or sea lettuce (Ulva rigida) macroalgae in a 12-week trial. RESULTS: The results demonstrated there was no significant difference in fish condition, gut morphology or hindgut microbiota between the U. rigida supplemented fish group and the control group at any time-point. This trend was not observed with the A. nodosum treatment. Fish within this group were further categorised as either 'Normal' or 'Lower Growth'. 'Lower Growth' individuals found the diet unpalatable resulting in reduced weight and condition factor combined with an altered gut morphology and microbiome relative to the other treatments. Excluding this group, our results show that the hindgut microbiota was largely driven by temporal pressures with the microbial communities becoming more similar over time irrespective of dietary treatment. The core microbiome at the final time-point consisted of the orders Vibrionales (Vibrio and Photobacterium), Bacteroidales (Bacteroidetes and Macellibacteroides) and Clostridiales (Lachnoclostridium). CONCLUSIONS: Our study indicates that U. rigida macroalgae can be supplemented at 10% inclusion levels in the diet of juvenile farmed Atlantic cod without any impact on fish condition or hindgut microbial community structure. We also conclude that 10% dietary inclusion of A. nodosum is not a suitable feed supplement in a farmed cod diet.

A hyperacute immune map of ischaemic stroke patients reveals alterations to circulating innate and adaptive cells.

Systemic immune changes following ischaemic stroke are associated with increased susceptibility to infection and poor patient outcome due to their role in exacerbating the ischaemic injury and long-term disability. Alterations to the abundance or function of almost all components of the immune system post-stroke have been identified, including lymphocytes, monocytes and granulocytes. However, subsequent infections have often confounded the identification of stroke-specific effects. Global understanding of very early changes to systemic immunity is critical to identify immune targets to improve clinical outcome. To this end, we performed a small, prospective, observational study in stroke patients with immunophenotyping at a hyperacute time point (< 3 h) to explore early changes to circulating immune cells. We report, for the first time, decreased frequencies of type 1 conventional dendritic cells (cDC1), haematopoietic stem and progenitor cells (HSPCs), unswitched memory B cells and terminally differentiated effector memory T cells re-expressing CD45RA (TEMRA). We also observed concomitant alterations to human leucocyte antigen D-related (HLA-DR), CD64 and CD14 expression in distinct myeloid subsets and a rapid activation of CD4+ T cells based on CD69 expression. The CD69+ CD4+ T cell phenotype inversely correlated with stroke severity and was associated with naive and central memory T (TCM) cells. Our findings highlight early changes in both the innate and adaptive immune compartments for further investigation as they could have implications the development of post-stroke infection and poorer patient outcomes.

Carboxylic Sulfuric Anhydrides.

Carboxylic acids react with sulfur trioxide to form carboxylic sulfuric anhydrides, RCOOSO2OH. In this article, new supersonic jet microwave spectra are presented for the anhydride derived from propiolic acid (HCCCOOH), and recent work on a series of carboxylic sulfuric anhydrides is reviewed. For the propiolic acid derivative, computed minimum-energy structures are reported for both the anhydride (HCCCOOSO2OH) and its precursor complex (HCCCOOH-SO3), and additional CCSD(T)/CBS(D-T)//M06-2X/6-311++G(3df,3pd) calculations indicate that, after zero-point energy corrections, the barrier to anhydride formation is effectively zero. These results are similar to those for other carboxylic sulfuric anhydrides studied and are consistent with their rapid production under supersonic jet conditions. Carboxylic sulfuric anhydrides, as a class, have not been widely characterized in the chemical literature and thus their study represents a new feature of the chemistry of sulfur oxides and oxyacids. As such, structural and energetic features of the carboxylic sulfuric anhydrides derived from formic, acetic, acrylic, trifluoroacetic, propiolic, pinic, and benzoic acids are compared. Computed vibrational frequencies are provided as Supporting Information and should be useful for possible future observation by infrared and/or Raman spectroscopy. Statistical thermodynamics is used to estimate the equilibrium constants for the formation reactions at a series of temperatures, and the results indicate values ranging from ∼104 atm-1 for formic acid at 288 K to over 1011 atm-1 for benzoic acid at 217 K. We speculate that carboxylic sulfuric anhydrides could be active species in the Earth's atmosphere and atmospheric concentrations have, therefore, been estimated assuming an equilibrium state. These estimates are subject to significant uncertainties in the atmospheric SO3 and carboxylic acid concentrations but may be as high as 107 molecules/cm3 in some locations. Related calculations suggest that equilibrium anhydride concentrations may exceed those of the sulfuric acid precursors SO3-H2O and SO3-(H2O)2 by several orders of magnitude. Kinetic modeling will ultimately be necessary to fully assess the role, if any, of carboxylic sulfuric anhydrides in atmospheric processes.

'Warning: allergic to penicillin': association between penicillin allergy status in 2.3 million NHS general practice electronic health records, antibiotic prescribing and health outcomes.

BACKGROUND: The prevalence of reported penicillin allergy (PenA) and the impact these records have on health outcomes in the UK general population are unknown. Without such data, justifying and planning enhanced allergy services is challenging. OBJECTIVES: To determine: (i) prevalence of PenA records; (ii) patient characteristics associated with PenA records; and (iii) impact of PenA records on antibiotic prescribing/health outcomes in primary care. METHODS: We carried out cross-sectional/retrospective cohort studies using patient-level data from electronic health records. Cohort study: exact matching across confounders identified as affecting PenA records. Setting: English NHS general practices between 1 April 2013 and 31 March 2014. Participants: 2.3 million adult patients. Outcome measures: prevalence of PenA, antibiotic prescribing, mortality, MRSA infection/colonization and Clostridioides difficile infection. RESULTS: PenA prevalence was 5.9% (IQR = 3.8%-8.2%). PenA records were more common in older people, females and those with a comorbidity, and were affected by GP practice. Antibiotic prescribing varied significantly: penicillins were prescribed less frequently in those with a PenA record [relative risk (RR)  = 0.15], and macrolides (RR = 4.03), tetracyclines (RR = 1.91) nitrofurantoin (RR = 1.09), trimethoprim (RR = 1.04), cephalosporins (RR = 2.05), quinolones (RR = 2.10), clindamycin (RR = 5.47) and total number of prescriptions were increased in patients with a PenA record. Risk of re-prescription of a new antibiotic class within 28 days (RR = 1.32), MRSA infection/colonization (RR = 1.90) and death during the year subsequent to 1 April 2013 (RR = 1.08) increased in those with PenA records. CONCLUSIONS: PenA records are common in the general population and associated with increased/altered antibiotic prescribing and worse health outcomes. We estimate that incorrect PenA records affect 2.7 million people in England. Establishing true PenA status (e.g. oral challenge testing) would allow more people to be prescribed first-line antibiotics, potentially improving health outcomes.

Carbide and nitride phase characterization in a transition metal carbo-nitride using x-ray spectroscopy and atom probe tomography.

A multi-phase hafnium carbo-nitride was investigated by various analytical methods. Incomplete homogenization between mixed HfC-HfN starting powders subjected to hot isostatic pressing resulted in both carbon-rich and nitrogen-rich phases. The compositions of these two phases were quantified in detail by wavelength dispersive spectroscopy and atom probe tomography, with the atom probe tips having either a small or a large shank angle geometry. For each of the two phases, an agreement of the compositions obtained by wavelength dispersive spectroscopy and atom probe tomography was found. However, the quality of the mass spectrum and hit multiplicity (single hits) were generally higher for the carbon-rich as compared to the nitrogen-rich carbo-nitride. Though the atom probe tip geometry does not appear to influence the composition, the mass resolving power did improve with the larger shank angle geometry while the hit multiplicity deteriorated slightly. Finally, our results demonstrate that hafnium carbide requires less thermal assistance to field evaporate than hafnium nitride.

A strong dependence of the CH3 internal rotation barrier on conformation in thioacetic acid: Microwave measurements and an energy decomposition analysis.

Rotational spectra of thioacetic acid (CH3COSH) have been observed by pulsed-nozzle Fourier transform microwave spectroscopy. Spectroscopic constants are reported for both the syn and anti conformers of the parent species, as well as the 34S and 13C carbonyl isotopologues. Transitions arising from the lowest A and E internal rotor states of the methyl group have been observed and analyzed. Experimental values of the three-fold internal rotation barrier, V3, for the syn and anti conformers of the parent isotopologue are 76.300(12) and 358.056(51) cm-1, respectively, indicating a large effect of the S-H orientation on the CH3 internal rotation potential. M06-2X/6-311+G(d,p) calculations are in good agreement with these results. The block localized energy decomposition method has been applied to understand the origins of this strong dependence of V3 on conformation. The results indicate that π conjugation from the SH to the carbonyl group and steric repulsion between the SH and the methyl group in the anti form are main contributors to the difference.

A Protocol for Sedation Free MRI and PET Imaging in Adults with Autism Spectrum Disorder.

Imaging technologies such as positron emission tomography (PET) and magnetic resonance imaging (MRI) present unparalleled opportunities to investigate the neural basis of autism spectrum disorder (ASD). However, challenges such as deficits in social interaction, anxiety around new experiences, impaired language abilities, and hypersensitivity to sensory stimuli make participating in neuroimaging studies challenging for individuals with ASD. In this commentary, we describe the existent training protocols for preparing individuals with ASD for PET/MRI scans and our own experience developing a training protocol to facilitate the inclusion of low-functioning adults with ASD in PET-MRI studies. We hope to raise awareness of the need for more information exchange between research groups about lessons learned in this context in order to include the entire disease spectrum in neuroimaging studies.

Additive manufacturing titanium components with isotropic or graded properties by hybrid electron beam melting/hot isostatic pressing powder processing.

A methodology has been demonstrated to consolidate Ti-6Al-4V powder without taking it to the liquid state by novel combination of the electron beam melting additive manufacture and hot isostatic pressing processes. This results in improved static mechanical properties (both strength and yield) in comparison to standard EBM processed material. In addition, the ability to generate microstructurally graded components has been demonstrated by generating a component with a significant change in both microstructure and mechanical properties. This is revealed by the use of electron backscattered diffraction and micro hardness testing to produce maps showing a clear distinction between materials consolidated in different ways. The variation in microstructure and mechanical properties is attributed to the different thermal history experienced by the material at different locations. In particular, it is found that the rapid cooling experienced during EBM leads to a typical fine α lath structure, whereas a more equiaxed α grains generated by diffusion is found in HIP consolidated powder.

A Perfluorinated Carboxylic Sulfuric Anhydride: Microwave and Computational Studies of CF3COOSO2OH.

Trifluoroacetic sulfuric anhydride (CF3COOSO2OH, TFASA) and its deuterated isotopologue have been observed by pulsed-nozzle Fourier transform microwave spectroscopy. TFASA was generated in situ in a supersonic expansion from the reaction of CF3COOH or CF3COOD with SO3. The spectrum, which was notably weaker than those of previously studied carboxylic sulfuric anhydrides, is that of a simple asymmetric rotor with no evidence of internal rotation of the CF3 group. Calculations at the M06-2X/6-311++G(3df,3pd) level indicate that the title compound is produced via a mechanism involving a concerted cycloaddition, analogous to that found for other carboxylic sulfuric anhydrides. The calculations further show that the equilibrium orientation of CF3 relative to the C═O bond changes upon formation of the anhydride, indicating that any path connecting the equilibrium structures of CF3COOH and CF3COOSO2OH necessarily includes both cycloaddition and internal rotation. CCSD(T)/complete basis set with double and triple extrapolation [CBS(D-T)] single-point energy calculations at key points on the potential surface indicate that the barrier to form TFASA from a putative CF3COOH···SO3 complex is about 1.2 kcal/mol after zero-point energy corrections. This value is significantly larger than the near-zero or slightly negative barriers previously reported for the reactions of SO3 with nonfluorinated carboxylic acids and likely accounts, at least in part, for the reduced spectral intensity. Thus, TFASA is a somewhat unique addition to the series of carboxylic sulfuric anhydrides studied to date. Theoretical values of certain structural parameters, atomic charges, and vibrational frequencies also support this point of view. Despite the differences, however, this work clearly demonstrates that the reaction RCOOH + SO3 → RCOOSO2OH readily occurs in the gas phase and is not restricted to acids with hydrocarbon R groups.

Long-term changes in the structure of benthic communities: Revisiting a sampling transect in Crete after 24 years.

A bathymetric transect in the north coast of Crete first studied in 1989, was revisited 24 years later. Identical sampling design, season, techniques and protocols were followed in both studies in order to minimize bias in the long-term comparisons. This comprehensive macrofaunal dataset (4 stations, 2 sampling seasons, 7 replicates in each study) revealed changes in benthic diversity and community composition between the sampling periods. The recorded changes were higher at the stations located close to the coastal zone. In addition, while benthic communities showed lower total abundance during the recent sampling period, species abundances were more evenly distributed indicating that some species dominated the historical communities. In spite of these changes, the ecological status remained above the threshold values for good ecological status. The results indicated that changes in the benthic community seem to have been driven by local anthropogenic factors and natural variability rather than by large-scale factors such as nutrients influxes in the entire Mediterranean Basin.

Efficacy of Climate Forcings in PDRMIP Models.

Quantifying the efficacy of different climate forcings is important for understanding the real-world climate sensitivity. This study presents a systematic multimodel analysis of different climate driver efficacies using simulations from the Precipitation Driver and Response Model Intercomparison Project (PDRMIP). Efficacies calculated from instantaneous radiative forcing deviate considerably from unity across forcing agents and models. Effective radiative forcing (ERF) is a better predictor of global mean near-surface air temperature (GSAT) change. Efficacies are closest to one when ERF is computed using fixed sea surface temperature experiments and adjusted for land surface temperature changes using radiative kernels. Multimodel mean efficacies based on ERF are close to one for global perturbations of methane, sulfate, black carbon, and insolation, but there is notable intermodel spread. We do not find robust evidence that the geographic location of sulfate aerosol affects its efficacy. GSAT is found to respond more slowly to aerosol forcing than CO2 in the early stages of simulations. Despite these differences, we find that there is no evidence for an efficacy effect on historical GSAT trend estimates based on simulations with an impulse response model, nor on the resulting estimates of climate sensitivity derived from the historical period. However, the considerable intermodel spread in the computed efficacies means that we cannot rule out an efficacy-induced bias of ±0.4 K in equilibrium climate sensitivity to CO2 doubling when estimated using the historical GSAT trend.

Complex evaporation behavior of a transition metal carbo-nitride (Hf(C,N)) studied by atom probe tomography.

The use of pulsed lasers in atom probe tomography has enabled the analysis of lower conductivity materials such as hafnium carbo-nitrides. The variability of experimental parameters can have a profound effect on field evaporation behavior, data quality and compositional accuracy. This is especially challenging for materials such as hafnium carbo-nitride, where a mixture of covalent, ionic and metallic bonding types is present. Here we study the influence of laser pulse energy on how the field evaporation evolves in a hafnium carbo-nitride and how that impacts data quality and compositional accuracy. Changing the laser pulse energy, while keeping other parameters constant, alters the resulting composition. A gain in Hf concentration is observed for higher laser pulse energies while at the same time the N concentration decreases. At lower laser pulse energies, the obtained composition is in good agreement with the reference bulk composition of the material. Furthermore, our results demonstrate that assessing the quality of an APT experiment or dataset merely based on commonly used metrics such as quality of mass spectrum, hit distribution on the detector, hit multiplicity and mass resolving power, can be misleading and is not enough to ensure the most accurate compositional data. Moreover, it is shown that the complex evaporation behavior of transition metal carbo-nitrides and potential ion loss mechanisms are not well enough understood yet and further work is required to fully comprehend these complex behaviors in these types of ceramics.

Impact of stroke-associated pneumonia on mortality, length of hospitalization, and functional outcome.

OBJECTIVES: Stroke-associated pneumonia (SAP) is common and associated with adverse outcomes. Data on its impact beyond 1 year are scarce. MATERIALS AND METHODS: This observational study was conducted in a cohort of stroke patients admitted consecutively to a tertiary referral center in the east of England, UK (January 2003-April 2015). Logistic regression models examined inpatient mortality and length of stay (LOS). Cox regression models examined longer-term mortality at predefined time periods (0-90 days, 90 days-1 year, 1-3 years, and 3-10 years) for SAP. Effect of SAP on functional outcome at discharge was assessed using logistic regression. RESULTS: A total of 9238 patients (mean age [±SD] 77.61 ± 11.88 years) were included. SAP was diagnosed in 1083 (11.7%) patients. The majority of these cases (n = 658; 60.8%) were aspiration pneumonia. After controlling for age, sex, stroke type, Oxfordshire Community Stroke Project (OCSP) classification, prestroke modified Rankin scale, comorbidities, and acute illness markers, mortality estimates remained significant at 3 time periods: inpatient (OR 5.87, 95%CI [4.97-6.93]), 0-90 days (2.17 [1.97-2.40]), and 91-365 days (HR 1.31 [1.03-1.67]). SAP was also associated with higher odds of long LOS (OR 1.93 [1.67-2.22]) and worse functional outcome (OR 7.17 [5.44-9.45]). In this cohort, SAP did not increase mortality risk beyond 1 year post-stroke, but it was associated with reduced mortality beyond 3 years. CONCLUSIONS: Stroke-associated pneumonia is not associated with increased long-term mortality, but it is linked with increased mortality up to 1 year, prolonged LOS, and poor functional outcome on discharge. Targeted intervention strategies are required to improve outcomes of SAP patients who survive to hospital discharge.

Cold adaptation and replicable microbial community development during long-term low-temperature anaerobic digestion treatment of synthetic sewage.

The development and activity of a cold-adapting microbial community was monitored during low-temperature anaerobic digestion (LtAD) treatment of wastewater. Two replicate hybrid anaerobic sludge bed-fixed-film reactors treated a synthetic sewage wastewater at 12°C, at organic loading rates of 0.25-1.0 kg chemical oxygen demand (COD) m-3 d-1, over 889 days. The inoculum was obtained from a full-scale anaerobic digestion reactor, which was operated at 37°C. Both LtAD reactors readily degraded the influent with COD removal efficiencies regularly exceeding 78% for both the total and soluble COD fractions. The biomass from both reactors was sampled temporally and tested for activity against hydrolytic and methanogenic substrates at 12°C and 37°C. Data indicated that significantly enhanced low-temperature hydrolytic and methanogenic activity developed in both systems. For example, the hydrolysis rate constant (k) at 12°C had increased 20-30-fold by comparison to the inoculum by day 500. Substrate affinity also increased for hydrolytic substrates at low temperature. Next generation sequencing demonstrated that a shift in a community structure occurred over the trial, involving a 1-log-fold change in 25 SEQS (OTU-free approach) from the inoculum. Microbial community structure changes and process performance were replicable in the LtAD reactors.

Hydration of an Acid Anhydride: The Water Complex of Acetic Sulfuric Anhydride.

The complex formed from acetic sulfuric anhydride (CH3COOSO2OH, ASA) and water has been observed by pulsed nozzle Fourier transform microwave spectroscopy. ASA was formed in situ in the supersonic jet via the reaction of SO3 and CH3COOH, and subsequently complexed with water using a concentric, dual injection needle that allows reagents to be introduced at different points along the expansion axis. Spectroscopic constants for the parent, fully deuterated, and CH313COOSO2OH species are reported. Both A and E internal rotor states have been observed and analyzed. The fitted internal rotation barrier of the methyl group is 219.598(21) cm-1 for the parent species, indicating that complexation with water lowers the internal rotation barrier of the methyl group by 9% relative to that of the free ASA. M06-2X/6-311++G(3df,3pd) calculations predict at least two distinct isomeric forms of ASA···H20. Spectroscopic constants for the observed species agree with those for the lower energy isomer in which the water inserts into the intramolecular hydrogen bond of the ASA monomer. CCSD(T)/CBS(D-T) calculations place the binding energy of this isomer at 13.3 kcal/mol below that of the isolated ASA and H2O monomers. The calculations further indicate that the doubly hydrogen bonded complex CH3COOH···H2SO4, which contains the hydrolysis products of ASA, lies even lower in energy, but this species was not observed in this study. This system represents the first stage of microsolvation of an acid anhydride, and the results indicate that a single water molecule does not induce spontaneous hydrolysis in a cold molecular cluster.

Climate Impacts From a Removal of Anthropogenic Aerosol Emissions.

Limiting global warming to 1.5 or 2.0°C requires strong mitigation of anthropogenic greenhouse gas (GHG) emissions. Concurrently, emissions of anthropogenic aerosols will decline, due to coemission with GHG, and measures to improve air quality. However, the combined climate effect of GHG and aerosol emissions over the industrial era is poorly constrained. Here we show the climate impacts from removing present-day anthropogenic aerosol emissions and compare them to the impacts from moderate GHG-dominated global warming. Removing aerosols induces a global mean surface heating of 0.5-1.1°C, and precipitation increase of 2.0-4.6%. Extreme weather indices also increase. We find a higher sensitivity of extreme events to aerosol reductions, per degree of surface warming, in particular over the major aerosol emission regions. Under near-term warming, we find that regional climate change will depend strongly on the balance between aerosol and GHG forcing.

Understanding Rapid Adjustments to Diverse Forcing Agents.

Rapid adjustments are responses to forcing agents that cause a perturbation to the top of atmosphere energy budget but are uncoupled to changes in surface warming. Different mechanisms are responsible for these adjustments for a variety of climate drivers. These remain to be quantified in detail. It is shown that rapid adjustments reduce the effective radiative forcing (ERF) of black carbon by half of the instantaneous forcing, but for CO2 forcing, rapid adjustments increase ERF. Competing tropospheric adjustments for CO2 forcing are individually significant but sum to zero, such that the ERF equals the stratospherically adjusted radiative forcing, but this is not true for other forcing agents. Additional experiments of increase in the solar constant and increase in CH4 are used to show that a key factor of the rapid adjustment for an individual climate driver is changes in temperature in the upper troposphere and lower stratosphere.