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During the summer of 2018, the upward-pointing Wyoming Cloud Lidar (WCL) was deployed on board the University of Wyoming King Air (UWKA) research aircraft for the Biomass Burning Flux Measurements of Trace Gases and Aerosols (BB-FLUX) field campaign. This paper describes the generation of calibrated attenuated backscatter coefficients and aerosol extinction coefficients from the WCL measurements. The retrieved aerosol extinction coefficients at the flight level strongly correlate (correlation coefficient, rr > 0.8) with in situ aerosol concentration and carbon monoxide (CO) concentration, providing a first-order estimate for converting WCL extinction coefficients into vertically resolved CO and aerosol concentration within wildfire smoke plumes. The integrated CO column concentrations from the WCL data in nonextinguished profiles also correlate (rr = 0.7) with column measurements by the University of Colorado Airborne Solar Occultation Flux instrument, indicating the validity of WCL-derived extinction coefficients. During BB-FLUX, the UWKA sampled smoke plumes from more than 20 wildfires during 35 flights over the western United States. Seventy percent of flight time was spent below 3 km above ground level (AGL) altitude, although the UWKA ascended up to 6 km AGL to sample the top of some deep smoke plumes. The upward-pointing WCL observed a nearly equal amount of thin and dense smoke below 2 km and above 5 km due to the flight purpose of targeted fresh fire smoke. Between 2 and 5 km, where most of the wildfire smoke resided, the WCL observed slightly more thin smoke than dense smoke due to smoke spreading. Extinction coefficients in dense smoke were 2–10 times stronger, and dense smoke tended to have larger depolarization ratio, associated with irregular aerosol particles.

As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.

This study presents upper troposphere–lower stratosphere (UTLS) water vapour and ozone climatologies generated from 14 years (June 2004 to May 2018) of measurements made by three Canadian limb-viewing satellite instruments: the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (MAESTRO), and the Optical Spectrograph and InfraRed Imaging System (OSIRIS; ozone only). This selection of instruments was chosen to explore the capability of these Canadian instruments in representing the UTLS and to enable analysis of the impact of different measurement sampling patterns. The water vapour and ozone climatologies have been constructed using tropopause-relative potential temperature and equivalent-latitude coordinates in an effort to best represent the distribution of these two gases in the UTLS, which is characterized by a high degree of dynamic and geophysical variability. Zonal-mean multiyear-mean climatologies are provided with 5∘ equivalent latitude and 10 K potential temperature spacing and have been constructed on a monthly, seasonal (3-month), and yearly basis. These climatologies are examined in-depth for two 3-month periods, December–January–February and June–July–August, and are compared to reference climatologies constructed from the Canadian Middle Atmosphere Model 39-year specified dynamics (CMAM39-SD) run, subsampled to the times and locations of the satellite measurements, in order to evaluate the consistency of water vapour and ozone between the datasets. Specifically, this method of using a subsampled model addresses the impact of each instrument's measuring pattern and allows for the quantification of the influence of different measurement patterns on multiyear climatologies. This in turn permits a more consistent evaluation of the distributions of these two gas species, as assessed through the differences between the model and measurement climatologies. For water vapour, the average absolute relative difference between CMAM39-SD and ACE-FTS differed between the two versions of ACE-FTS by less than 8 %, while the MAESTRO climatologies were found to differ by 15 %–41 % from ACE-FTS, depending on the version of ACE-FTS and the season. When considering the ozone climatologies, those constructed from the two ACE-FTS versions agreed to within 2 % overall, and the OSIRIS ozone climatologies agreed with these to within 10 %. The MAESTRO ozone climatologies differ from those from ACE-FTS and OSIRIS by 30 %–35 % and 25 %, respectively, albeit with regions of better agreement within the UTLS. These findings indicate that this set of Canadian limb sounders yields generally similar water vapour and ozone distributions in the UTLS, with some exceptions for MAESTRO depending on the season and gas species.

As the third most important greenhouse gas (GHG) after CO2 and methane, tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime, however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been reported previously, and we show that there continues to be no convergence among models, nor improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of +/- 50 % depending on the model and the altitude. The MMM performs best, within +/- 8 % at most locations and seasons. However, nearly all models overestimate O3 near the tropopause (~300 hPa or ~8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade , model results are as highly variable as ever, and have not increased in accuracy for representing Arctic tropospheric.

The Arctic atmosphere is warming rapidly and its relatively pristine environment is sensitive to the long-range transport of atmospheric pollutants. While carbon dioxide is the main cause for global warming, short-lived climate forcers (SLCFs) such as methane, ozone, and particles also play a role in Arctic climate on near-term time scales. Atmospheric modelling is critical for understanding the abundance and distribution of SLCFs throughout the Arctic atmosphere, and is used as a tool towards determining SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models, assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over four years (2008–2009 and 2014–2015) conducted for the 2021 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship and aircraft-based observations. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean was able to represent the general features of SLCFs in the Arctic, though vertical mixing, long-range transport, deposition, and wildfire emissions remain highly uncertain processes. These need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment.

Studies have recently reported statistically significant relationships between observed year-to-year spring Antarctic ozone variability and the Southern Hemisphere annular mode and surface temperatures in spring–summer. This study investigates whether current chemistry–climate models (CCMs) can capture these relationships, in particular, the connection between November total column ozone (TCO) and Australian summer surface temperatures, where years with anomalously high TCO over the Antarctic polar cap tend to be followed by warmer summers. The interannual ozone–temperature teleconnection is examined over the historical period in the observations and simulations from the Whole Atmosphere Community Climate Model (WACCM) and nine other models participating in the Chemistry–Climate Model Initiative (CCMI). There is a systematic difference between the WACCM experiments forced with prescribed observed sea surface temperatures (SSTs) and those with an interactive ocean. Strong correlations between TCO and Australian temperatures are only obtained for the uncoupled experiment, suggesting that the SSTs could be important for driving both variations in Australian temperatures and the ozone hole, with no causal link between the two. Other CCMI models also tend to capture this relationship with more fidelity when driven by observed SSTs, although additional research and targeted modeling experiments are required to determine causality and further explore the role of model biases and observational uncertainty. The results indicate that CCMs can reproduce the relationship between spring ozone and summer Australian climate reported in observational studies, suggesting that incorporating ozone variability could improve seasonal predictions; however, more work is required to understand the difference between the coupled and uncoupled simulations.

The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability, and its changes and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified-dynamics chemistry–climate model (CCM) simulations from the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the International Global Atmospheric Chemistry – Stratosphere-troposphere Processes And their Role in Climate (IGAC-SPARC) (IGAC–SPARC) Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozone-sonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (∼0–5.5 km) sub-column ozone is found for EMAC, ranging from 2 to 8 Dobson units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (∼±4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozone-sondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with a negative bias in the troposphere resulting from a likely underestimation of photochemical ozone production. This has ramifications for diagnosing the level of model–measurement agreement. Model variability is found to be more similar in magnitude to that implied from ozone-sondes in comparison with OMI, which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is inferred that CMAM simulates a faster and shallower Brewer–Dobson circulation (BDC) compared to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is significant and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long-term changes in the CCM ozone tracers are calculated for different seasons. An overall statistically significant increase in tropospheric ozone is found across much of the world but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5 %–10 %) between 1980–1989 and 2001–2010. Our model study implies that attribution from stratosphere–troposphere exchange (STE) to such ozone changes ranges from 25 % to 30 % at the surface to as much as 50 %–80 % in the upper troposphere–lower stratosphere (UTLS) across some regions of the world, including western Eurasia, eastern North America, the South Pacific and the southern Indian Ocean. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere.

The observing system design of multi-disciplinary field measurements involves a variety of considerations on logistics, safety, and science objectives. Typically, this is done based on investigator intuition and designs of prior field measurements. However, there is potential for considerable increase in efficiency, safety, and scientific success by integrating numerical simulations in the design process. Here, we present a novel approach to observing system simulation experiments that aids surface-atmosphere synthesis at the interface of meso- and microscale meteorology. We used this approach to optimize the Chequamegon Heterogeneous Ecosystem Energy-balance Study Enabled by a High-density Extensive Array of Detectors 2019 (CHEESEHEAD19).During pre-field simulation experiments, we considered the placement of 20 eddy-covariance flux towers, operations for 72 hours of low-altitude flux aircraft measurements, and integration of various remote sensing data products. High-resolution Large Eddy Simulations generated a super-sample of virtual ground, airborne, and satellite observations to explore two specific design hypotheses. We then analyzed these virtual observations through Environmental Response Functions to yield an optimal aircraft flight strategy for augmenting a stratified random flux tower network in combination with satellite retrievals.We demonstrate how this novel approach doubled CHEESEHEAD19’s ability to explore energy balance closure and spatial patterning science objectives while substantially simplifying logistics. Owing to its extensibility, the approach lends itself to optimize observing system designs also for natural climate solutions, emission inventory validation, urban air quality, industry leak detection and multi-species applications, among other use cases.

In order to validate satellite measurements of atmospheric composition, it is necessary to understand the range of random and systematic uncertainties inherent in the measurements. On occasions where measurements from two different satellite instruments do not agree within those estimated uncertainties, a common explanation is that the difference can be assigned to geophysical variability, i.e., differences due to sampling the atmosphere at different times and locations. However, the expected geophysical variability is often left ambiguous and rarely quantified. This paper describes a case study where the geophysical variability of O3 between two satellite instruments – ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) and OSIRIS (Optical Spectrograph and InfraRed Imaging System) – is estimated using simulations from climate models. This is done by sampling the models CMAM (Canadian Middle Atmosphere Model), EMAC (ECHAM/MESSy Atmospheric Chemistry), and WACCM (Whole Atmosphere Community Climate Model) throughout the upper troposphere and stratosphere at times and geolocations of coincident ACE-FTS and OSIRIS measurements. Ensemble mean values show that in the lower stratosphere, O3 geophysical variability tends to be independent of the chosen time coincidence criterion, up to within 12 h; and conversely, in the upper stratosphere geophysical variation tends to be independent of the chosen distance criterion, up to within 2000 km. It was also found that in the lower stratosphere, at altitudes where there is the greatest difference between air composition inside and outside the polar vortex, the geophysical variability in the southern polar region can be double of that in the northern polar region. This study shows that the ensemble mean estimates of geophysical variation can be used when comparing data from two satellite instruments to optimize the coincidence criteria, allowing for the use of more coincident profiles while providing an estimate of the geophysical variation within the comparison results.

The observing system design of multi-disciplinary field measurements involves a variety of considerations on logistics, safety, and science objectives. Typically, this is done based on investigator...

The Chequamegon Heterogeneous Ecosystem Energy-Balance Study Enabled by a High-Density Extensive Array of Detectors 2019 (CHEESEHEAD19) is an ongoing National Science Foundation project based on an intensive field campaign that occurred from June to October 2019. The purpose of the study is to examine how the atmospheric boundary layer (ABL) responds to spatial heterogeneity in surface energy fluxes. One of the main objectives is to test whether lack of energy balance closure measured by eddy covariance (EC) towers is related to mesoscale atmospheric processes. Finally, the project evaluates data-driven methods for scaling surface energy fluxes, with the aim to improve model–data comparison and integration. To address these questions, an extensive suite of ground, tower, profiling, and airborne instrumentation was deployed over a 10 km × 10 km domain of a heterogeneous forest ecosystem in the Chequamegon–Nicolet National Forest in northern Wisconsin, United States, centered on an existing 447-m tower that anchors an AmeriFlux/NOAA supersite (US-PFa/WLEF). The project deployed one of the world’s highest-density networks of above-canopy EC measurements of surface energy fluxes. This tower EC network was coupled with spatial measurements of EC fluxes from aircraft; maps of leaf and canopy properties derived from airborne spectroscopy, ground-based measurements of plant productivity, phenology, and physiology; and atmospheric profiles of wind, water vapor, and temperature using radar, sodar, lidar, microwave radiometers, infrared interferometers, and radiosondes. These observations are being used with large-eddy simulation and scaling experiments to better understand submesoscale processes and improve formulations of subgrid-scale processes in numerical weather and climate models.

The observing system design of multidisciplinary field measurements involves a variety of considerations on logistics, safety, and science objectives. Typically, this is done based on investigator intuition and designs of prior field measurements. However, there is potential for considerable increases in efficiency, safety, and scientific success by integrating numerical simulations in the design process. Here, we present a novel numerical simulation–environmental response function (NS–ERF) approach to observing system simulation experiments that aids surface–atmosphere synthesis at the interface of mesoscale and microscale meteorology. In a case study we demonstrate application of the NS–ERF approach to optimize the Chequamegon Heterogeneous Ecosystem Energy-balance Study Enabled by a High-density Extensive Array of Detectors 2019 (CHEESEHEAD19). During CHEESEHEAD19 pre-field simulation experiments, we considered the placement of 20 eddy covariance flux towers, operations for 72 h of low-altitude flux aircraft measurements, and integration of various remote sensing data products. A 2 h high-resolution large eddy simulation created a cloud-free virtual atmosphere for surface and meteorological conditions characteristic of the field campaign domain and period. To explore two specific design hypotheses we super-sampled this virtual atmosphere as observed by 13 different yet simultaneous observing system designs consisting of virtual ground, airborne, and satellite observations. We then analyzed these virtual observations through ERFs to yield an optimal aircraft flight strategy for augmenting a stratified random flux tower network in combination with satellite retrievals. We demonstrate how the novel NS–ERF approach doubled CHEESEHEAD19's potential to explore energy balance closure and spatial patterning science objectives while substantially simplifying logistics. Owing to its modular extensibility, NS–ERF lends itself to optimizing observing system designs also for natural climate solutions, emission inventory validation, urban air quality, industry leak detection, and multi-species applications, among other use cases.

International audience; Ozone profile measurements collected at L'Aquila (Italy, 42.4°N) during seventeen years of radio-sounding 30 (2000-2016) are presented here, with an analysis of derived trends. Model results from the SPARC-CCMI exercise are used in parallel to highlight the physical and chemical mechanisms regulating mid-latitude ozone trends. The statistically significant trends highlighted in time series at L'Aquila are those in the mid-upper stratosphere (+5.9±4.2), mid troposphere https://doi.org/10.5194/acp-2020-525 Preprint. Discussion started: 1 July 2020 c Author(s) 2020. CC BY 4.0 License. 2 (+5.9±2.4) and upper troposphere (+2.5±0.9), all in percent/decade. The upper stratospheric positive trend was already well documented in recent WMO assessments and attributed to the starting decline of stratospheric Cly and Bry and to the 35 stratospheric cooling induced by increasing well mixed greenhouse gases, thus slowing down gas-phase reactions that destroy ozone in the upper stratosphere. The ozone increase in the mid-upper troposphere is largely regulated by the increasing strength of the Brewer-Dobson circulation, which moves more ozone from the tropics to the extratropics and enhances the tropospheric influx from the lowermost stratosphere. This climate feedback mechanism on tropospheric ozone is only partially compensated by the increasing chemical ozone loss associated to higher H2O values in response to the 40 tropospheric warming. We also note that ozone trends obtained in the lower stratosphere are negative (-2.2 percent/decade), but do not result to be statistically significant in our analyses.

Water vapor (H2O) is the source of reactive hydrogen radicals in the middle atmosphere, whereas carbon monoxide (CO), being formed by CO2 photolysis, is suitable as a dynamical tracer. In the mesosphere, both H2O and CO are sensitive to solar irradiance variability because of their destruction/production by solar radiation. This enables to analyze the solar signal in both, models and observed data. Here, we evaluate the mesospheric H2O and CO response to solar irradiance variability using the Chemistry-Climate Model Initiative (CCMI-1) simulations and satellite data. We analyzed the results of four CCMI models (CMAM, EMAC-L90MA, SOCOLv3, CESM1-WACCM 3.5) operated in CCMI reference simulation REF-C1SD in specified dynamics mode, covering the period from 1984 to 2017. Multiple linear regression analysis shows a pronounced and statistically robust response of H2O and CO to solar irradiance variability, and to the annual and semiannual cycles. For periods with available satellite data, we compared the simulated solar signal against satellite observations, namely during 1992–2017 for H2O and 2005–2017 for CO. The model results generally agree with observations and reproduce an expected negative and positive correlation for H2O and CO, respectively, with solar irradiance. However, the magnitude of the response and patterns of the solar signal varies among the considered models, indicating differences in the applied chemical reaction and dynamical schemes including the representation of photolyses. We suggest that there is no dominating thermospheric influence of solar irradiance in CO, as reported in previous studies because the response to solar variability is comparable with observations in both, low-top and high-top models. We stress the importance of this work for improving our understanding of the current ability and limitations of state-of-the-art models to simulate a solar signal in the chemistry and dynamic of the middle atmosphere.

Climate models consistently predict an acceleration of the Brewer-Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among individual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyze the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyze the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesized to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10% to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.

One of the key questions in the air quality and climate sciences is how tropospheric ozone concentrations will change in the future. This will depend on two factors: changes in stratosphere-to-troposphere transport (STT) and changes in tropospheric chemistry. Here we aim to identify robust changes in STT using simulations from the Chemistry Climate Model Initiative (CCMI) under a common climate change scenario (RCP6.0). We use two idealized stratospheric tracers to isolate changes in transport: stratospheric ozone (O3S), which is exactly like ozone but has no chemical sources in the troposphere, and st80, a passive tracer with fixed volume mixing ratio in the stratosphere. We find a robust increase in the tropospheric columns of these two tracers across the models. In particular, stratospheric ozone in the troposphere is projected to increase 10 %–16 % by the end of the 21st century in the RCP6.0 scenario. Future STT is enhanced in the subtropics due to the strengthening of the shallow branch of the Brewer–Dobson circulation (BDC) in the lower stratosphere and of the upper part of the Hadley cell in the upper troposphere. The acceleration of the deep branch of the BDC in the Northern Hemisphere (NH) and changes in eddy transport contribute to increased STT at high latitudes. These STT trends are caused by greenhouse gas (GHG) increases, while phasing out of ozone-depleting substances (ODS) does not lead to robust transport changes. Nevertheless, the decline of ODS increases the reservoir of ozone in the lower stratosphere, which results in enhanced STT of O3S at middle and high latitudes. A higher emission scenario (RCP8.5) produces stronger STT trends, with increases in tropospheric column O3S more than 3 times larger than those in the RCP6.0 scenario by the end of the 21st century.

Objectives The primary objective of this study was to provide physician-level data about the frequency of critical procedures at a combined adult and pediatric Level I trauma center, high-acuity, high-volume academic ED. The inspiration for this study question came from a previous study by Mittiga et al. (2013) describing pediatric critical procedure data at a similar high-acuity, high-volume, pediatric-only academic ED. Our secondary objective is to compare our pediatric level procedural spectrum and frequency with those published by Mittiga et al. (2013). Methods This prospective observational study occurred over eleven consecutive months at an urban, Level I combined adult/pediatric trauma center with 96,000 annual visits (8500 pediatric). We recorded only procedures performed in the resuscitation bays. All data analysis is descriptive. Results Over eleven months, data on 3891 resuscitations were collected (3686 adults and 205 children); 38 faculty physicians supervised 1838 total critical procedures, 64 on children. The mean number of critical procedures per physician per month was 4.42 (0.15 on children). Additionally, ultrasound for intravenous access, extended focused assessment with sonography for trauma (e-FAST), or cardiac ultrasound were performed in 3862 resuscitations (178 pediatric). Conclusions Emergency medicine faculty physicians at a combined Level I adult and pediatric trauma center performed and/or supervised 4.4 total (0.15 pediatric) critical procedures per month per faculty which is nearly 6 times more critical procedures monthly than faculty at a similar volume pediatric-only trauma center. However, fewer critical procedures were performed on children at the combined facility.

Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 ± 9%) but smaller growth between 1960 and 2000 (approximately 16 ± 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050–2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation.

The top-of-atmosphere (TOA) outgoing longwave flux over the 9.6 µm ozone band is a fundamental quantity for understanding chemistry–climate coupling. However, observed TOA fluxes are hard to estimate as they exhibit considerable variability in space and time that depend on the distributions of clouds, ozone (O3), water vapor (H2O), air temperature (Ta), and surface temperature (Ts). Benchmarking present-day fluxes and quantifying the relative influence of their drivers is the first step for estimating climate feedbacks from ozone radiative forcing and predicting radiative forcing evolution. To that end, we constructed observational instantaneous radiative kernels (IRKs) under clear-sky conditions, representing the sensitivities of the TOA flux in the 9.6 µm ozone band to the vertical distribution of geophysical variables, including O3, H2O, Ta, and Ts based upon the Aura Tropospheric Emission Spectrometer (TES) measurements. Applying these kernels to present-day simulations from the Chemistry-Climate Model Initiative (CCMI) project as compared to a 2006 reanalysis assimilating satellite observations, we show that the models have large differences in TOA flux, attributable to different geophysical variables. In particular, model simulations continue to diverge from observations in the tropics, as reported in previous studies of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) simulations. The principal culprits are tropical middle and upper tropospheric ozone followed by tropical lower tropospheric H2O. Five models out of the eight studied here have TOA flux biases exceeding 100 mW m−2 attributable to tropospheric ozone bias. Another set of five models have flux biases over 50 mW m−2 due to H2O. On the other hand, Ta radiative bias is negligible in all models (no more than 30 mW m−2). We found that the atmospheric component (AM3) of the Geophysical Fluid Dynamics Laboratory (GFDL) general circulation model and Canadian Middle Atmosphere Model (CMAM) have the lowest TOA flux biases globally but are a result of cancellation of opposite biases due to different processes. Overall, the multi-model ensemble mean bias is −133±98 mW m−2, indicating that they are too atmospherically opaque due to trapping too much radiation in the atmosphere by overestimated tropical tropospheric O3 and H2O. Having too much O3 and H2O in the troposphere would have different impacts on the sensitivity of TOA flux to O3 and these competing effects add more uncertainties on the ozone radiative forcing. We find that the inter-model TOA outgoing longwave radiation (OLR) difference is well anti-correlated with their ozone band flux bias. This suggests that there is significant radiative compensation in the calculation of model outgoing longwave radiation., Atmospheric Chemistry and Physics, 20 (1), ISSN:1680-7375, ISSN:1680-7367

The Convective Precipitation Experiment (COPE) documented the dynamical and microphysical evolution of convection in southwestern England for testing and improving quantitative precipitation forecasting. A strong warm rain process was hypothesized to produce graupel quickly, initiating ice production by rime splintering earlier to increase graupel production and, ultimately, produce heavy rainfall. Here, convection observed on two subsequent days (2 and 3 August 2013) is used to test this hypothesis and illustrate how environmental factors may alter the microphysical progression. The vertical wind shear and cloud droplet number concentrations on 2 August were 2 times those observed on 3 August. Convection on both days produced comparable maximum radar-estimated rain rates, but in situ microphysical measurements indicated much less ice in the clouds on 2 August, despite having maximum cloud tops that were nearly 2 km higher than on 3 August. Idealized 3D numerical simulations of the convection in their respective environments suggest that the relative importance of particular microphysical processes differed. Higher (lower) cloud droplet number concentrations slow (accelerate) the warm rain process as expected, which in turn slows (accelerates) graupel formation. Rime splintering can explain the abundance of ice observed on 3 August, but it was hampered by strong vertical wind shear on 2 August. In the model, the additional ice produced by rime splintering was ineffective in enhancing surface rainfall; strong updrafts on both days lofted supercooled raindrops well above the 0°C level where they froze to become graupel. The results illustrate the complexity of dynamical–microphysical interactions in producing convective rainfall and highlight unresolved issues in understanding and modeling the competing microphysical processes.

Natural methane emissions from wetlands and fire, and soil uptake of methane, simulated using the Canadian Land Surface Scheme and Canadian Terrestrial Ecosystem (CLASS-CTEM) modelling framework, over the historical 1850–2008 period, are assessed by using a one-box model of atmospheric methane burden. This one-box model also requires anthropogenic emissions and the methane sink in the atmosphere to simulate the historical evolution of global methane burden. For this purpose, global anthropogenic methane emissions for the period 1850–2008 were reconstructed based on the harmonized representative concentration pathway (RCP) and Emission Database for Global Atmospheric Research (EDGAR) data sets. The methane sink in the atmosphere is represented using bias-corrected methane lifetimes from the Canadian Middle Atmosphere Model (CMAM). The resulting evolution of atmospheric methane concentration over the historical period compares reasonably well with observation-based estimates (correlation  =  0.99, root mean square error  =  35 ppb). The modelled natural emissions are also assessed using an inverse procedure where the methane lifetimes required to reproduce the observed year-to-year increase in atmospheric methane burden are calculated based upon the specified global anthropogenic and modelled natural emissions that we have used here. These calculated methane lifetimes over the historical period fall within the uncertainty range of observation-based estimates. The present-day (2000–2008) values of modelled methane emissions from wetlands (169 Tg CH4 yr−1) and fire (27 Tg CH4 yr−1), methane uptake by soil (29 Tg CH4 yr−1), and the budget terms associated with overall anthropogenic and natural emissions are consistent with estimates reported in a recent global methane budget that is based on top-down approaches constrained by observed atmospheric methane burden. The modelled wetland emissions increase over the historical period in response to both increases in precipitation and in atmospheric CO2 concentration. This increase in wetland emissions over the historical period yields evolution of the atmospheric methane concentration that compares better with observation-based values than the case when wetland emissions are held constant over the historical period.

The co-occurrence of heat waves and pollution events and the resulting high mortality rates emphasize the importance of the co-occurrence of pollution and temperature extremes. Through the use of extreme value theory and other statistical methods, tropospheric surface ozone and temperature extremes and their joint occurrence are analyzed over the United States during the summer months (JJA) using measurements and simulations of the present and future climate and chemistry. Five simulations from the Chemistry-Climate Model Initiative (CCMI) reference experiment using specified dynamics (REFC1SD) were analyzed: the CESM1 CAM4-chem, CHASER, CMAM, MOCAGE and MRI-ESM1r1 simulations. In addition, a 25-year present-day simulation branched off the CCMI REFC2 simulation in the year 2000 and a 25-year future simulation branched off the CCMI REFC2 simulation in 2100 were analyzed using CESM1 CAM4-chem. The last two simulations differed in their concentration of carbon dioxide (representative of the years 2000 and 2100) but were otherwise identical. In general, regions with relatively high ozone extremes over the US do not occur in regions of relatively high temperature extremes. A new metric, the spectral density, is developed to measure the joint extremal dependence of ozone and temperature by evaluating the spectral dependence of their extremes. While in many areas of the country ozone and temperature are highly correlated overall, the correlation is significantly reduced when examined on the higher end of the distributions. Measures of spectral density are less than about 0.35 everywhere, suggesting that at most only about a third of the time do extreme temperatures coincide with extreme ozone. Two regions of the US have the strongest measured extreme dependence of ozone and temperature: the northeast and the southeast. The simulated future increase in temperature and ozone is primarily due to a shift in their distributions, not to an increase in their extremes. The locations where the right-hand side of the temperature distribution does increase (by up to 30 %) are consistent with locations where soil–moisture feedback may be expected. Future changes in the right-hand side of the ozone distribution range regionally between +20 % and −10 %. The location of future increases in the high-end tail of the ozone distribution are weakly related to those of temperature with a correlation of 0.3. However, the regions where the temperature extremes increase are not located where the extremes in ozone are large, suggesting a muted ozone response.

30 pags., 11 figs., 5 tabs., We quantify the stratospheric injection of brominated very short-lived substances (VSLS) based on aircraft observations acquired in winter 2014 above the Tropical Western Pacific during the CONvective TRansport of Active Species in the Tropics (CONTRAST) and the Airborne Tropical TRopopause EXperiment (ATTREX) campaigns. The overall contribution of VSLS to stratospheric bromine was determined to be 5.0 ± 2.1 ppt, in agreement with the 5 ± 3 ppt estimate provided in the 2014 World Meteorological Organization (WMO) Ozone Assessment report (WMO 2014), but with lower uncertainty. Measurements of organic bromine compounds, including VSLS, were analyzed using CFC-11 as a reference stratospheric tracer. From this analysis, 2.9 ± 0.6 ppt of bromine enters the stratosphere via organic source gas injection of VSLS. This value is two times the mean bromine content of VSLS measured at the tropical tropopause, for regions outside of the Tropical Western Pacific, summarized in WMO 2014. A photochemical box model, constrained to CONTRAST observations, was used to estimate inorganic bromine from measurements of BrO collected by two instruments. The analysis indicates that 2.1 ± 2.1 ppt of bromine enters the stratosphere via inorganic product gas injection. We also examine the representation of brominated VSLS within 14 global models that participated in the Chemistry-Climate Model Initiative. The representation of stratospheric bromine in these models generally lies within the range of our empirical estimate. Models that include explicit representations of VSLS compare better with bromine observations in the lower stratosphere than models that utilize longer-lived chemicals as a surrogate for VSLS., The CONTRAST field deployment was supported by the U.S. NSF, and the ATTREX field deployment was supported by the National Aeronautics and Space Administration (NASA). P. A. W., R. J. S., T. P. C., J. M. N., and D. C. A. received support from NSF, NASA Atmospheric Composition Modeling and Analysis Program (ACMAP), and the NASA Modeling, Analysis, and Prediction (MAP). D. C. A. also received support from the NASA Upper Atmospheric Research Program. J. M. N. was also supported by the NASA Postdoctoral Program at the NASA Goddard Space Flight Center, administered by Universities Space Research Association under contract with NASA. R. V. acknowledges funding from NSF awards AGS‐1261740 and AGS‐1620530. CONTRAST data are publicly available at “http://data.eol.ucar.edu/master_list/?project= CONTRAST.” ATTREX data are publicly available at “https://espoarchive.nasa.gov/archive/browse/attrex/id4/GHawk.” The National Center for Environmental Prediction (NCEP) meteorological data are available at “https://doi.org/10.5065/D6M043C6.” CCMI outputs from CESM1‐WACCM and CESM1‐CAM4Chem are archived by the National Center for Atmospheric Research (NCAR) at “www.earthsystemgrid.org,” and NCAR is sponsored by NSF. CCMI output from the EMAC‐L90MA‐SD simulation is available at “https://doi.org/10.5281/zenodo.1204495.” All other CCMI simulations are archived by the British Atmospheric Data Centre at “http://badc.nerc.ac.uk/”. Output from CAM‐chem‐SD is available as “NCAR/ACD CAMChem 1 Degree Forecast” at “http://catalog.eol.ucar.edu/contrast/model/CAMChem_NCAR_1deg/.” WACCM and CAM‐Chem are components of the Community Earth System Model (CESM), which is also supported by NSF. Computing resources were provided by NCAR's Climate Simulation Laboratory, sponsored by NSF and other agencies. This research was enabled by the computational and storage resources of NCAR's Computational and Information System Laboratory (CISL). R. S. and K. A. S., with ACCESS‐CCM, acknowledge support from Australian Research Council's Centre of Excellence for Climate System Science (CE110001028), the Australian Government's National Computational Merit Allocation Scheme (q90), and Australian Antarctic science grant program (FoRCES 4012). CCSRNIES research was supported by the Environment Research and Technology Development Fund (2‐1303 and 2‐1709) of the Ministry of the Environment, Japan, and computations were performed on NEC‐SX9/A(ECO) computers at the CGER, NIES. The EMAC simulations have been performed at the German Climate Computing Centre (DKRZ) through support from the Bundesministerium für Bildung und Forschung (BMBF). DKRZ and its scientific steering committee are gratefully acknowledged for providing the HPC and data archiving resources for the consortial project ESCiMo (Earth System Chemistry integrated Modelling). The TOMCAT modeling was supported by NERC NCAS and the SISLAC project (NE/R001782/1), and the simulations were performed on the Archer and Leeds HPC Systems.

Formaldehyde (HCHO) directly affects the atmospheric oxidative capacity through its effects on HOx. In remote marine environments, such as the Tropical Western Pacific (TWP), it is particularly important to understand the processes controlling the abundance of HCHO because model output from these regions is used to correct satellite retrievals of HCHO. Here, we have used observations from the CONTRAST field campaign, conducted during January and February 2014, to evaluate our understanding of the processes controlling the distribution of HCHO in the TWP as well as its representation in chemical transport/climate models. Observed HCHO mixing ratios varied from ~500 pptv near the surface to ~75 pptv in the upper troposphere. Recent convective transport of near surface HCHO and its precursors, acetaldehyde and possibly methyl hydroperoxide, increased upper tropospheric HCHO mixing ratios by ~33% (22 pptv); this air contained roughly 60% less NO than more aged air. Output from the CAM-Chem chemistry transport model (2014 meteorology) as well as nine chemistry climate models from the Chemistry-Climate Model Initiative (free-running meteorology) are found to uniformly underestimate HCHO columns derived from in situ observations by between 4 and 50%. This underestimate of HCHO likely results from a near factor of two underestimate of NO in most models, which strongly suggests errors in NOx emissions inventories and/or in the model chemical mechanisms. Likewise, the lack of oceanic acetaldehyde emissions and potential errors in the model acetaldehyde chemistry lead to additional underestimates in modeled HCHO of up to 75 pptv (~15%) in the lower troposphere.

The GEM-MACH-Global model is a global online meteorology-chemistry system currently being developed at the Department of Environment and Climate Change Canada (ECCC). The model is an extension of the Department’s operational, regional GEM-MACH numerical weather and air quality prediction system. The objectives for its development are to improve our understanding of the long range transport and fate of criteria air contaminants, and to improve our forecasting system by providing chemical boundary conditions for the regional air quality forecast system, and background fields for global chemical data assimilation (O3 and NOy species). For this purpose, GEM-MACH-Global was recently updated with a comprehensive photolysis module (JVAL14-MESSy) and a detailed gas-phase chemistry module based on the SAPRC07C mechanism. Compared to its original ADOM2 chemistry mechanism, the revised gas-phase chemistry is more explicit, with new species and ~15 additional reactions important in the upper troposphere and lower stratosphere (UTLS) region. Furthermore, a lightning emission module was incorporated to represent NOx emissions aloft. These changes were evaluated with a 2010 annual simulation on a 400 × 200 global-grid. The simulation included inputs from 2010 HTAP global anthropogenic emissions, GFEDv3 biomass burning emissions and ECCC’s operational meteorological analyses. The presentation will describe the current state-of-science development of GEM-MACH-Global and show comparisons results of the annual simulation.

Here we provide an overview of the REF-C1SD Specified-Dynamics experiment that was conducted as part of Phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly online general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and we evaluate how well the simulations represent different measures of the dynamical and transport circulations. In the troposphere there are large (~ 40 %) differences in the climatological mean distributions and seasonal cycle amplitude of the meridional and vertical winds. In the stratosphere there are similarly large (~ 50 %) differences in the magnitude and seasonal cycle amplitude of the Transformed Eulerian Mean circulation and among various chemical and idealized tracers. For nearly all variables these differences are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. Furthermore, in most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition.

Climate model simulations show an acceleration of the Brewer–Dobson circulation (BDC) in response to climate change. While the general mechanisms for the BDC strengthening are widely understood, there are still open questions concerning the influence of the details of the wave driving. Mean age of stratospheric air (AoA) is a useful transport diagnostic for assessing changes in the BDC. Analyzing AoA from a subset of Chemistry–Climate Model Initiative part 1 climate projection simulations, we find a remarkable agreement between most of the models in simulating the largest negative AoA trends in the extratropical lower to middle stratosphere of both hemispheres (approximately between 20 and 25 geopotential kilometers (gpkm) and 20–50∘ N and S). We show that the occurrence of AoA trend minima in those regions is directly related to the climatological AoA distribution, which is sensitive to an upward shift of the circulation in response to climate change. Also other factors like a reduction of aging by mixing (AbM) and residual circulation transit times (RCTTs) contribute to the AoA distribution changes by widening the AoA isolines. Furthermore, we analyze the time evolution of AbM and RCTT trends in the extratropics and examine the connection to possible drivers focusing on local residual circulation strength, net tropical upwelling and wave driving. However, after the correction for a vertical shift of pressure levels, we find only seasonally significant trends of residual circulation strength and zonal mean wave forcing (resolved and unresolved) without a clear relation between the trends of the analyzed quantities. This indicates that additional causative factors may influence the AoA, RCTT and AbM trends. In this study, we postulate that the shrinkage of the stratosphere has the potential to influence the RCTT and AbM trends and thereby cause additional AoA changes over time. Czech Science Foundation (GACˇ R) | Ref. 16- 01562J Czech Science Foundation (GACˇ R) | Ref. 18-01625S Ministerio de Ciencia e Innovación | Ref. CGL2015-71575-P Xunta de Galicia | Ref. ED481B 2018/103 Ministerio de Economía y Competitividad | Ref. RYC-2013-14560

Transport from the Northern Hemisphere (NH) midlatitudes to the Arctic plays a crucial role in determining the abundance of trace gases and aerosols that are important to Arctic climate via impacts on radiation and chemistry. Here we examine this transport using an idealized tracer with a fixed lifetime and predominantly midlatitude land-based sources in models participating in the Chemistry Climate Model Initiative (CCMI). We show that there is a 25 %–45 % difference in the Arctic concentrations of this tracer among the models. This spread is correlated with the spread in the location of the Pacific jet, as well as the spread in the location of the Hadley Cell (HC) edge, which varies consistently with jet latitude. Our results suggest that it is likely that the HC-related zonal-mean meridional transport rather than the jet-related eddy mixing is the major contributor to the inter-model spread in the transport of land-based tracers into the Arctic. Specifically, in models with a more northern jet, the HC generally extends further north and the tracer source region is mostly covered by surface southward flow associated with the lower branch of the HC, resulting in less efficient transport poleward to the Arctic. During boreal summer, there are poleward biases in jet location in free-running models, and these models likely underestimate the rate of transport into the Arctic. Models using specified dynamics do not have biases in the jet location, but do have biases in the surface meridional flow, which may result in differences in transport into the Arctic. In addition to the land-based tracer, the midlatitude-to-Arctic transport is further examined by another idealized tracer with zonally uniform sources. With equal sources from both land and ocean, the inter-model spread of this zonally uniform tracer is more related to variations in parameterized convection over oceans rather than variations in HC extent, particularly during boreal winter. This suggests that transport of land-based and oceanic tracers or aerosols towards the Arctic differs in pathways and therefore their corresponding inter-model variabilities result from different physical processes.

An analysis of the microphysical structure of elevated convection within the comma head region of two winter cyclones over the midwestern United States is presented using data from the Wyoming Cloud Radar (WCR) and microphysical probes on the NSF/NCAR C-130 aircraft during the Profiling of Winter Storms campaign. The aircraft penetrated 36 elevated convective cells at various temperatures T and distances below cloud top zd. The statistical properties of ice water content (IWC), liquid water content (LWC), ice particle concentration with diameter > 500 μm N>500, and median mass diameter Dmm, as well as particle habits within these cells were determined as functions of zd and T for active updrafts and residual stratiform regions originating from convective towers that ascended through unsaturated air. Insufficient data were available for analysis within downdrafts. For updrafts stratified by zd, distributions of IWC, N>500, and Dmm for all zd between 1000 and 4000 m proved to be statistically indistinct. These results imply that turbulence and mixing within the updrafts effectively distributed particles throughout their depths. A decrease in IWC and N>500 in the layer closest to cloud top was likely related to cloud-top entrainment. Within residual stratiform regions, decreases in IWC and N>500 and increases in Dmm were observed with depth below cloud top. These trends are consistent with particles falling and aggregating while entrainment and subsequent sublimation was occurring.

Since the advent of dual-polarization radar, methods of classifying hydrometeors by type from measured polarization variables have been developed. The deterministic approach of existing hydrometeor classification algorithms of assigning only one dominant habit to each radar sample volume does not properly consider the distribution of habits present in that volume, however. During the Profiling of Winter Storms field campaign, the “NSF/NCAR C-130” aircraft, equipped with in situ microphysical probes, made multiple passes through the comma heads of two cyclones as the Mobile Alabama X-band dual-polarization radar performed range–height indicator scans in the same plane as the C-130 flight track. On 14–15 February and 21–22 February 2010, 579 and 202 coincident data points, respectively, were identified when the plane was within 10 s (~1 km) of a radar gate. For all particles that occurred for times within different binned intervals of radar reflectivity ZHH and of differential reflectivity ZDR, the reflectivity-weighted contribution of each habit and the frequency distributions of axis ratio and sphericity were determined. This permitted the determination of habits that dominate particular ZHH and ZDR intervals; only 40% of the ZHH–ZDR bins were found to have a habit that contributes over 50% to the reflectivity in that bin. Of these bins, only 12% had a habit that contributes over 75% to the reflectivity. These findings show the general lack of dominance of a given habit for a particular ZHH and ZDR and suggest that determining the probability of specific habits in radar volumes may be more suitable than the deterministic methods currently used.

The Convective Precipitation Experiment (COPE) was a joint U.K.–U.S. field campaign held during the summer of 2013 in the southwest peninsula of England, designed to study convective clouds that produce heavy rain leading to flash floods. The clouds form along convergence lines that develop regularly as a result of the topography. Major flash floods have occurred in the past, most famously at Boscastle in 2004. It has been suggested that much of the rain was produced by warm rain processes, similar to some flash floods that have occurred in the United States. The overarching goal of COPE is to improve quantitative convective precipitation forecasting by understanding the interactions of the cloud microphysics and dynamics and thereby to improve numerical weather prediction (NWP) model skill for forecasts of flash floods. Two research aircraft, the University of Wyoming King Air and the U.K. BAe 146, obtained detailed in situ and remote sensing measurements in, around, and below storms on several days. A new fast-scanning X-band dual-polarization Doppler radar made 360° volume scans over 10 elevation angles approximately every 5 min and was augmented by two Met Office C-band radars and the Chilbolton S-band radar. Detailed aerosol measurements were made on the aircraft and on the ground. This paper i) provides an overview of the COPE field campaign and the resulting dataset, ii) presents examples of heavy convective rainfall in clouds containing ice and also in relatively shallow clouds through the warm rain process alone, and iii) explains how COPE data will be used to improve high-resolution NWP models for operational use.

Analyses of the radar-observed structure and derived rainfall statistics of warm-season convection developing columns of enhanced positive differential reflectivity ZDR over England’s southwest peninsula are presented here. Previous observations of ZDR columns in developing cumulonimbus clouds over England were rare. The observations presented herein suggest otherwise, at least in the southwesterly winds over the peninsula. The results are the most extensive of their kind in the United Kingdom; the data were collected using the National Centre for Atmospheric Science dual-polarization X-band radar (NXPol) during the Convective Precipitation Experiment (COPE). In contrast to recent studies of ZDR columns focused on deep clouds that developed in high-instability environments, the COPE measurements show relatively frequent ZDR columns in shallower clouds, many only 4–5 km deep. The presence of ZDR columns is used to infer that an active warm rain process has contributed to precipitation evolution in convection deep enough for liquid and ice growth to take place. Clouds with ZDR columns were identified objectively in three COPE deployments, with both discrete convection and clouds embedded in larger convective complexes developing columns. Positive ZDR values typically extended to 1–1.25 km above 0°C in the columns, with ZDR ≥ 1 dB sometimes extending nearly 4 km above 0°C. Values above 3 dB typically occurred in the lowest 500 m above 0°C, with coincident airborne measurements confirming the presence of supercooled raindrops. Statistical analyses indicated that the convection that produced ZDR columns was consistently associated with the larger derived rainfall rates when compared with the overall convective population sampled by the NXPol during COPE.

The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades, but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability and changes, and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified dynamics chemistry-climate model (CCM) simulations from the ECHAM/MESSy Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the IGAC/SPARC Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozonesonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (~ 0–5.5 km) subcolumn ozone is found for EMAC, ranging from 2–8 Dobson Units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (~ −4 to +4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozonesondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with an underestimation of photochemical ozone production (negative bias) in the troposphere. Model variability is found to be more similar in magnitude to that implied from ozonesondes, in comparison with OMI which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is shown that CMAM simulates a faster and shallower Brewer-Dobson Circulation (BDC) relative to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone, over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is larger than previously thought and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long term changes in the CCM ozone tracers are calculated for different seasons between 1980–89 and 2001–10. An overall statistically significant increase in tropospheric ozone is found across much of the world, but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5–10 %). Our model study implies that attribution from stratosphere-troposphere exchange (STE) to such ozone changes ranges from 25–30 % at the surface to as much as 50–80 % in the upper troposphere-lower stratosphere (UTLS) across many regions of the world. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere.

Climate models consistently predict an acceleration of the Brewer-Dobson circulation (BDC) due to climate change in the 21st century. However, the strength of this acceleration varies considerably among individual models, which constitutes a notable source of uncertainty for future climate projections. To shed more light upon the magnitude of this uncertainty and on its causes, we analyze the stratospheric mean age of air (AoA) of 10 climate projection simulations from the Chemistry Climate Model Initiative phase 1 (CCMI-I), covering the period between 1960 and 2100. In agreement with previous multi-model studies, we find a large model spread in the magnitude of the AoA trend over the simulation period. Differences between future and past AoA are found to be predominantly due to differences in mixing (reduced aging by mixing and recirculation) rather than differences in residual mean transport. We furthermore analyze the mixing efficiency, a measure of the relative strength of mixing for given residual mean transport, which was previously hypothesized to be a model constant. Here, the mixing efficiency is found to vary not only across models, but also over time in all models. Changes in mixing efficiency are shown to be closely related to changes in AoA and quantified to roughly contribute 10 % to the long-term AoA decrease over the 21st century. Additionally, mixing efficiency variations are shown to considerably enhance model spread in AoA changes. To understand these mixing efficiency variations, we also present a consistent dynamical framework based on diffusive closure, which highlights the role of basic state potential vorticity gradients in controlling mixing efficiency and therefore aging by mixing.