Products of Criegee Intermediate Reactions with NO2: Experimental Measurements and Tropospheric Implications.
Abstract not provided.
Caravan, Rebecca Louise↗
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Role of Troposphere-Convection-Land Coupling in the Southwestern Amazon Precipitation Bias of the Community Earth System Model version 1 (CESM1)
The Amazon forest plays an important role in the tropical circulation and global water and biogeochemical cycles. However, the common Amazon precipitation biases in global climate models undermine our ability to understand future changes in the Amazon and their global consequences. The Community Earth System Model exhibits a persistent wet season dry bias over the southwestern Amazon. The bias is also characterized by inaccurate diurnal timing and intensity of rainfall events. Analysis of a diverse set of simulations suggests that the bias originates from local processes. A known land model bias in the partitioning of surface energy fluxes is found not to contribute significantly to the rainfall bias. Key model processes are identified to be the low-level divergent circulation controlling horizontal moisture flow and the sensitivity of the modeled deep convection to the lower tropospheric moisture. The lower tropospheric moisture divergence dictates the spatiotemporal distributions of convective precipitation through parameterized entrainment mixing, which generally improves the rainfall diurnal cycle. However, it also limits convective precipitation over the areas with frequent and large-scale divergence in the lower troposphere. The southwestern Amazon is such an area, particularly in the late afternoon, although uncertainty exists in the low-level flow in the simulation and reanalyses. One way to sustain rainfall in the presence of low-level divergence is a convective trigger based on both the moisture and temperature changes by large-scale processes, which is shown to help in reducing the dry bias.
Sakaguchi, Koichi↗
A review of the remote sensing of lower tropospheric thermodynamic profiles and its indispensable role for the understanding and the simulation of water and energy cycles: REMOTE SENSING OF THERMODYNAMIC PROFILES
A review of remote sensing technology for lower tropospheric thermodynamic (TD) profiling is presented with focus on high accuracy and high temporal-vertical resolution. The contributions of these instruments to the understanding of the Earth system are assessed with respect to radiative transfer, land surface-atmosphere feedback, convection initiation, and data assimilation. We demonstrate that for progress in weather and climate research, TD profilers are essential. These observational systems must resolve gradients of humidity and temperature in the stable or unstable atmospheric surface layer close to the ground, in the mixed layer, in the interfacial layer—usually characterized by an inversion—and the lower troposphere. A thorough analysis of the current observing systems is performed revealing significant gaps that must be addressed to fulfill existing needs. We analyze whether current and future passive and active remote sensing systems can close these gaps. A methodological analysis and demonstration of measurement capabilities with respect to bias and precision is executed both for passive and active remote sensing including passive infrared and microwave spectroscopy, the global navigation satellite system, as well as water vapor and temperature Raman lidar and water vapor differential absorption lidar. Whereas passive remote sensing systems are already mature with respect to operational applications, active remote sensing systems require further engineering to become operational in networks. However, active remote sensing systems provide a smaller bias as well as higher temporal and vertical resolutions. For a suitable mesoscale network design, TD profiler system developments should be intensified and dedicated observing system simulation experiments should be performed.
58 GEOSCIENCES↗
Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016
The southeast Atlantic is home to well-defined smoke outflow from Africa coinciding vertically with extensive marine boundary-layer cloud decks, both reaching their climatological maxima in spatial extent around September. A framework is put forth for evaluating the performance of a range of global and regional aerosol models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. The sparse airborne observations are first aggregated into 2o grid boxes and into three vertical layers: the cloud-topped marine boundary layer (MBL), the layer from cloud top to 3 km, and the 3-6 km layer. Aerosol extensive properties simulated for the entire study region for all September suggest that the 2016 ORACLES observations are reasonably representative of the regional monthly average, with systematic deviations of 30% or less. All six models typically place the bottom of the smoke layer at lower altitudes than do the airborne lidar observations by 300-1400 m, whereas model aerosol top heights are within 0-500 m of the observations. All but one of the models that report carbonaceous aerosol masses underestimate the ratio of particulate extinction to the masses, a proxy for mass extinction efficiency, in 3-6 km. Notable findings on individual models include that WRF-CAM5 predicts the mass of black carbon and organic aerosols with minor (~10% or less) biases. GEOS-5 overestimates the carbonaceous particle masses in the MBL by a factor of 3-6. Extinction coefficients in the free troposphere (FT) and above-cloud aerosol optical depth (ACAOD) are 10-30% lower in WRF-CAM5, 30-50% lower in GEOS-5, 10-40% higher in GEOS-Chem, 10-20% higher in EAM-E3SM except for the practically unbiased 3-6 km extinction, and 20-70% lower in the Unified Model, than the airborne in situ, lidar and sunphotometer measurements. ALADIN-Climate also underestimates the ACAOD, by 30%. GEOS-5 and GEOS-Chem predict carbon monoxide in the MBL with small (10% or less) negative biases, despite their overestimates of carbonaceous aerosol masses. Overall, this study highlights a new approach to utilizing airborne aerosol measurements for model diagnosis.
Shinozuka, Yohei↗
Exploring mechanisms of a tropospheric archetype: CH{sub 3}O{sub 2} + NO
Methylperoxy radical (CH{sub 3}O{sub 2}) and nitric oxide (NO) contribute to the propagation of photochemical smog in the troposphere via the production of methoxy radical (CH{sub 3}O) and nitrogen dioxide (NO{sub 2}). This reaction system also furnishes trace quantities of methyl nitrate (CH{sub 3}ONO{sub 2}), a sink for reactive NO{sub x} species. Here, the CH{sub 3}O{sub 2} + NO reaction is examined with highly reliable coupled-cluster methods. Specifically, equilibrium geometries for the reactants, products, intermediates, and transition states of the ground-state potential energy surface are characterized. Relative reaction enthalpies at 0 K (ΔH{sub 0K}) are reported; these values are comprised of electronic energies extrapolated to the complete basis set limit of CCSDT(Q) and zero-point vibrational energies computed at CCSD(T)/cc-pVTZ. A two-part mechanism involving CH{sub 3}O and NO{sub 2} production followed by radical recombination to CH{sub 3}ONO{sub 2} is determined to be the primary channel for formation of CH{sub 3}ONO{sub 2} under tropospheric conditions. Constrained optimizations of the reaction paths at CCSD(T)/cc-pVTZ suggest that the homolytic bond dissociations involved in this reaction path are barrierless.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Physicochemical and Molecular Insights into the Boundary Layer and Free Troposphere Aerosol Interactions over the Southern Great Plains
Ambient aerosols’ vertical profiles are critical for evaluating the role of aerosols in atmospheric chemistry and radiative transfer, but limited data on these profiles hinders our ability to fully assess their impact on the Earth's radiative balance. Here, in this study, we investigated the size-, time-, and altitude resolved composition of individual particles and bulk molecular composition of particle samples collected by an uncrewed aerial system–ArcticShark over the Southern Great Plains. Single particle microanalysis shows that, the free tropospheric (FT) samples are dominated (56-66%) by carbonaceous sulfate particles, while boundary layer (BL) samples are dominated (57-74%) by carbonaceous particles. Back trajectory simulations suggest that FT particles are likely influenced by long-range transport and have undergone aqueous-phase processing. Conversely, in-situ size distribution data shows evidence of particle growth in the upper BL and just below the FT. This observation may indicate vertical transport of particles from an elevated aerosol layer in the FT, possibly linked to a new particle formation event. This observation is further supported by high resolution molecular composition data, which reveals particle volatility increasing with increasing size, which aligns with the growth event. This study aids in fundamental understanding of the compositional and molecular specificity of vertically resolved organic aerosols to provide insights into particle size evolution for future atmospheric models.
ArcticShark↗
Ensemble simulations of the role of the stratosphere in the attribution of northern extratropical tropospheric ozone variability
Despite the need to understand the impact of changes in emissions and climate on tropospheric ozone, the attribution of tropospheric interannual ozone variability to specific processes has proven difficult. Here, we analyze the stratospheric contribution to tropospheric ozone variability and trends from 1953 to 2005 in the Northern Hemisphere (NH) mid-latitudes using four ensemble simulations of the free running (FR) Whole Atmosphere Community Climate Model (WACCM). The simulations are externally forced with observed time-varying (1) sea-surface temperatures (SSTs), (2) greenhouse gases (GHGs), (3) ozone depleting substances (ODS), (4) quasi-biennial oscillation (QBO), (5) solar variability (SV) and (6) stratospheric sulfate surface area density (SAD). A detailed representation of stratospheric chemistry is simulated, including the ozone loss due to volcanic eruptions and polar stratospheric clouds. In the troposphere, ozone production is represented by CH 4 –NO x smog chemistry, where surface chemical emissions remain interannually constant. Despite the simplicity of its tropospheric chemistry, at many NH measurement locations, the interannual ozone variability in the FR WACCM simulations is significantly correlated with the measured interannual variability. This suggests the importance of the external forcing applied in these simulations in driving interannual ozone variability. The variability and trend in the simulated 1953–2005 tropospheric ozone from 30 to 90° N at background surface measurement sites, 500 hPa measurement sites and in the area average are largely explained on interannual timescales by changes in the 30–90° N area averaged flux of ozone across the 100 hPa surface and changes in tropospheric methane concentrations. The average sensitivity of tropospheric ozone to methane (percent change in ozone to a percent change in methane) from 30 to 90° N is 0.17 at 500 hPa and 0.21 at the surface; the average sensitivity of tropospheric ozone to the 100 hPa ozone flux (percent change in ozone to a percent change in the ozone flux) from 30 to 90° N is 0.19 at 500 hPa and 0.11 at the surface. The 30–90° N simulated downward residual velocity at 100 hPa increased by 15% between 1953 and 2005. Yet, the impact of this on the 30–90° N 100 hPa ozone flux is modulated by the long-term changes in stratospheric ozone. The ozone flux decreases from 1965 to 1990 due to stratospheric ozone depletion, but increases again by approximately 7% from 1990 to 2005. The first empirical orthogonal function of interannual ozone variability explains from 40% (at the surface) to over 80% (at 150 hPa) of the simulated ozone interannual variability from 30 to 90° N. This identified mode of ozone variability shows strong stratosphere–troposphere coupling, demonstrating the importance of the stratosphere in an attribution of tropospheric ozone variability. The simulations, with no change in emissions, capture almost 50% of the measured ozone change during the 1990s at a variety of locations. This indicates that a large portion of the measured change is not due to changes in emissions, but can be traced to changes in large-scale modes of ozone variability. This emphasizes the difficulty in the attribution of ozone changes, and the importance of natural variability in understanding the trends and variability of ozone. We find little relation between the El Niño–Southern Oscillation (ENSO) index and large-scale tropospheric ozone variability over the long-term record.
54 ENVIRONMENTAL SCIENCES↗
Description and evaluation of tropospheric chemistry and aerosols in the Community Earth System Model (CESM1.2)
The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. The main focus of this paper is to compare the performance of configurations with internally derived "free running" (FR) meteorology and "specified dynamics" (SD) against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We focus on the representation of aerosols and chemistry. All model configurations reproduce tropospheric ozone for most regions based on in situ and satellite observations. However, shortcomings exist in the representation of ozone precursors and aerosols. Tropospheric ozone in all model configurations agrees for the most part with ozonesondes and satellite observations in the tropics and the Northern Hemisphere within the variability of the observations. Southern hemispheric tropospheric ozone is consistently underestimated by up to 25%. Differences in convection and stratosphere to troposphere exchange processes are mostly responsible for differences in ozone in the different model configurations. Carbon monoxide (CO) and other volatile organic compounds are largely underestimated in Northern Hemisphere mid-latitudes based on satellite and aircraft observations. Nitrogen oxides (NO x ) are biased low in the free tropical troposphere, whereas peroxyacetyl nitrate (PAN) is overestimated in particular in high northern latitudes. The present-day methane lifetime estimates are compared among the different model configurations. These range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem and are therefore underestimated compared to observational estimations. We find that differences in tropospheric aerosol surface area between CAM4 and CAM5 play an important role in controlling the burden of the tropical tropospheric hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of NO x from lightning explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss but also by transport and mixing. For future studies, we recommend the use of CAM5-chem configurations, due to improved aerosol description and inclusion of aerosol–cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.
54 ENVIRONMENTAL SCIENCES↗
Comparing the Effect of Anthropogenically Amplified Halogen Natural Emissions on Tropospheric Ozone Chemistry Between Pre-Industrial and Present-Day
Reactive halogens (X + XO, X = I, Br or Cl) catalytically destroy a fraction of tropospheric ozone under present-day (PD) conditions, however, their distribution and potential impact on tropospheric ozone under pre-industrial (PI) conditions remain largely unexplored. This study uses the Community Atmosphere Model with Chemistry (CAM-Chem) to investigate the effect of anthropogenically amplified natural emissions of halogenated species and their subsequent chemistry on tropospheric ozone under PI and PD atmospheric conditions. Model results show that the global tropospheric ozone depletion due to natural halogens is slightly more sensitive in PI than PD, with percentage changes in tropospheric ozone burden (TOB) of -14.1 ± 0.6% for PI and -12.9 ± 0.6% for PD. Individually, the role of iodine and chlorine in ozone depletion is equivalent in both periods (ΔTOB I : ~-7% and ΔTOB Cl : ~-2.5%), while bromine plays a larger role in PI (ΔTOB Br : -5.5 ± 0.6%) versus PD (ΔTOB Br : -4.3 ± 0.7%). The increase in anthropogenic ozone precursor emissions from PI to PD has amplified the natural emission of inorganic halogens and led to a shift in the partitioning of inorganic halogens from reactive to reservoir species. Consequently, halogen-driven ozone depletion from the surface to the free troposphere is larger in PI than PD. In contrast, in the upper troposphere, the ozone depletion is larger in PD influenced mainly by stratospheric intrusion of reactive halogens from long-lived species. This study highlights the importance of including a complete chemical coupling of natural halogens and atmospheric pollutants in chemistry-climate models to adequately assess their effects on tropospheric ozone in a changing climate.
54 ENVIRONMENTAL SCIENCES↗
Molecular and physical characteristics of aerosol at a remote free troposphere site: implications for atmospheric aging
Aerosol properties are transformed by atmospheric processes during long-range transport and play a key role in the Earth's radiative balance. To understand the molecular and physical characteristics of free tropospheric aerosol, we studied samples collected at the Pico Mountain Observatory in the North Atlantic. The observatory is located in the marine free troposphere at 2225 m above sea level, on Pico Island in the Azores archipelago. The site is ideal for the study of long-range-transported free tropospheric aerosol with minimal local influence. Three aerosol samples with elevated organic carbon concentrations were selected for detailed analysis. FLEXPART retroplumes indicated that two of the samples were influenced by North American wildfire emissions transported in the free troposphere and one by North American outflow mainly transported within the marine boundary layer.Ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry was used to determine the detailed molecular composition of the samples. Thousands of molecular formulas were assigned to each of the individual samples. On average ~60 % of the molecular formulas contained only carbon, hydrogen, and oxygen atoms (CHO), ~30 %contained nitrogen (CHNO), and ~10 % contained sulfur (CHOS). The molecular formula compositions of the two wildfire-influenced aerosol samples transported mainly in the free troposphere had relatively low averageO/C ratios (0.48±0.13 and 0.45±0.11) despite the 7–10 days of transport time according to FLEXPART. In contrast, the molecular composition of the North American outflow transported mainly in the boundary layer had a higher average O/C ratio (0.57±0.17) with 3 days of transport time. To better understand the difference between free tropospheric transport and boundary layer transport, the meteorological conditions along the FLEXPART simulated transport pathways were extracted from the Global Forecast System analysis for the model grids. We used the extracted meteorological conditions and the observed molecular chemistry to predict the relative-humidity-dependent glass transition temperatures (T g ) of the aerosol components. Comparisons of the T g to the ambient temperature indicated that a majority of the organic aerosol components transported in the free troposphere were more viscous and therefore less susceptible to oxidation than the organic aerosol components transported inthe boundary layer. Although the number of observations is limited, the results suggest that biomass burning organic aerosol injected into the free troposphere is more persistent than organic aerosol in the boundary layer having broader implications for aerosol aging.
54 ENVIRONMENTAL SCIENCES↗
Arctic tropospheric ozone: assessment of current knowledge and model performance
As the third most important greenhouse gas (GHG) after carbon dioxide (CO 2 ) and methane (CH 4 ), tropospheric ozone (O 3 ) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O 3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O 3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O 3 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 O 3 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 O 3 and its precursor species. The MMM underestimates Arctic surface O 3 by 5% to 15% depending on the location. The vertical distribution of tropospheric O 3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O 3 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 O 3 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 O 3 at high latitudes. For example, the MMM is biased high by about 20% at Eureka. Observed and simulated O 3 precursors (CO, NO x , 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 NO x but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O 3 matches the observed O 3 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 O 3 .
54 ENVIRONMENTAL SCIENCES↗
Quantifying isentropic stratosphere-troposphere exchange of ozone
There is increased evidence that stratosphere-troposphere exchange (STE) of ozone has a significant impact on tropospheric chemistry and radiation. Traditional diagnostics of STE consider the ozone budget in the lowermost stratosphere (LMS) as a whole. However, this can only render the hemispherically integrated ozone flux and therefore does not distinguish the exchange of ozone into low latitudes from that into high latitudes. The exchange of ozone at different latitudes may have different tropospheric impacts. This present study extends the traditional approach from the entire LMS to individual isentropic layers in the LMS and therefore gives the meridional distribution of STE by the latitudes where each isentropic surface intersects the tropopause. The specified dynamics version of the Whole Atmosphere Community Climate Model is used to estimate the STE ozone flux on each isentropic surface. It is found that net troposphere-to-stratosphere ozone transport occurs in low latitudes along the 350–380 K isentropic surfaces and that net stratosphere-to-troposphere ozone transport takes place in the extratropics along the 280–350 K isentropes. Particularly, the seasonal cycle of extratropical STE ozone flux in the Northern Hemisphere displays a maximum in late spring and early summer, following the seasonal migration of the upper tropospheric jet and associated isentropic mixing. Moreover, differential diabatic heating and isentropic mixing tend to induce STE ozone fluxes in opposite directions, but the net effect results in a spatiotemporal pattern similar to the STE ozone flux associated with isentropic mixing.
54 ENVIRONMENTAL SCIENCES↗
Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI
Abstract Acetic acid (CH 3 COOH) is one of the most abundant carboxylic acids in the troposphere. In the study, the tropospheric chemistry of CH 3 COOH is investigated using the 3‐D global chemistry transport model, STOCHEM‐CRI. The highest mixing ratios of surface CH 3 COOH are found in the tropics by as much as 1.6 ppb in South America. The model predicts the seasonality of CH 3 COOH reasonably well and correlates with some surface and flight measurement sites, but the model drastically underpredicts levels in urban and midlatitudinal regions. The possible reasons for the underprediction are discussed. The simulations show that the lifetime and global burden of CH 3 COOH are 1.6–1.8 days and 0.45–0.61 Tg, respectively. The reactions of the peroxyacetyl radical (CH 3 CO 3 ) with the hydroperoxyl radical (HO 2 ) and other organic peroxy radicals (RO 2 ) are found to be the principal sources of tropospheric CH 3 COOH in the model, but the model‐measurement discrepancies suggest the possible unknown or underestimated sources which can contribute large fractions of the CH 3 COOH burden. The major sinks of CH 3 COOH in the troposphere are wet deposition, dry deposition, and OH loss. However, the reaction of CH 3 COOH with Criegee intermediates is proposed to be a potentially significant chemical loss process of tropospheric CH 3 COOH that has not been previously accounted for in global modeling studies. Inclusion of this loss process reduces the tropospheric CH 3 COOH level significantly which can give even larger discrepancies between model and measurement data, suggesting that the emissions inventory and the chemical production sources of CH 3 COOH are underpredicted even more so in current global models.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A process-based evaluation of biases in extratropical stratosphere–troposphere coupling in subseasonal forecast systems
Abstract. Two-way coupling between the stratosphere and troposphere is recognized as an important source of subseasonal-to-seasonal (S2S) predictability and can open windows of opportunity for improved forecasts. Model biases can, however, lead to a poor representation of such coupling processes; drifts in a model's circulation related to model biases, resolution, and parameterizations have the potential to feed back on the circulation and affect stratosphere–troposphere coupling. We introduce a set of diagnostics using readily available data that can be used to reveal these biases and then apply these diagnostics to 22 S2S forecast systems. In the Northern Hemisphere, nearly all S2S forecast systems underestimate the strength of the observed upward coupling from the troposphere to the stratosphere, downward coupling within the stratosphere, and the persistence of lower-stratospheric temperature anomalies. While downward coupling from the lower stratosphere to the near surface is well represented in the multi-model ensemble mean, there is substantial intermodel spread likely related to how well each model represents tropospheric stationary waves. In the Southern Hemisphere, the stratospheric vortex is oversensitive to upward-propagating wave flux in the forecast systems. Forecast systems generally overestimate the strength of downward coupling from the lower stratosphere to the troposphere, even as most underestimate the radiative persistence in the lower stratosphere. In both hemispheres, models with higher lids and a better representation of tropospheric quasi-stationary waves generally perform better at simulating these coupling processes.
Garfinkel, Chaim I. (ORCID:000000017258666X)↗
The Radiative Role of Free Tropospheric Aerosols and Marine Clouds over the Central North Atlantic
The scientific scope of the project was to exploit the unique location of the Pico Mountain Observatory (PMO) located in the summit caldera of the Pico Volcano in Pico Island in the Azores, for atmospheric studies. The observatory, located at 2225m a.s.l., typically samples free tropospheric aerosols laying above the marine low-level clouds and long-range transported from North America. The broad purpose of this research was to provide the scientific community with a better understanding of fundamental physical processes governing the effects of aerosols on radiative forcing and climate; with the ultimate goal of improving our abilities to understand past climate and to predict future changes through numerical models. The project was 'exploratory' in nature, with the plan to demonstrate the feasibility of deploying for the first time, an extensive aerosol research package at PMO. One of the primary activities was to test the deployment of these instruments at the site, to collect data during the 2012 summer season, and to further develop the infrastructure and the knowledge for performing novel research at PMO in follow-up longer-term aerosol-cloud studies. In the future, PMO could provide an elevated research outpost to support the renewed DOE effort in the Azores that was intensified in 2013 with the opening of the new sea-level ARM-DOE Eastern North Atlantic permanent facility at Graciosa Island. During the project period, extensive new data sets were collected for the planned 2012 season. Thanks to other synergistic activities and opportunities, data collection was then successfully extended to 2013 and 2014. Highlights of the scientific findings during this project include: a) biomass burning contribute significantly to the aerosol loading in the North Atlantic free troposphere; however, long-range transported black carbon concentrations decreased substantially in the last decade. b) Single black carbon particles – analyzed off-line at the electron microscope – were often very compacted, suggesting cloud processing and exhibiting different optical properties from fresh emissions. In addition, black carbon was found to be sometimes mixed with mineral dust, affecting its optical properties and potential forcing. c) Some aerosols collected at PMO acted as ice nuclei, potentially contributing to cirrus cloud formation during their transport in the upper free troposphere. Identified good ice nuclei were often mineral dust particles. d) The free tropospheric aerosols studied at PMO have relevance to low level marine clouds due, for example, to synoptic subsidence entraining free tropospheric aerosols into the marine boundary layer. This has potentially large consequences on cloud condensation nuclei concentrations and compositions in the marine boundary layer; therefore, having an effect on the marine stratus clouds, with potentially important repercussions on the radiative forcing. The scientific products of this project currently include contributions to two papers published in the Nature Publishing group (Nature Communications and Scientific Reports), one paper under revision for Atmospheric Chemistry and Physics, one in review in Geophysical Research Letters and one recently submitted to Atmospheric Chemistry and Physics Discussion. In addition, four manuscripts are in advanced state of preparation. Finally, twenty-eight presentations were given at international conferences, workshops and seminars.
54 ENVIRONMENTAL SCIENCES↗
Stratosphere-Troposphere Coupling of Extreme Stratospheric Wave Activity in CMIP6 Models
Extreme stratospheric wave activity has been suggested to be connected to surface temperature anomalies, but some key processes are not well understood. Using observations, we show that the stratospheric events featuring weaker-than-normal wave activity are associated with increased North American (NA) cold extreme risks before and near the event onset, accompanied by less frequent atmospheric river (AR) events on the west coast of the United States. Strong stratospheric wave events, on the other hand, exhibit a tropospheric weather regime transition. Further, they are preceded by NA warm anomalies and increased AR frequency over the west coast, followed by increased risks of NA cold extremes and north-shifted ARs over the Atlantic. Moreover, these links between the stratosphere and troposphere are attributed to the vertical structure of wave coupling. Weak wave events show a wave structure of westward tilt with increasing altitudes, while strong wave events feature a shift from westward tilt to eastward tilt during their life cycle. This wave phase shift indicates vertical wave coupling and likely regional planetary wave reflection. Further examinations of CMIP6 models show that models with a degraded representation of stratospheric wave structure exhibit biases in the troposphere during strong wave events. Specifically, models with a stratospheric ridge weaker than the reanalysis exhibit a weaker tropospheric signal. Our findings suggest that the vertical coupling of extreme stratospheric wave activity should be evaluated in the model representation of stratosphere-troposphere coupling.
54 ENVIRONMENTAL SCIENCES↗
Upper troposphere dust belt formation processes vary seasonally and spatially in the Northern Hemisphere
Dust aerosols impact global energy balance substantially by acting as efficient ice nuclei to alter cold cloud properties. However, the estimate of dust indirect effect remains uncertain due to simulating dust distributions poorly and lacking reliable dust observations, especially in the upper-troposphere. Here, we characterize and understand upper-troposphere dust sources and transport with an improved dust dataset derived from A-train satellite lidar and radar measurements and an air parcel trajectory model. The distinct upper-troposphere dust belt over the northern hemisphere has seasonally varying base and top heights of 3.65 ± 2.84 and 8.35 ± 1.50 km above mean sea level and its column loading is strongest during spring (March-April-May). The out-of-phase annual cycles of mid-level dust concentration and westerly wind over source regions control the seasonal upper-tropospheric dust loading variations. African deserts contribute the most (46.3%) to the upper-troposphere dust belt in spring and the synoptic trough is the leading (49%) dust lifting mechanism.
54 ENVIRONMENTAL SCIENCES↗
Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources
Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗