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At least 109 records · Page 6

Long-Term Simulation of Dust Distribution with the GOCART Model: Correlation with the North Atlantic Oscillation

Global distribution of aeolian dust is simulated from 1981 to 1996 with the Goddard Ozone Chemistry Aerosol Radiation and Transport (GOCART) model. The results are assessed with in-situ measurements and the Total Ozone Mapping Spectrometer (TOMS) aerosol products. The annual budget over the different continents and oceans are analyzed. It is found that there is a maximum of 25% difference of global annual emission from the minimum in 1996 to the maximum in 1988. There is a downward trend of dust emission over Africa and East Asia, of 6 and 2 Tg/yr, respectively. The inter-annual variability of dust distribution is analyzed over the North Atlantic and Africa. It is found that in winter most of the North Atlantic and Africa dust loading is correlated with the North Atlantic Oscillation. The GOCART model indicates that a controlling factor of such correlation can be attributed to dust emission from the Sahel. The Bodele depression is the major dust source in winter and its inter-annual variability is highly correlated with the NAO. However, it is not possible to conclude without further analysis that the North Atlantic Oscillation is forcing the inter-annual variability of dust emission and in-turn dust concentration over the North Atlantic.

Ginoux, P.↗

Interannual Comparison of Water Vapor in the North Polar Region of Mars

In order to better understand the current climate of Mars, we seek to understand atmospheric water in the north polar region. Our approach is to examine the water transport and cycling issues within the north polar region and in/out of the region on seasonal and annual timescales. Viking Mars Atmospheric Water Detector (MAWD) data showed that water vapor increased as the northern summer season progressed and temperatures increased, and that vapor appeared to be transported southward . However, there has been uncertainty about the amount of water cycling in and out of the north polar region, as evidenced by residual polar cap visible brightness changes between one Martian year (Mariner 9 data) and a subsequent year (Viking data). These changes were originally thought to be interannual variations in the amount of frost sublimed based on global dust storm activity . However, Viking thermal and imaging data were re-examined and it was found that 14-35 pr m of water -ice appeared to be deposited on the cap later in the summer season, indicating that some water may be retained and redistributed within the polar cap region. This late summer deposition could be due to adsorption directly onto the cap surface or due to snowfall. We seek to understand what happens to the water on seasonal and interannual timescales. We address these issues by examining water vapor in the north polar region of Mars during the north spring and summer period from MGS TES data and by comparing these results to the Viking MAWD results.

Tamppari, L. K.↗

The Response of the North Atlantic Bloom to NAO Forcing

Results from the climatologically forced coupled ice/ocean/biogeochemical model that covers the Arctic and North Atlantic Oceans are presented and compared to the chlorophyll fields of satellite-derived ocean color measurements. Biogeochemical processes in the model are determined from the interactions among four phytoplankton functional groups (diatoms, chlorophytes, cyanobacteria and coccolithophores) and four nutrients (nitrate, ammonium, silicate and dissolved iron). The model simulates the general large-scale pattern in April, May and June, when compared to both satellite-derived and in situ observations. The subpolar North Atlantic was cool in the 1980s and warm in the latter 1990s, corresponding to the CZCS and SeaWiFS satellite observing periods, respectively. The oceanographic conditions during these periods resemble the typical subpolar upper ocean response to the NAO+ and NAO-phases, respectively. Thus, we use the atmospheric forcing composites from the two NAO phases to simulate the variability of the mid-ocean bloom during the satellite observing periods. The model results show that when the subpolar North Atlantic is cool, the NAO+ case, more nutrients are available in early spring than when the North Atlantic is warm, the NAO-case. However, the NAO+ simulation produces a later bloom than the NAO-simulation. This difference in the bloom times is also identified in SeaWiFS and CZCS satellite measurements. In the model results, we can trace the difference to the early diatom bloom due to a warmer upper ocean. The higher nutrient abundance in the NAO+ case did not provide larger total production than in the NAO- case, instead the two cases had a comparable area averaged amplitude. This leads us to conclude that in the subpolar North Atlantic, the timing of the spring phytoplankton bloom depends on surface temperature and the magnitude of the bloom is not significantly impacted by the nutrient abundance.

Mizoguchi, Ken-Ichi↗

Mapping Isoprene Emissions over North America using Formaldehyde Column Observations from Space

I] We present a methodology for deriving emissions of volatile organic compounds (VOC) using space-based column observations of formaldehyde (HCHO) and apply it to data from the Global Ozone Monitoring Experiment (GOME) satellite instrument over North America during July 1996. The HCHO column is related to local VOC emissions, with a spatial smearing that increases with the VOC lifetime. lsoprene is the dominant HCHO precursor over North America in summer, and its lifetime (approx. = 1 hour) is sufficiently short that the smearing can be neglected. We use the Goddard Earth Observing System global 3-D model of tropospheric chemistry (GEOS-CHEM) to derive the relationship between isoprene emissions and HCHO columns over North America and use these relationships to convert the GOME HCHO columns to isoprene emissions. We also use the GEOS-CHEM model as an intermediary to validate the GOME HCHO column measurements by comparison with in situ observations. The GEOS-CHEM model including the Global Emissions Inventory Activity (GEIA) isoprene emission inventory provides a good simulation of both the GOME data (r(sup 2) = 0.69, n = 756, bias = +l1 %) and the in situ summertime HCHO measurements over North America (r(sup 2) = 0.47, n = 10, bias = -3%). The GOME observations show high values over regions of known high isoprene emissions and a day-to-day variability that is consistent with the temperature dependence of isoprene emission. Isoprene emissions inferred from the GOME data are 20% less than GEIA on average over North America and twice those from the U S . EPA Biogenic Emissions Inventory System (BEIS2) inventory. The GOME isoprene inventory when implemented in the GEOS-CHEM model provides a better simulation of the HCHO in situ measurements thaneitherGEIAorBEIS2 (r(sup 2) = 0.71,n= 10, bias = -10 %).

Palmer, Paul I.↗

North American Vegetation Dynamics Observed with Multi-Resolution Satellite Data

North American vegetation has been discovered to be a net carbon sink, with atypical behavior of drawing down more carbon from the atmosphere during the past century. It has been suggested that the Northern Hemisphere will respond favorably to climate warming by enhancing productivity and reducing the impact of fossil fuel emissions into the atmosphere. Many investigations are currently underway to understand and identify mechanisms of storage so they might be actively managed to offset carbon emissions which have detrimental consequences to the functioning of ecosystems and human well being. This paper used a time series of satellite data from multiple sensors at multiple resolutions over the past thlrty years to identify and understand mechanisms of change to vegetation productivity throughout North America. We found that humans had a marked impact to vegetation growth in half of the six selected study regions which cover greater than two million km2. We found climatic influences of increasing temperatures, and longer growing seasons with reduced snow cover in the northern regions of North America with forest fire recovery in the Northern coniferous forests of Canada. The Mid-latitudes had more direct land cover changes induced by humans coupled with climatic influences such as severe drought and altered production strategies of rain-fed agriculture in the upper Midwest, expansion of irrigated agriculture in the lower Midwest, and insect outbreaks followed by subsequent logging in the upper Northeast. Vegetation growth over long time periods (20+ years) in North America appears to be associated with long term climate change but most of the marked changes appear to be associated with climate variability on decadal and shorter time scales along with direct human land cover conversions. Our results document regional land cover land use change and climatic influences that have altered continental scale vegetation dynamics in North America.

Neigh, Christopher S. R.↗

Atmospheric Circulation Anomalies During Two Persistent North American Droughts: 1932-1939 and 1948-1957

We use an early twentieth century (1908-1958) atmospheric reanalysis, based on assimilation of surface and sea level pressure observations, to contrast atmospheric circulation during two periods of persistent drought in North America: 1932-1939 (the Dust Bowl) and 1948-1957. Primary forcing for both droughts is believed to come from anomalous sea surface temperatures (SSTs): a warm Atlantic and a cool eastern tropical Pacific. For boreal winter (October-March) in the 1950s, a stationary wave pattern originating from the tropical Pacific is present, with positive centers over the north Pacific and north Atlantic ocean basins and a negative center positioned over northwest North America and the tropical/subtropical Pacific. This wave train is largely absent for the 1930s drought; boreal winter height anomalies are organized much more zonally, with positive heights extending across northern North America. For boreal summer (April-September) during the 1930s, a strong upper level ridge is centered over the Great Plains; this feature is absent during the 1950s and appears to be linked to a weakening of the Great Plains low-level jet (GPLLJ). Subsidence anomalies are co-located over the centers of each drought: in the central Great Plains for the 1930s and in a band extending from the southwest to the southeastern United States for the 1950s. The location and intensity of this subsidence during the 1948-1957 drought is a typical response to a cold eastern tropical Pacific, but for 1932-1939 deviates in terms of the expected intensity, location, and spatial extent. Overall, circulation anomalies during the 1950s drought appear consistent with the expected response to the observed SST forcing. This is not the case for the 1930s, implying some other causal factor may be needed to explain the Dust Bowl drought anomalies. In addition to SST forcing, the 1930s were also characterized by massive alterations to the land surface, including regional-scale devegetation from crop failures and intensive wind erosion and dust storms. Incorporation of these land surface factors into a general circulation model greatly improves the simulation of precipitation and subsidence anomalies during this drought, relative to simulations with SST forcing alone. Even with additional forcing from the land surface, however, the model still has difficulty reproducing some of the other circulation anomalies, including weakening of the GPLLJ and strengthening of the upper level ridge during AMJJAS. This may be due to either weaknesses in the model or uncertainties in the boundary condition estimates. Still, analysis of the circulation anomalies supports the conclusion of an earlier paper (Cook et al. in Proc Natl Acad Sci 106:4997, 2009), demonstrating that land degradation factors are consistent with the anomalous nature of the Dust Bowl drought.

Cook, Benjamin↗

High Latitude Meridional Flow on the Sun May Explain North-South Polar Field Asymmetry

We measured the flows of magnetic elements on the Sun at very high latitudes by analyzing magnetic images from the Helioseismic and Magnetic Imager (HMI) on the NASA Solar Dynamics Observatory (SDO) Mission. Magnetic maps constructed using a fixed, and north ]south symmetric, meridional flow profile give weaker than observed polar fields in the North and stronger than observed polar fields in the South during the decline of Cycle 23 and rise of Cycle 24. Our measurements of the meridional flow at high latitudes indicate systematic north ]south differences. There was a strong flow in the North while the flow in the South was weaker. With these results, we have a possible solution to the polar field asymmetry. The weaker flow in the South should keep the polar fields from becoming too strong while the stronger flow in the North should strengthen the field there. In order to gain a better understanding of the Solar Cycle and magnetic flux transport on the Sun, we need further observations and analyses of the Sun fs polar regions in general and the polar meridional flow in particular

Kosak, Katie↗

High Latitude Meridional Flow on the Sun May Explain North-South Polar Field Asymmetry

We measured the flows of magnetic elements on the Sun at very high latitudes by analyzing magnetic images from the Helioseismic and Magnetic Imager (HMI) on the NASA Solar Dynamics Observatory (SDO) Mission. Magnetic maps constructed using a fixed, and north-south symmetric, meridional flow profile give weaker than observed polar fields in the North and stronger than observed polar fields in the South during the decline of Cycle 23 and rise of Cycle 24. Our measurements of the meridional flow at high latitudes indicate systematic north-south differences. There was a strong flow in the North while the flow in the South was weaker. With these results, we have a possible solution to the polar field asymmetry. The weaker flow in the South should keep the polar fields from becoming too strong while the stronger flow in the North should strengthen the field there. In order to gain a better understanding of the Solar Cycle and magnetic flux transport on the Sun, we need further observations and analyses of the Sun's polar regions in general and the polar meridonal flow in particular.

Kosak, Katie↗

Monitoring River Basin Development and Variation in Water Resources in Transboundary Imjin River in North and South Korea Using Remote Sensing

This paper presents methods of monitoring river basin development and water variability for the transboundary river in North and South Korea. River basin development, such as dams and water infrastructure in transboundary rivers, can be a potential factor of tensions between upstream and downstream countries since dams constructed upstream can adversely affect downstream riparians. However, because most of the information related to North Korea has been limited to the public, the information about dams constructed and their locations were inaccurate in many previous studies. In addition, water resources in transboundary rivers can be exploited as a political tool. Specifically, due to the unexpected water release from the Hwanggang Dam, upstream of the transboundary Imjin River in North and South Korea, six South Koreans died on 6 September 2009. The Imjin River can be used as a political tool by North Korea, and seven events were reported as water conflicts in the Imjin River from 2001 to 2016. In this paper, firstly, we have updated the information about the dams constructed over the Imjin River in North Korea using multi-temporal images with a high spatial resolution (15-30 cm) obtained from Google Earth. Secondly, we analyzed inter- and intra-water variability over the Hwanggang Reservoir using open-source images obtained from the Global Surface Water Explorer. We found a considerable change in water surface variability before and after 2008, which might result from the construction of the Hwanggang Dam. Thirdly, in order to further investigate intra-annual water variability, we present a method monitoring water storage changes of the Hwanggang Reservoir using the area-elevation curve (AEC), which was derived from multi-sensor Synthetic Aperture Radar (SAR) images (Sentinel-1A and -1B) and the Shuttle Radar Topography Mission (SRTM) Digital Elevation Model (DEM). Since many previous studies for estimating water storage change have depended on satellite altimetry dataset and optical images for deriving AEC, the method adopted in this study is the only application for such inaccessible areas since no altimetry ground track exists for the Hwanggang Reservoir and because clouds can block the study area for wet seasons. Moreover, this study has newly proven that unexpected water release can occur in dry seasons because the water storage in the Hwanggang Reservoir can be high enough to conduct a release that can be used as a geopolitical tool. Using our method, potential risks can be mitigated, not in response to a water release, but based on pre-event water storage changes in the Hwanggang Reservoir.

Kim, Donghwan↗

Roles of the atmosphere and ocean in the projected north atlantic warming hole

There exists a warming deficit in sea surface temperatures (SST) over the subpolar North Atlantic in response to quadrupled CO 2 , referred to as the projected North Atlantic warming hole (WH). This study employs a partial coupling technique to accurately verify the relative roles of oceanic and atmospheric processes in the formation of the projected WH within an atmosphere-ocean coupled framework. By decomposing the SST anomalies in the subpolar North Atlantic into two components: those induced by atmospheric processes (i.e., the atmosphere-forced component) and those driven by changes in ocean circulation (i.e., the ocean-driven component), we find that the projected WH is primarily driven by changes in ocean circulation, with almost no contribution from atmospheric processes. Specifically, the slowdown of the Atlantic Meridional Overturning Circulation (AMOC) results in a cooling of SST in the WH region due to reduced northward ocean heat transport into this region. This study further quantifies the influence of a positive coupled feedback through surface heat flux (SHF) on the AMOC response under greenhouse gas forcing within this self-consistent framework. It is found that the AMOC slowdown leads to a negative SST anomaly in the subpolar North Atlantic and subsequently a positive ocean-driven SHF anomaly, which in turn further weakens the AMOC. In conclusion, this positive feedback through the SHF contributes about 50% to the total AMOC slowdown in response to quadrupled CO 2 .

54 ENVIRONMENTAL SCIENCES↗

Permafrost, Peatland, and Cropland Regions Are Key to Reconciling North American Carbon Sink Estimates

Persistent discrepancies between bottom-up, terrestrial biosphere models (TBMs), and top-down, atmospheric inversions, have made it difficult to quantify the magnitude of the North American terrestrial carbon sink. Previous studies have compared aggregated continent-scale estimates of carbon fluxes from TBMs and inversions for all of North America, but this provides limited insights into finer-scale mismatches that contribute to the overall discrepancies. Here we evaluate agreement between TBM and inversion carbon flux estimates at 1° × 1° resolution to provide more direct insights into where models disagree and what underlying factors drive discrepancies. We find that the additional carbon uptake estimated by inversions, in just 16% of the area of North America, is large enough to account for the discrepancy between TBMs and inversions across the whole continent. The majority of these differences occur in permafrost, peatland, and cropland regions. In these regions, we find a higher likelihood of potential biases in the weaker sink estimates from TBMs, suggesting that the stronger sink implied by inversions is more likely to be realistic. However, the current observational coverage is insufficient for fully assessing the causes of discrepancies or the magnitude of biases in either approach. Encouragingly, improved representation of agricultural processes in a TBM led to better agreement with inversions in croplands. Efforts to accurately model cropland dynamics will help improve agreement between TBMs and inversions. Overall, this work presents a clear path for reconciling the discrepancies between inversion and TBM estimates of the North American carbon sink that have persisted for two decades.

54 ENVIRONMENTAL SCIENCES↗

DE-FE0029488 - North Dakota Integrated Carbon Capture and Storage Complex Feasibility Study Public Data

Data from award DE-FE0029488 - North Dakota Integrated Carbon Capture and Storage Complex Feasibility Study performed by the Energy & Environmental Research Center including the following: - 2D Seismic {Input data, sgy files, maps, logs, and descriptors} - Core Petrophysics {Core analysis of plugs from the two stratigraphic test wells (Flemmer-1 [API 33-057-00039] and BNI-1 [API 33-065-00018])} - North Dakota Oil and Gas File No 37380 Files - North Dakota Oil and Gas File No 37672 Files - Well Testing Data {Summary of well testing methods and results from the stratigraphic test wells (Flemmer-1 and BNI-1)} Additional References: https://www.netl.doe.gov/sites/default/files/2017-12/Wesley-Peck-_Mastering-the-Subsurface_CarbonSAFE-Phase-II_August-2017-final.pdf Peck, W.D., Ayash, S.C., Klapperich, R.J., Gorecki, C.D. (2019) The North Dakota integrated carbon storage complex feasibility study, International Journal of Greenhouse Gas Control, Volume 84, 2019, Pages 47-53, https://doi.org/10.1016/j.ijggc.2019.03.001

Carbon Storage↗

The Future Intensification of the North Atlantic Winter Storm Track: The Key Role of Dynamic Ocean Coupling

Climate models project an intensification of the wintertime North Atlantic storm track, over its downstream region, by the end of this century. Previous studies have suggested that ocean-atmosphere coupling plays a key role in this intensification, but the precise role of the different components of the coupling has not been explored and quantified. In this paper, using a hierarchy of ocean coupling experiments, we isolate and quantify the respective roles of thermodynamic (changes in surface heat fluxes) and dynamic (changes in ocean heat flux convergence) ocean coupling in the projected intensification of North Atlantic transient eddy kinetic energy (TEKE). We show that dynamic coupling accounts for nearly all of the future TEKE strengthening as it overcomes the much smaller effect of surface heat flux changes to weaken the TEKE. We further show that by reducing the Arctic amplification in the North Atlantic, ocean heat flux convergence increases the meridional temperature gradient aloft, causing a larger eddy growth rate, and resulting in the strengthening of North Atlantic TEKE. Our results stress the importance of better monitoring and investigating the changes in ocean heat transport, for improving climate change adaptation strategies.

North Atlantic winter storms↗

Spring Dust in Western North America and its Interannual Variability – Understanding the Role of Local and Transported Dust

Mineral dust over western North America is an important aerosol type contributing up to one half of surface aerosol concentrations in spring. In the present study, we use data from in-situ and remote-sensing observations and the NASA Unified WRF (NU-WRF) model to investigate the sources and interannual variations of the springtime fine-mode dust over western North America. The horizontal distribution, seasonality, and interannual variability of the springtime dust over the region are characterized with observations of fine dust concentrations at the Interagency Monitoring of Protected Visual Environments (IMPROVE) sites and dust optical depth (DOD) from the Aerosol Robotic Network (AERONET) measurements. We have conducted detailed modeling and analysis for April in selected years of 2005, 2008, and 2009, to understand the causes of interannual variabilities of the springtime dust with model experiments that separate the dust generated from local deserts with that transported across the Pacific Ocean. The results suggest that although several permanent deserts and semi-arid regions in the western North America are the major source of surface fine dust concentrations in the immediate vicinity, long-range transpacific transported dust is a dominant dust source in springtime, especially over the coastal regions and areas remote from the local deserts. Interannual variability of fine dust over western North America is explained with both local dust emission and long-range transported dust.

North America spring dust↗

Wide range of possible trajectories of North Atlantic climate in a warming world

Decadal variability in the North Atlantic Ocean impacts regional and global climate, yet changes in internal decadal variability under anthropogenic radiative forcing remain largely unexplored. Here we use the Community Earth System Model 2 Large Ensemble under historical and the Shared Socioeconomic Pathway 3-7.0 future radiative forcing scenarios and show that the ensemble spread in northern North Atlantic sea surface temperature (SST) more than doubles during the mid-twenty-first century, highlighting an exceptionally wide range of possible climate states. Furthermore, there are strikingly distinct trajectories in these SSTs, arising from differences in the North Atlantic deep convection among ensemble members starting by 2030. We propose that these are stochastically triggered and subsequently amplified by positive feedbacks involving coupled ocean-atmosphere-sea ice interactions. Freshwater forcing associated with global warming seems necessary for activating these feedbacks, accentuating the impact of external forcing on internal variability. Further investigation on seven additional large ensembles affirms the robustness of our findings. By monitoring these mechanisms in real time and extending dynamical model predictions after positive feedbacks activate, we may achieve skillful long-lead North Atlantic decadal predictions that are effective for multiple decades.

54 ENVIRONMENTAL SCIENCES↗

Influence of Background Divergent Moisture Flux on the Frequency of North Pacific Atmospheric Rivers

The frequency of North Pacific atmospheric rivers (ARs) affects water supply and flood risk over western North America. Thus, understanding factors that affect the variability of landfalling AR frequency is of scientific and societal importance. This study aims at identifying the sources of the moisture for North Pacific ARs and assessing how different modes of variability modulate these sources. To this end, the sources and variability of the background divergent component of the integrated moisture flux (DIVT) in ARs are identified using MERRA reanalysis. It is shown that in the boreal winter, this background DIVT in ARs is related to the outflow from the subsidence over the subtropics which transports moisture northward, while in summer it is related to the Asian monsoon and it transports moisture northwestward. This leads to a seasonal northwest/southeast movement of the AR frequency climatology. At the intra-seasonal scale, propagation of the Madden-Julian Oscillation introduces an anti-clockwise rotation of the background DIVT, with northward transport in phases 1 and 2, westward in 3 and 4, southward in 5 and 6 and eastward in 7 and 8, making landfall over the west coast of North America most likely during the last two phases. Similarly, El Niño Southern Oscillation variability also affects the frequency of ARs through modulation of the westerly background DIVT, favoring landfall over the US west coast during strong El Niño phases. It is shown that in general the likelihood of AR landfall over the western US is correlated with the zonal background DIVT over northeastern Pacific.

54 ENVIRONMENTAL SCIENCES↗

Predictability and empirical dynamics of fisheries time series in the North Pacific

Previous studies have documented a strong relationship between marine ecosystems and large-scale modes of sea surface height (SSH) and sea surface temperature (SST) variability in the North Pacific such as the Pacific Decadal Oscillation and the North Pacific Gyre Oscillation. In the central and western North Pacific along the Kuroshio-Oyashio Extension (KOE), the expression of these modes in SSH and SST is linked to the propagation of long oceanic Rossby waves, which extend the predictability of the climate system to ~3 years. Using a multivariate physical-biological linear inverse model (LIM) we explore the extent to which this physical predictability leads to multi-year prediction of dominant fishery indicators inferred from three datasets (i.e., estimated biomasses, landings, and catches). We find that despite the strong autocorrelation in the fish indicators, the LIM adds dynamical forecast skill beyond persistence up to 5-6 years. By performing a sensitivity analysis of the LIM forecast model, we find that two main factors are essential for extending the dynamical predictability of the fishery indicators beyond persistence. The first is the interaction of the fishery indicators with the SST/SSH of the North and tropical Pacific. The second is the empirical relationship among the fisheries time series. This latter component reflects stock-stock interactions as well as common technological and human socioeconomic factors that may influence multiple fisheries and are captured in the training of the LIM. These results suggest that empirical dynamical models and machine learning algorithms, such as the LIM, provide an alternative and promising approach for forecasting key ecological indicators beyond the skill of persistence.

60 APPLIED LIFE SCIENCES↗

Fine Aerosol Acidity and Water during Summer in the Eastern North Atlantic

Aerosol pH governs many important atmospheric processes that occur in the marine boundary layer, including regulating halogen and sulfur chemistries, and nutrient fertilization of surface ocean waters. In this study, we investigated the acidity of PM1 over the eastern North Atlantic during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) aircraft campaign. The ISORROPIA-II thermodynamic model was used to predict PM1 pH and water. We first investigated the sensitivities of PM1 pH and water predictions to gas-phase NH3 and HNO3 concentrations. Our sensitivity analysis indicated that even though NH3 and HNO3 were present at very low concentrations in the eastern North Atlantic during the campaign, PM1 pH calculations can still be sensitive to NH3 concentrations. Specifically, NH3 was needed to constrain the pH of populations of PM1 that had low mass concentrations of NH4+ and non-volatile cations (NVCs). We next assumed that gas-phase NH3 and HNO3 concentrations during the campaign were 0.15 and 0.09 µg m−3, respectively, based on previous measurements conducted in the eastern North Atlantic. Using the assumption that PM1 were internally mixed (i.e., bulk PM1), we determined that PM1 pH ranged from 0.3–8.6, with a mean pH of 5.0 ± 2.3. The pH depended on both Hair+ and Wi. Hair+ was controlled primarily by the NVCs/SO42− molar ratio, while Wi was controlled by the SO42− mass concentration and RH. Changes in pH with altitude were driven primarily by changes in SO42−. Since aerosols in marine atmospheres are rarely internally mixed, the scenario where non-sea salt species and sea-salt species were present in two separate aerosol modes in the PM1 (i.e., completely externally mixed) was also considered. Smaller pH values were predicted for the aerosol mode comprised only of non-sea salt species compared to the bulk PM1 (difference of around 1 unit on average). This was due to the exclusion of sea-salt species (especially hygroscopic alkaline NVCs) in this aerosol mode, which led to increases in Hair+ values and decreases in Wi values. This result demonstrated that assumptions of aerosol mixing states can impact aerosol pH predictions substantially, which will have important implications for evaluating the nature and magnitude of pH-dependent atmospheric processes that occur in the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗