ALBERT

Description: We use observations from the April 2008 NASA ARCTAS aircraft campaign to the North American Arctic, interpreted with a global 3-D chemical transport model (GEOS-Chem), to better understand the sources and cycling of hydrogen oxide radicals (HOx≡H+OH+peroxy radicals) and their reservoirs (HOy≡HOx+peroxides) in the springtime Arctic atmosphere. We find that a standard gas-phase chemical mechanism overestimates the observed HO2 and H2O2 concentrations. Computation of HOx and HOy gas-phase chemical budgets on the basis of the aircraft observations also indicates a large missing sink for both. We hypothesize that this could reflect HO2 uptake by aerosols, favored by low temperatures and relatively high aerosol loadings, through a mechanism that does not produce H2O2. We implemented such an uptake of HO2 by aerosol in the model using a standard reactive uptake coefficient parameterization with γ(HO2) values ranging from 0.02 at 275 K to 0.5 at 220 K. This successfully reproduces the concentrations and vertical distributions of the different HOx species and HOy reservoirs. HO2 uptake by aerosol is then a major HOx and HOy sink, decreasing mean OH and HO2 concentrations in the Arctic troposphere by 32% and 31% respectively. Better rate and product data for HO2 uptake by aerosol are needed to understand this role of aerosols in limiting the oxidizing power of the Arctic atmosphere.

Description: Vertical profiles of aerosol extinction obtained with the CALIOP lidar onboard CALIPSO are used in conjunction with the GEOS-Chem chemical transport model and NOAA's HYSPLIT trajectory model to document three aerosol export events from East Asia to the Arctic in the year 2007. During each of these events CALIOP sampled the pollution plumes multiple times over periods of five to seven days. Midlatitude cyclones lifted the pollution to the free troposphere with net diabatic heating of ~5 °C day−1 and precipitation in this initial ascending stage. Rapid meridional transport to the Arctic took place at 3–7 km altitude, and was mediated by either a blocking high pressure system in the NW Pacific or a trough-ridge configuration. Once in the Arctic transport was nearly isentropic with slow subsidence and radiative cooling at a rate of 1–1.5 °C day−1. We find good agreement between modeled and observed plumes in terms of length, altitude, thickness and, within the measurement uncertainties, extinction coefficient. In one event the satellite algorithm misclassifies the aerosol layer as ice clouds as a result of the relatively high depolarization ratio (0.06), likely caused by a high dust component in the aerosol mixture. Using 500 hPa geopotential height anomalies for these three events along with eight other export events observed by CALIOP in 2007–2009, we develop a meteorological index that captures 40–60% of the variance of Asian transport events to the Arctic in winter and spring. Simulations with the GEOS-Chem model show that 6 major export events from Asia to the Arctic occur each year, on average. The maximum probability for such events is during March–June, with a secondary maximum in October–November. During these events, Asian pollution and dust aerosols account for 50–70% of the aerosol optical depth over the Siberian sector of the Arctic, compared to a mean background contribution of 33%.

Description: We have developed a new nested-grid mercury (Hg) simulation over North America with a 1/2° latitude by 2/3° longitude horizontal resolution employing the GEOS-Chem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4° latitude by 5° longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in 2008–2009. The nested simulation resolves features such as higher deposition due to orographic precipitation, land/ocean contrast and and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27%. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid in-plume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to −2.3% over the ORV region. Over the contiguous US, the correlation coefficient (r) between MDN observations and our IPR simulation increases from 0.60 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean gaseous and particulate-bound Hg(II) are within 140% and 11% of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 4 and 2 for gaseous and particulate-bound Hg(II), respectively. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. The nested model suggests that North American anthropogenic emissions account for 10–22% of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The modeled percent contribution can be as high as 60% near large point sources in ORV. Our results indicate that the North American anthropogenic contribution to dry deposition is 13–20%.

Description: We use retrievals of aerosol extinction from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard the CALIPSO satellite to examine the vertical, horizontal and temporal variability of tropospheric Arctic aerosols during the period 2006–2012. We develop an empirical method that takes into account the difference in sensitivity between daytime and nighttime retrievals over the Arctic. Comparisons of the retrieved aerosol extinction to in situ measurements at Barrow (Alaska) and Alert (Canada) show that CALIOP reproduces the observed seasonal cycle and magnitude of surface aerosols to within 25 %. In the free troposphere, we find that daytime CALIOP retrievals will only detect the strongest aerosol haze events, as demonstrated by a comparison to aircraft measurements obtained during NASA's ARCTAS mission during April 2008. This leads to a systematic underestimate of the column aerosol optical depth by a factor of 2–10. However, when the CALIOP sensitivity threshold is applied to aircraft observations, we find that CALIOP reproduces in situ observations to within 20% and captures the vertical profile of extinction over the Alaskan Arctic. Comparisons with the ground-based high spectral resolution lidar (HSRL) at Eureka, Canada, show that CALIOP and HSRL capture the evolution of the aerosol backscatter vertical distribution from winter to spring, but a quantitative comparison is inconclusive as the retrieved HSRL backscatter appears to overestimate in situ observations by a factor of 2 at all altitudes. In the High Arctic (〉70° N) near the surface (

Description: We use satellite observations of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectrometer (MODIS) together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30%) is found in the model fine mode AOD, particularly during summer. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-year study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward to the Arctic in 3–4 days, with the other crossing the Pacific Ocean in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High during spring and summer. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. This dipole structure during outflow events is a strong feature for all seasons except summer, when convection becomes more important. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a broad spring/summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow is mostly found in the lower troposphere (1–3 km altitude), the Asian sulfate outflow occurs at higher altitudes (2–6 km). In the Asian outflow 42–59% of the sulfate column is present above 2 km altitude, with only 24–35% in the N. American outflow. We link this to the factor of 2–5 lower precipitation in the warm conveyor belts (WCB) of midlatitude cyclones over E. Asia compared to N. America. This relative lack of precipitation makes Asian WCB very efficient for injecting aerosols in the middle troposphere.

Description: We combine in situ measurements of sea salt aerosols (SS) from open ocean cruises and ground-based stations together with aerosol optical depth (AOD) observations from MODIS and AERONET, and the GEOS-Chem global chemical transport model to provide new constraints on SS emissions over the world's oceans. We find that the GEOS-Chem model using the Gong (2003) source function overestimates cruise observations of coarse mode SS mass concentrations by factors of 2–3 at high wind speeds over the cold waters of the Southern, North Pacific and North Atlantic Oceans. Furthermore, the model systematically underestimates SS over the warm tropical waters of the Central Pacific, Atlantic, and Indian Oceans. This pattern is confirmed by SS measurements from a global network of 15 island and coastal stations. The model discrepancy at high wind speeds (〉6 m s −1) has a clear dependence on sea surface temperature (SST). We use the cruise observations to derive an empirical SS source function depending on both wind speed and SST. Implementing this new source function in GEOS-Chem results in improved agreement with in situ observations, with a decrease in the model bias from +64% to +33% for the cruises and from +32% to −5% for the ground-based sites. We also show that the wind speed-SST source function significantly improves agreement with MODIS and AERONET AOD, and provides an explanation for the high AOD observed over the tropical oceans. With the wind speed-SST formulation, global SS emissions show a small decrease from 5200 Mg yr−1 to 4600 Mg yr−1, while the SS burden decreases from 9.1 to 8.5 mg m−2. The spatial distribution of SS, however, is greatly affected, with the SS burden increasing by 50% in the tropics and decreasing by 40% at mid- and high-latitudes. Our results imply a stronger than expected halogen source from SS in the tropical marine boundary layer. They also imply stronger radiative forcing of SS in the tropics and a larger response of SS emissions to climate change than previously thought.

Description: We use satellite observations of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectrometer (MODIS) together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30%) is found in the model fine mode AOD. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-yr study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward towards the Arctic, with the other crossing the Pacific in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a weak summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow is mostly found in the lower troposphere (1–3 km altitude), the Asian sulfate outflow occurs at higher altitudes (2–6 km). In the Asian outflow 42–59% of the sulfate column is present above 2 km altitude, with only 24–35% in the N. American outflow. We link this to the factor of 2–5 lower precipitation in the warm conveyor belts (WCB) of midlatitude cyclones over E. Asia compared to N. America. This relative lack of precipitation makes Asian WCB very efficient for injecting aerosols in the middle troposphere.

Description: We have developed a new high-resolution (1/2° latitude by 2/3° longitude) nested-grid mercury (Hg) simulation over North America employing the GEOS-Chem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4° latitude by 5° longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in 2008–2009. The nested simulation resolves features such as land/ocean contrast and higher deposition due to orographic precipitation, and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27%. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid in-plume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to +3% over the ORV region. Over the contiguous US, the correlation coefficient (r) between MDN observations and our IPR simulation increases from 0.63 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean reactive gaseous and particulate-bound Hg are within 80% and 10% of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 2 to 4. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. We find that North American anthropogenic emissions account for 10–22% of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The percent contribution can be as high as 60% near large point emission sources in ORV. The contribution for the dry deposition is 13–20%.

Description: We use retrievals of aerosol extinction from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the CALIPSO satellite to examine the vertical, horizontal and temporal variability of tropospheric Arctic aerosols during 2006–2012. We develop an empirical method that takes into account the difference in sensitivity between daytime and nighttime retrievals over the Arctic. Comparisons of the retrieved aerosol extinction to in situ measurements at Barrow (Alaska) and Alert (Canada) show that CALIOP reproduces the observed seasonal cycle and magnitude of surface aerosols to within 25%. In the free troposphere, we find that daytime CALIOP retrievals will only detect the strongest aerosol haze events as demonstrated by a comparison to aircraft measurements obtained during NASA's ARCTAS mission during April 2008. This leads to a systematic underestimate of the column aerosol optical depth by a factor of 2–10. However, when the CALIOP sensitivity threshold is applied to aircraft observations, we find that CALIOP reproduces in situ observations to within 20% and captures the vertical profile of extinction over the Alaskan Arctic. Comparisons with the ground-based HSRL Lidar at Eureka, Canada, show that CALIOP and HSRL capture the evolution of the aerosol backscatter vertical distribution from winter to spring, but a quantitative comparison is inconclusive as the retrieved HSRL backscatter appears to overestimate in situ observations factor of 2 at all altitudes. In the High Arctic (〉 70° N) near the surface (〈 2 km), CALIOP aerosol extinctions reach a maximum in December-March (10–20 Mm−1), followed by a sharp decline and a minimum in May–September (1–4 Mm−1), thus providing the first Pan-Arctic view of Arctic Haze seasonality. The European and Asian Arctic sectors display the highest wintertime extinctions, while the Atlantic sector is the cleanest. Over the Low Arctic (60–70° N) near the surface, CALIOP extinctions reach a maximum over land in summer due to boreal forest fires. During summer, we find that smoke aerosols reach higher altitudes (up to 4 km) over Eastern Siberia and North America than over Northern Eurasia, where it remains mostly confined below 2 km. In the free troposphere, the extinction maximum over the Arctic occurs in March–April at 2–5 km altitude and April–May at 5–8 km. This is consistent with transport from the mid-latitudes associated with the annual maximum in cyclonic activity and blocking patterns in the Northern Hemisphere. A strong gradient in aerosol extinction is observed between 60° N and 70° N in the summer. This is likely due to efficient stratocumulus wet scavenging at high latitudes combined with the poleward retreat of the polar front. Interannual variability in the middle and upper troposphere is associated with biomass burning events (high extinctions observed by CALIOP in spring 2008 and summer 2010) and volcanic eruptions (Kasatochi in August 2008 and Sarychev in June 2009). CALIOP displays below-average extinctions observed from August 2009 through May 2010, which appear to be linked with a strongly negative Arctic Oscillation index.