scholarly journals High gas-phase mixing ratios of formic and acetic acid in the High Arctic

2018 ◽  
Vol 18 (14) ◽  
pp. 10237-10254 ◽  
Author(s):  
Emma L. Mungall ◽  
Jonathan P. D. Abbatt ◽  
Jeremy J. B. Wentzell ◽  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
...  
Keyword(s):  
Acetic Acid ◽  
Gas Phase ◽  
Transport Model ◽  
High Arctic ◽  
Early Summer ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Phase Measurements ◽  
Diurnal Cycles ◽  
Mixing Ratios

Abstract. Formic and acetic acid are ubiquitous and abundant in the Earth's atmosphere and are important contributors to cloud water acidity, especially in remote regions. Their global sources are not well understood, as evidenced by the inability of models to reproduce the magnitude of measured mixing ratios, particularly at high northern latitudes. The scarcity of measurements at those latitudes is also a hindrance to understanding these acids and their sources. Here, we present ground-based gas-phase measurements of formic acid (FA) and acetic acid (AA) in the Canadian Arctic collected at 0.5 Hz with a high-resolution chemical ionization time-of-flight mass spectrometer using the iodide reagent ion (iodide HR-ToF-CIMS, Aerodyne). This study was conducted at Alert, Nunavut, in the early summer of 2016. FA and AA mixing ratios for this period show high temporal variability and occasional excursions to very high values (up to 11 and 40 ppbv respectively). High levels of FA and AA were observed under two very different conditions: under overcast, cold conditions during which physical equilibrium partitioning should not favor their emission, and during warm and sunny periods. During the latter, sunny periods, the FA and AA mixing ratios also displayed diurnal cycles in keeping with a photochemical source near the ground. These observations highlight the complexity of the sources of FA and AA, and suggest that current chemical transport model implementations of the sources of FA and AA in the Arctic may be incomplete.

scholarly journals High gas-phase mixing ratios of formic and acetic acid in the High Arctic

2018 ◽  
Author(s):  
Emma L. Mungall ◽  
Jonathan P. D. Abbatt ◽  
Jeremy J. B. Wentzell ◽  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
...  
Keyword(s):  
Acetic Acid ◽  
Gas Phase ◽  
Transport Model ◽  
High Arctic ◽  
Early Summer ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Phase Measurements ◽  
Diurnal Cycles ◽  
Mixing Ratios

Abstract. Formic and acetic acid are ubiquitous and abundant in the Earth's atmosphere and are important contributors to cloud water acidity, especially in remote regions. Their global sources are not well understood, as evidenced by the inability of models to reproduce the magnitude of measured mixing ratios, particularly at high northern latitudes. The scarcity of measurements at those latitudes is also a hindrance to understanding these acids and their sources. Here, we present ground-based gas-phase measurements of formic acid (FA) and acetic acid (AA) in the Canadian Arctic collected at 0.5 Hz with a high resolution chemical ionization time-of-flight mass spectrometer using the iodide reagent ion (Iodide HR-ToF-CIMS, Aerodyne). This study was conducted at Alert, Nunavut, in the early summer of 2016. FA and AA mixing ratios for this period show high temporal variability and occasional excursions to very high values (up to 11 and 40 ppbv respectively). High levels of FA and AA were observed under two very different conditions: under overcast, cold conditions during which physical equilibrium partitioning should not favour their emission, and during warm and sunny periods. During the latter, sunny periods, the FA and AA mixing ratios also displayed diurnal cycles in keeping with a photochemical source near the ground. These observations highlight the complexity of the sources of FA and AA, and suggest that current chemical transport model implementations of the sources of FA and AA in the Arctic may be incomplete.

scholarly journals Boundary layer and free-tropospheric dimethyl sulfide in the Arctic spring and summer

2017 ◽  
Vol 17 (14) ◽  
pp. 8757-8770 ◽  
Author(s):  
Roghayeh Ghahremaninezhad ◽  
Ann-Lise Norman ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  
Keyword(s):  
Dimethyl Sulfide ◽  
Transport Model ◽  
Dispersion Model ◽  
Open Water ◽  
Particle Dispersion ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Model Simulations ◽  
Baffin Bay ◽  
Mixing Ratios

Abstract. Vertical distributions of atmospheric dimethyl sulfide (DMS(g)) were sampled aboard the research aircraft Polar 6 near Lancaster Sound, Nunavut, Canada, in July 2014 and on pan-Arctic flights in April 2015 that started from Longyearbyen, Spitzbergen, and passed through Alert and Eureka, Nunavut, and Inuvik, Northwest Territories. Larger mean DMS(g) mixing ratios were present during April 2015 (campaign mean of 116  ±  8 pptv) compared to July 2014 (campaign mean of 20  ±  6 pptv). During July 2014, the largest mixing ratios were found near the surface over the ice edge and open water. DMS(g) mixing ratios decreased with altitude up to about 3 km. During April 2015, profiles of DMS(g) were more uniform with height and some profiles showed an increase with altitude. DMS reached as high as 100 pptv near 2500 m. Relative to the observation averages, GEOS-Chem (www.geos-chem.org) chemical transport model simulations were higher during July and lower during April. Based on the simulations, more than 90 % of the July DMS(g) below 2 km and more than 90 % of the April DMS(g) originated from Arctic seawater (north of 66° N). During April, 60 % of the DMS(g), between 500 and 3000 m originated from Arctic seawater. During July 2014, FLEXPART (FLEXible PARTicle dispersion model) simulations locate the sampled air mass over Baffin Bay and the Canadian Arctic Archipelago 4 days back from the observations. During April 2015, the locations of the air masses 4 days back from sampling were varied: Baffin Bay/Canadian Archipelago, the Arctic Ocean, Greenland and the Pacific Ocean. Our results highlight the role of open water below the flight as the source of DMS(g) during July 2014 and the influence of long-range transport (LRT) of DMS(g) from further afield in the Arctic above 2500 m during April 2015.

scholarly journals Surface ozone and its precursors at Summit, Greenland: comparison between observations and model simulations

2017 ◽  
Vol 17 (23) ◽  
pp. 14661-14674 ◽  
Author(s):  
Yaoxian Huang ◽  
Shiliang Wu ◽  
Louisa J. Kramer ◽  
Detlev Helmig ◽  
Richard E. Honrath
Keyword(s):  
Transport Model ◽  
Surface Ozone ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Atmospheric Models ◽  
Contributing Factors ◽  
Model Simulations ◽  
Mixing Ratios ◽  
The Us ◽  
Coarse Model

Abstract. Recent studies have shown significant challenges for atmospheric models to simulate tropospheric ozone (O3) and its precursors in the Arctic. In this study, ground-based data were combined with a global 3-D chemical transport model (GEOS-Chem) to examine the abundance and seasonal variations of O3 and its precursors at Summit, Greenland (72.34° N, 38.29° W; 3212 m a.s.l.). Model simulations for atmospheric nitrogen oxides (NOx), peroxyacetyl nitrate (PAN), ethane (C2H6), propane (C3H8), carbon monoxide (CO), and O3 for the period July 2008–June 2010 were compared with observations. The model performed well in simulating certain species (such as CO and C3H8), but some significant discrepancies were identified for other species and further investigated. The model generally underestimated NOx and PAN (by  ∼  50 and 30 %, respectively) for March–June. Likely contributing factors to the low bias include missing NOx and PAN emissions from snowpack chemistry in the model. At the same time, the model overestimated NOx mixing ratios by more than a factor of 2 in wintertime, with episodic NOx mixing ratios up to 15 times higher than the typical NOx levels at Summit. Further investigation showed that these simulated episodic NOx spikes were always associated with transport events from Europe, but the exact cause remained unclear. The model systematically overestimated C2H6 mixing ratios by approximately 20 % relative to observations. This discrepancy can be resolved by decreasing anthropogenic C2H6 emissions over Asia and the US by  ∼ 20 %, from 5.4 to 4.4 Tg year−1. GEOS-Chem was able to reproduce the seasonal variability of O3 and its spring maximum. However, compared with observations, it underestimated surface O3 by approximately 13 % (6.5 ppbv) from April to July. This low bias appeared to be driven by several factors including missing snowpack emissions of NOx and nitrous acid in the model, the weak simulated stratosphere-to-troposphere exchange flux of O3 over the summit, and the coarse model resolution.

scholarly journals Supplementary material to "High gas-phase mixing ratios of formic and acetic acid in the High Arctic"

2018 ◽  
Author(s):  
Emma L. Mungall ◽  
Jonathan P. D. Abbatt ◽  
Jeremy J. B. Wentzell ◽  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
...  
Keyword(s):  
Acetic Acid ◽  
Gas Phase ◽  
High Arctic ◽  
Phase Mixing ◽  
Mixing Ratios ◽  
Supplementary Material

scholarly journals Vertical profile of atmospheric dimethyl sulfide in the Arctic Spring and Summer

2017 ◽  
Author(s):  
Roghayeh Ghahremaninezhad ◽  
Ann-Lise Norman ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  
Keyword(s):  
Dimethyl Sulfide ◽  
Transport Model ◽  
Open Water ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Air Mass ◽  
Baffin Bay ◽  
Mixing Ratios ◽  
Vertical Distributions ◽  
Research Aircraft

Abstract. Vertical distributions of atmospheric dimethyl sulfide (DMS(g)) were sampled aboard the research aircraft Polar 6 near Lancaster Sound, Nunavut, Canada in July 2014 and on pan-Arctic flights in April 2015 that started from Longyearbyen, Spitzbergen, and passed through Alert and Eureka, Nunavut and Inuvik, Northwest Territories. Larger mean DMS(g) mixing ratios were present during April 2015 (campaign-mean of 116±8 pptv) compared to July 2014 (campaign-mean of 20±6 pptv). Observations in July 2014 indicated a decrease in DMS(g) mixing ratios with altitude up to about 3 km, and the largest mixing ratios were found near the surface above ice-edge and open water, coincident with increased particle concentrations. In contrast, DMS(g) mixing ratios sampled in April 2015 were as high as 100 pptv near 2500 m. The April campaign also exhibited uniform campaign-mean vertical profiles overall although some profiles showed an increase with altitude. GEOS-Chem chemical-transport model simulations indicate that Arctic seawater (north of 66° N) contributes the majority of DMS(g) to the Arctic profiles (>90 %) in July 2014 flight tracks which were below 3000 m. More than 90 % of DMS(g) in April 2015 was from Arctic seawater for measurements below 500 m, but that declined to 60 % for altitudes between 500 m and 3000 m. FLEXPART simulations indicate that for summer 2014, the sampled air mass originated over Baffin Bay and the Canadian Arctic Archipelago. Whereas, for springtime 2015, the air mass sampled on flights near Alert and Eureka originated from Baffin Bay/Canadian Archipelago and from long-range transport (LRT) around the northern tip of Greenland. Our results highlight the role of open water below the flight as the source of DMS(g) during July 2014, and the influence of LRT of DMS(g) from further afield in the Arctic above 2500 m during April 2015.

scholarly journals Tropospheric ozone and its precursors at Summit, Greenland: comparison between observations and model simulations

2017 ◽  
Author(s):  
Yaoxian Huang ◽  
Shiliang Wu ◽  
Louisa J. Kramer ◽  
Detlev Helmig ◽  
Richard E. Honrath
Keyword(s):  
Tropospheric Ozone ◽  
Transport Model ◽  
Deposition Velocity ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Contributing Factors ◽  
Model Simulations ◽  
Mixing Ratios ◽  
Resolution Model ◽  
Coarse Model

Abstract. Recent studies have shown some significant challenges for atmospheric models to simulate tropospheric ozone (O3) and some of its precursors in the Arctic. In this study, ground based data are combined with a global 3-D chemical transport model (GEOS-Chem) to examine the abundance and seasonal variations of O3 and its precursors at Summit, Greenland (72.34˚ N, 38.29˚ W, 3212 m a.s.l). Model simulations for atmospheric nitrogen oxides (NOx), peroxyacetyl nitrate (PAN), ethane (C2H6), propane (C3H8), carbon monoxide (CO), and O3 for the period of 07/2008–06/2010 are compared with observations. The model performs well in simulating certain species (such as CO and C3H8), but some significant discrepancies are identified for other species and further investigated. The model generally underestimates NOx and PAN (by around 50 % and 30 %, respectively) for March–June. Likely contributing factors to the low bias include missing NOx and PAN emissions from snowpack chemistry in the model. At the same time, the model overestimates NOx mixing ratios by more than a factor of 2 in wintertime, with episodic NOx mixing ratios up to 15 times higher than the typical NOx levels at Summit. Further investigation shows that these simulated episodic NOx spikes are always associated with transport events from Europe, but the exact cause remains unclear. The model systematically overestimates C2H6 mixing ratios by approximately 20 % relative to observations. This discrepancy can be resolved by decreasing anthropogenic C2H6 emissions over Asia and the US by 20 %, from 5.4 to 4.4 Tg/yr. GEOS-Chem is able to reproduce the seasonal variability of O3 and its spring maximum. However, compared with observations, it underestimates surface O3 by approximately 13 % (6.5 ppbv) from April to July. This low bias appears to be driven by several factors including missing snowpack emissions for NOx and nitrous acid, the coarse model resolution, model overestimated O3 dry deposition velocity during springtime, as well as the uncertainties in the stratosphere-to-troposphere exchange scheme for O3.

scholarly journals Tropospheric bromine chemistry: implications for present and pre-industrial ozone and mercury

2012 ◽  
Vol 12 (15) ◽  
pp. 6723-6740 ◽  
Author(s):  
J. P. Parrella ◽  
D. J. Jacob ◽  
Q. Liang ◽  
Y. Zhang ◽  
L. J. Mickley ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Elemental Mercury ◽  
Tropospheric Chemistry ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Mixing Ratios ◽  
The North

Abstract. We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1–8 nmol mol−1 (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4%. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

scholarly journals Chemistry of hydrogen oxide radicals (HO<sub>x</sub>) in the Arctic troposphere in spring

2010 ◽  
Vol 10 (13) ◽  
pp. 5823-5838 ◽  
Author(s):  
J. Mao ◽  
D. J. Jacob ◽  
M. J. Evans ◽  
J. R. Olson ◽  
X. Ren ◽  
...  
Keyword(s):  
Gas Phase ◽  
Transport Model ◽  
Chemical Mechanism ◽  
The Arctic ◽  
Peroxy Radicals ◽  
Chemical Transport Model ◽  
The North ◽  
Arctic Atmosphere ◽  
Hydrogen Oxide ◽  
Phase Chemical

Abstract. 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.

scholarly journals Characterization of Transport Regimes and the Polar Dome during Arctic Spring and Summer using in-situ Aircraft Measurements

2019 ◽  
Author(s):  
Heiko Bozem ◽  
Peter Hoor ◽  
Daniel Kunkel ◽  
Franziska Köllner ◽  
Johannes Schneider ◽  
...  
Keyword(s):  
Lower Troposphere ◽  
High Arctic ◽  
The Arctic ◽  
Trace Gas ◽  
Second Phase ◽  
Aerosol Formation ◽  
Transport Barrier ◽  
Data Set ◽  
Air Masses ◽  
Mixing Ratios

Abstract. The springtime composition of the Arctic lower troposphere is to a large extent controlled by transport of mid-latitude air masses into the Arctic, whereas during the summer precipitation and natural sources play the most important role. Within the Arctic region, there exists a transport barrier, known as the polar dome, which results from sloping isentropes. The polar dome, which varies in space and time, exhibits a strong influence on the transport of air masses from mid-latitudes, enhancing it during winter and inhibiting it during summer. Furthermore, a definition for the location of the polar dome boundary itself is quite sparse in the literature. We analyzed aircraft based trace gas measurements in the Arctic during two NETCARE airborne field camapigns (July 2014 and April 2015) with the Polar 6 aircraft of Alfred Wegener Institute Helmholtz Center for Polar and Marine Research (AWI), Bremerhaven, Germany, covering an area from Spitsbergen to Alaska (134° W to 17° W and 68° N to 83° N). For the spring (April 2015) and summer (July 2014) season we analyzed transport regimes of mid-latitude air masses travelling to the high Arctic based on CO and CO2 measurements as well as kinematic 10-day back trajectories. The dynamical isolation of the high Arctic lower troposphere caused by the transport barrier leads to gradients of chemical tracers reflecting different local chemical life times and sources and sinks. Particularly gradients of CO and CO2 allowed for a trace gas based definition of the polar dome boundary for the two measurement periods with pronounced seasonal differences. For both campaigns a transition zone rather than a sharp boundary was derived. For July 2014 the polar dome boundary was determined to be 73.5° N latitude and 299–303.5 K potential temperature, respectively. During April 2015 the polar dome boundary was on average located at 66–68.5° N and 283.5–287.5 K. Tracer-tracer scatter plots and probability density functions confirm different air mass properties inside and outside of the polar dome for the July 2014 and April 2015 data set. Using the tracer derived polar dome boundaries the analysis of aerosol data indicates secondary aerosol formation events in the clean summertime polar dome. Synoptic-scale weather systems frequently disturb this transport barrier and foster exchange between air masses from midlatitudes and polar regions. During the second phase of the NETCARE 2014 measurements a pronounced low pressure system south of Resolute Bay brought inflow from southern latitudes that pushed the polar dome northward and significantly affected trace gas mixing ratios in the measurement region. Mean CO mixing ratios increased from 77.9 ± 2.5 ppbv to 84.9 ± 4.7 ppbv from the first period to the second period. At the same time CO2 mixing ratios significantly dropped from 398.16 ± 1.01 ppmv to 393.81 ± 2.25 ppmv. We further analysed processes controlling the recent transport history of air masses within and outside the polar dome. Air masses within the spring time polar dome mainly experienced diabatic cooling while travelling over cold surfaces. In contrast air masses in the summertime polar dome were diabatically heated due to insolation. During both seasons air masses outside the polar dome slowly descended into the Arctic lower troposphere from above caused by radiative cooling. The ascent to the middle and upper troposphere mainly took place outside the Arctic, followed by a northward motion. Our results demonstrate the successful application of a tracer based diagnostic to determine the location of the polar dome boundary.

Record springtime stratospheric ozone depletion at 80°N in 2020

2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
Ozone Depletion ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Polar Vortex ◽  
The Arctic ◽  
Optical Absorption Spectroscopy ◽  
Chemical Transport Model ◽  
Polar Stratospheric Clouds ◽  
Ozone Loss ◽  
Stratospheric Clouds

&lt;p&gt;The Arctic winter of 2019-2020 was characterized by an unusually persistent polar vortex and temperatures in the lower stratosphere that were consistently below the threshold for the formation of polar stratospheric clouds (PSCs). These conditions led to ozone loss that is comparable to the Antarctic ozone hole. Ground-based measurements from a suite of instruments at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Canada (80.05&amp;#176;N, 86.42&amp;#176;W) were used to investigate chemical ozone depletion. The vortex was located above Eureka longer than in any previous year in the 20-year dataset and lidar measurements provided evidence of polar stratospheric clouds (PSCs) above Eureka. Additionally, UV-visible zenith-sky Differential Optical Absorption Spectroscopy (DOAS) measurements showed record ozone loss in the 20-year dataset, evidence of denitrification along with the slowest increase of NO&lt;sub&gt;2&lt;/sub&gt; during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO&lt;sub&gt;2&lt;/sub&gt; (chlorine reservoir species) from a Fourier transform infrared (FTIR) spectrometer showed unusually low columns that were comparable to 2011, the previous year with significant chemical ozone depletion. Record low values of HNO&lt;sub&gt;3&lt;/sub&gt; in the FTIR dataset are in accordance with the evidence of PSCs and a denitrified atmosphere. Estimates of chemical ozone loss were derived using passive ozone from the SLIMCAT offline chemical transport model to account for dynamical contributions to the stratospheric ozone budget.&lt;/p&gt;

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