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 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 Dimethyl sulfide in the summertime Arctic atmosphere: measurements and source sensitivity simulations

2016 ◽  
Vol 16 (11) ◽  
pp. 6665-6680 ◽  
Author(s):  
Emma L. Mungall ◽  
Betty Croft ◽  
Martine Lizotte ◽  
Jennie L. Thomas ◽  
Jennifer G. Murphy ◽  
...  
Keyword(s):  
Dimethyl Sulfide ◽  
Transport Model ◽  
Sulfur Cycle ◽  
Oxidation Products ◽  
The Arctic ◽  
High Time Resolution ◽  
Study Region ◽  
Baffin Bay ◽  
Mixing Ratios ◽  
Arctic Atmosphere

Abstract. Dimethyl sulfide (DMS) plays a major role in the global sulfur cycle. In addition, its atmospheric oxidation products contribute to the formation and growth of atmospheric aerosol particles, thereby influencing cloud condensation nuclei (CCN) populations and thus cloud formation. The pristine summertime Arctic atmosphere is strongly influenced by DMS. However, atmospheric DMS mixing ratios have only rarely been measured in the summertime Arctic. During July–August, 2014, we conducted the first high time resolution (10 Hz) DMS mixing ratio measurements for the eastern Canadian Archipelago and Baffin Bay as one component of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments (NETCARE). DMS mixing ratios ranged from below the detection limit of 4 to 1155 pptv (median 186 pptv) during the 21-day shipboard campaign. A transfer velocity parameterization from the literature coupled with coincident atmospheric and seawater DMS measurements yielded air–sea DMS flux estimates ranging from 0.02 to 12 µmol m−2 d−1. Air-mass trajectory analysis using FLEXPART-WRF and sensitivity simulations with the GEOS-Chem chemical transport model indicated that local sources (Lancaster Sound and Baffin Bay) were the dominant contributors to the DMS measured along the 21-day ship track, with episodic transport from the Hudson Bay System. After adjusting GEOS-Chem oceanic DMS values in the region to match measurements, GEOS-Chem reproduced the major features of the measured time series but was biased low overall (2–1006 pptv, median 72 pptv), although within the range of uncertainty of the seawater DMS source. However, during some 1–2 day periods the model underpredicted the measurements by more than an order of magnitude. Sensitivity tests indicated that non-marine sources (lakes, biomass burning, melt ponds, and coastal tundra) could make additional episodic contributions to atmospheric DMS in the study region, although local marine sources of DMS dominated. Our results highlight the need for both atmospheric and seawater DMS data sets with greater spatial and temporal resolution, combined with further investigation of non-marine DMS sources for the Arctic.

scholarly journals Observations of filamentary structures near the vortex edge in the Arctic winter lower stratosphere

2013 ◽  
Vol 13 (21) ◽  
pp. 10859-10871 ◽  
Author(s):  
C. Kalicinsky ◽  
J.-U. Grooß ◽  
G. Günther ◽  
J. Ungermann ◽  
J. Blank ◽  
...  
Keyword(s):  
Cross Sections ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
The Arctic ◽  
Small Scale ◽  
Air Mass ◽  
Mixing Ratios ◽  
Passive Tracers

Abstract. The CRISTA-NF (Cryogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers) instrument is an airborne infrared limb sounder operated aboard the Russian research aircraft M55-Geophysica. The instrument successfully participated in a large Arctic aircraft campaign within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) project in Kiruna (Sweden) from January to March 2010. This paper concentrates on the measurements taken during one flight of the campaign, which took place on 2 March in the vicinity of the polar vortex. We present two-dimensional cross-sections of derived volume mixing ratios for the trace gases CFC-11, O3, and ClONO2 with an unprecedented vertical resolution of about 500 to 600 m for a large part of the observed altitude range (≈ 6–19 km) and a dense horizontal sampling along flight direction of ≈ 15 km. The trace gas distributions show several structures, for example a part of the polar vortex and a vortex filament, which can be identified by means of O3–CFC-11 tracer–tracer correlations. The observations made during this flight are interpreted using the chemistry and transport model CLaMS (Chemical Lagrangian Model of the Stratosphere). Comparisons of the observations with the model results are used to assess the performance of the model with respect to advection, mixing, and the chemistry in the polar vortex. These comparisons confirm the capability of CLaMS to reproduce even very small-scale structures in the atmosphere, which partly have a vertical extent of only 1 km. Based on the good agreement between simulation and observation, we use artificial (passive) tracers, which represent different air mass origins (e.g. vortex, tropics), to further analyse the CRISTA-NF observations in terms of the composition of air mass origins. These passive tracers clearly illustrate the observation of filamentary structures that include tropical air masses. A characteristic of the Arctic winter 2009/10 was a sudden stratospheric warming in December that led to a split of the polar vortex. The vortex re-established at the end of December. Our passive tracer simulations suggest that large parts of the re-established vortex consisted to about 45% of high- and mid-latitude air.

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 MAX-DOAS measurements of NO<sub>2</sub>, HCHO and CHOCHO at a rural site in Southern China

2012 ◽  
Vol 12 (2) ◽  
pp. 3983-4029 ◽  
Author(s):  
X. Li ◽  
T. Brauers ◽  
A. Hofzumahaus ◽  
K. Lu ◽  
Y. P. Li ◽  
...  
Keyword(s):  
Transport Model ◽  
Southern China ◽  
High Ratio ◽  
Rural Site ◽  
Pearl River Delta Region ◽  
Chemical Transport Model ◽  
Vertical Column ◽  
Mixing Ratios ◽  
In Situ Data ◽  
Vertical Distributions

Abstract. We performed MAX-DOAS measurements during the PRIDE-PRD2006 campaign in the Pearl River Delta region (PRD), China, for 4 weeks in July 2006 at a site located 60 km north of Guangzhou. The vertical distributions of NO2, HCHO, and CHOCHO were independently retrieved by an automated iteration method. The MAX-DOAS measured NO2 mixing ratios showed reasonable agreement with the simultaneous, ground based in-situ data. While the tropospheric NO2 vertical column densities (VCDs) observed by OMI on board EOS-Aura satellite agreed with those by MAX-DOAS, the 3-D chemical transport model CMAQ overestimated the NO2 VCDs as well as the surface concentrations by about 40%. From this observation, a reduction of NOX emission strength in CMAQ seems to be necessary in order to well reproduce the NO2 observations. The average mixing ratios of HCHO and CHOCHO were 12 ppb and 1.6 ppb, respectively, substantially higher than in other rural or semirural environments. The high ratio of 0.135 between CHOCHO and HCHO corresponds to the high VOCs reactivity and high HOX turnover rate consistent with other observations during the campaign.

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 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 MAX-DOAS measurements of NO<sub>2</sub>, HCHO and CHOCHO at a rural site in Southern China

2013 ◽  
Vol 13 (4) ◽  
pp. 2133-2151 ◽  
Author(s):  
X. Li ◽  
T. Brauers ◽  
A. Hofzumahaus ◽  
K. Lu ◽  
Y. P. Li ◽  
...  
Keyword(s):  
Transport Model ◽  
Southern China ◽  
High Ratio ◽  
Rural Site ◽  
Pearl River Delta Region ◽  
Chemical Transport Model ◽  
Vertical Column ◽  
Mixing Ratios ◽  
In Situ Data ◽  
Vertical Distributions

Abstract. We performed MAX-DOAS measurements during the PRIDE-PRD2006 campaign in the Pearl River Delta region (PRD), China, for 4 weeks in July 2006 at a site located 60 km north of Guangzhou. The vertical distributions of NO2, HCHO, and CHOCHO were independently retrieved by an automated iteration method. The NO2 mixing ratios measured by MAX-DOAS showed reasonable agreement with the simultaneous, ground based in-situ data. The tropospheric NO2 vertical column densities (VCDs) observed by OMI on board EOS-Aura satellite were higher than with those by MAX-DOAS. The 3-D chemical transport model CMAQ overestimated the NO2 VCDs as well as the surface concentrations by about 65%. From this observation, a reduction of NOx emission strength in CMAQ seems to be necessary in order to well reproduce the NO2 observations. The average mixing ratios of HCHO and CHOCHO were 7 ppb and 0.4 ppb, respectively, higher than in other rural or semirural environments. The high ratio of 0.062 between CHOCHO and HCHO corresponds to the high VOCs reactivity and high HOx turnover rate consistent with other observations during the campaign.

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.

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