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

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.

2017 ◽  
Author(s):  
Yaoxian Huang ◽  
Shiliang Wu ◽  
Louisa J. Kramer ◽  
Detlev Helmig ◽  
Richard E. Honrath

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.


2017 ◽  
Vol 17 (14) ◽  
pp. 8757-8770 ◽  
Author(s):  
Roghayeh Ghahremaninezhad ◽  
Ann-Lise Norman ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  

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.


2012 ◽  
Vol 12 (15) ◽  
pp. 6723-6740 ◽  
Author(s):  
J. P. Parrella ◽  
D. J. Jacob ◽  
Q. Liang ◽  
Y. Zhang ◽  
L. J. Mickley ◽  
...  

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.


2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2011 ◽  
Vol 11 (2) ◽  
pp. 4105-4139 ◽  
Author(s):  
E. V. Fischer ◽  
D. A. Jaffe ◽  
E. C. Weatherhead

Abstract. We report on the first multi-year springtime measurements of PAN in the free troposphere over the US Pacific Northwest. The measurements were made at the summit of Mount Bachelor (43.979° N, 121.687° W; 2.7 km a.s.l.) by gas chromatography with electron capture detector during spring 2008, 2009, and 2010. This dataset provides an observational estimate of the month-to-month and springtime interannual variability of PAN mixing ratios in this region. Springtime seasonal mean (1 April–20 May) PAN mixing ratios at Mount Bachelor varied from 100 pptv to 152 pptv. The standard deviation of the three seasonal means was 28 pptv, 21% of the springtime mean. We focus on three factors that we expect to drive PAN variability: biomass burning, transport efficiency over the central and eastern Pacific, and transport temperature. There was an early and unusually strong fire source in southeastern Russia in spring 2008 due to early snow melt, and several fire plumes were observed at Mount Bachelor. Colder air mass transport from higher altitudes in April 2009 is consistent with the higher average PAN mixing ratios observed at MBO during this month. A trough located off the US Pacific Northwest coast in April 2010 caused reduced transport from the north in spring 2010 as compared to previous years. It also facilitated more frequent transport to Mount Bachelor during spring 2010 from the southwest and from lower elevations. Zhang et al. (2008) used the GEOS-Chem global chemical transport model to show that rising Asian NOx emissions from 2000 to 2006 resulted in a relatively larger positive trend in PAN than O3 over western North America. However the model results only considered monotonic changes in Asian emissions, whereas other factors, such as biomass burning, isoprene emissions or climate change can complicate the atmospheric concentrations. We combined the observed variability in PAN and O3 at Mount Bachelor with a range of possible trends in these species to determine the observational requirements to detect the trends. Though the relative increase in PAN is expected to be nearly four times larger than that of O3, PAN is more variable. If PAN mixing ratios are currently increasing at a rate of 4% per year due to rising Asian emissions, we would detect a trend with 13 yr of measurements at a site like Mount Bachelor. If the corresponding trend in O3 is 1% per year, the trends in O3 and PAN should be detected on approximately the same timescale.


2010 ◽  
Vol 10 (11) ◽  
pp. 26361-26410 ◽  
Author(s):  
H. Sodemann ◽  
M. Pommier ◽  
S. R. Arnold ◽  
S. A. Monks ◽  
K. Stebel ◽  
...  

Abstract. During the POLARCAT summer campaign in 2008, two episodes (2–5 July and 7–10 July 2008) occurred where low-pressure systems traveled from Siberia across the Arctic Ocean towards the North Pole. The two cyclones had extensive smoke plumes embedded in their associated air masses, creating an excellent opportunity to use satellite and aircraft observations to validate the performance of atmospheric transport models in the Arctic, which is a challenging model domain due to numerical and other complications. Here we compare transport simulations of carbon monoxide (CO) from the Lagrangian transport model FLEXPART, the Eulerian chemical transport model TOMCAT, and for numerical aspects the limited-area chemical transport model WRF-Chem. Retrievals of total column CO from the IASI passive infrared sensor onboard the MetOp-A satellite are used as a total column CO reference for the two simulations. Main aspect of the comparison is how realistic horizontal and vertical structures are represented in the model simulations. Analysis of CALIPSO lidar curtains and in situ aircraft measurements provide further independent reference points to assess how reliable the model simulations are and what the main limitations are. The horizontal structure of mid-latitude pollution plumes agrees well between the IASI total column CO and the model simulations. However, finer-scale structures are too quickly diffused in the Eulerian models. Aircraft data suggest that the satellite data are biased high, while TOMCAT and WRF-Chem are biased low. FLEXPART fits the aircraft data rather well, but due to added background concentrations the simulation is not independent from observations. The multi-data, multi-model approach allows separating the influences of meteorological fields, model realisation, and grid type on the plume structure. In addition to the very good agreement between simulated and observed total column CO fields, the results also highlight the difficulty to identify a data set that most realistically represents the actual state of the atmosphere.


2012 ◽  
Vol 12 (3) ◽  
pp. 6877-6908
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period, from December to mid-April, and a strong and stable vortex was present during that period. Analyses with the Mimosa-Chim CTM simulations show that the chemical ozone loss started by early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 40% from the ClO–ClO cycle and about 35–40% from the ClO-BrO cycle in late February and March, and about 30–50% from the HOx cycle in April. We also estimate a loss of around 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K also exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2018 ◽  
Author(s):  
Emma L. Mungall ◽  
Jonathan P. D. Abbatt ◽  
Jeremy J. B. Wentzell ◽  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
...  

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.


2017 ◽  
Author(s):  
Roghayeh Ghahremaninezhad ◽  
Ann-Lise Norman ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  

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.


2020 ◽  
Author(s):  
Xin Yang ◽  
Anne-M Blechschmidt ◽  
Kristof Bognar ◽  
Audra McClure–Begley ◽  
Sara Morris ◽  
...  

Abstract. Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites: Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish Realm), and ozonesonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models: a global chemistry transport model (p-TOMCAT) and a global chemistry climate model (UKCA), are used for model-data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument and ground-based Multi-axis Differential Optical Absorption Spectroscopy (MAX-DOAS) at Eureka, Canada are used for model validation. The observed climatology data show that spring surface ozone at coastal sites is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10–20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs) (defined as ozone volume mixing ratios VMRs 


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