scholarly journals Organic Functional Groups in the Submicron Aerosol at 82.5° N from 2012 to 2014

Author(s):  
W. Richard Leaitch ◽  
Lynn M. Russell ◽  
Jun Liu ◽  
Felicia Kolonjari ◽  
Desiree Toom ◽  
...  

Abstract. The first multi-year contributions from organic functional groups to the Arctic submicron aerosol are documented using 126 weekly-integrated samples collected from April, 2012 to October, 2014 at the Alert Observatory (82.45° N, 62.51° W). Results from the particle transport model FLEXPART, linear regressions among the organic and inorganic components and Positive Matrix Factorization (PMF) enable associations of organic aerosol components with source types and regions. Lower organic mass concentrations (OM) but higher ratios of OM to non-sea-salt sulphate mass concentrations (nss-SO4=) accompany smaller particles during the summer (JJA). Conversely, higher OM but lower OM/nss-SO4= accompany larger particles during winter-spring. OM ranges from 7–463 ng m−3, and the study average is 129 ng m−3. The monthly maximum in OM occurs during May, one month after the peak in nss-SO4= and two months after that of elemental carbon (EC). Winter (DJF), spring (MAM), summer and fall (SON) values of OM/nss-SO4= are 26 %, 28 %, 107 % and 39 %, respectively, and overall about 40 % of the weekly variability in the OM is associated with nss-SO4=. Respective study-averaged concentrations of alkane, alcohol, acid, amine and carbonyl groups are 57 ng m−3, 24 ng m−3, 23 ng m−3, 16 ng m−3 and 11 ng m−3, representing 42 %, 22 %, 18 %, 14 % and 5 % of the OM, respectively. Carbonyl groups, detected mostly during spring, may have a connection with snow chemistry. The seasonally highest O/C occurs during winter (0.85) and the lowest O/C is during spring (0.51); increases in O/C are largely due to increases in alcohol groups. During winter, more than 50 % of the alcohol groups are associated with primary marine emissions, consistent with Shaw et al. (2010) and Frossard et al. (2011). A secondary marine connection, rather than a primary source, is suggested for the highest and most persistence O/C observed during the coolest and cleanest summer (2013), when alcohol and acid groups made up 63% of the OM. A secondary marine source may be a general feature of the summer OM, but higher contributions from alkane groups to OM during the warmer summers of 2012 (53 %) and 2014 (50 %) were likely due to increased contributions from combustion sources. Evidence for significant contributions from biomass burning (BB) was present in 4 % of the weeks. During the dark months (NDJF), 29 %, 28 % and 14 % of the nss-SO4=, EC and OM were associated with transport times over the gas flaring region of Northern Russia and other parts of Eurasia. During spring, those percentages drop to 11 % and 8 % for nss-SO4= and EC, respectively, and there is no association of OM. Large percentages of the Arctic Haze characterized at Alert likely have origins farther than 10 days transport time and may be from outside of the Eurasian region. Possible sources of unusually high nss-SO4= and OM during September–October, 2014 are volcanic emissions or the Smoking Hills’ area of the Northwest Territories, Canada.

2018 ◽  
Vol 18 (5) ◽  
pp. 3269-3287 ◽  
Author(s):  
W. Richard Leaitch ◽  
Lynn M. Russell ◽  
Jun Liu ◽  
Felicia Kolonjari ◽  
Desiree Toom ◽  
...  

Abstract. The first multi-year contributions from organic functional groups to the Arctic submicron aerosol are documented using 126 weekly-integrated samples collected from April 2012 to October 2014 at the Alert Observatory (82.45° N, 62.51° W). Results from the particle transport model FLEXPART, linear regressions among the organic and inorganic components and positive matrix factorization (PMF) enable associations of organic aerosol components with source types and regions. Lower organic mass (OM) concentrations but higher ratios of OM to non-sea-salt sulfate mass concentrations (nss-SO4=) accompany smaller particles during the summer (JJA). Conversely, higher OM but lower OM ∕ nss-SO4= accompany larger particles during winter–spring. OM ranges from 7 to 460 ng m−3, and the study average is 129 ng m−3. The monthly maximum in OM occurs during May, 1 month after the peak in nss-SO4= and 2 months after that of elemental carbon (EC). Winter (DJF), spring (MAM), summer and fall (SON) values of OM ∕ nss-SO4= are 26, 28, 107 and 39 %, respectively, and overall about 40 % of the weekly variability in the OM is associated with nss-SO4=. Respective study-averaged concentrations of alkane, alcohol, acid, amine and carbonyl groups are 57, 24, 23, 15 and 11 ng m−3, representing 42, 22, 18, 14 and 5 % of the OM, respectively. Carbonyl groups, detected mostly during spring, may have a connection with snow chemistry. The seasonally highest O ∕ C occurs during winter (0.85) and the lowest O ∕ C is during spring (0.51); increases in O ∕ C are largely due to increases in alcohol groups. During winter, more than 50 % of the alcohol groups are associated with primary marine emissions, consistent with Shaw et al. (2010) and Frossard et al. (2011). A secondary marine connection, rather than a primary source, is suggested for the highest and most persistent O ∕ C observed during the coolest and cleanest summer (2013), when alcohol and acid groups made up 63 % of the OM. A secondary marine source may be a general feature of the summer OM, but higher contributions from alkane groups to OM during the warmer summers of 2012 (53 %) and 2014 (50 %) were likely due to increased contributions from combustion sources. Evidence for significant contributions from biomass burning (BB) was present in 4 % of the weeks. During the dark months (NDJF), 29, 28 and 14 % of the nss-SO4=, EC and OM were associated with transport times over the gas flaring region of northern Russia and other parts of Eurasia. During spring, those percentages dropped to 11 % for each of nss-SO4= and EC values, respectively, and there is no association of OM. Large percentages of the Arctic haze characterized at Alert likely have origins farther than 10 days of transport time and may be from outside of the Eurasian region. Possible sources of unusually high nss-SO4= and OM during September–October 2014 are volcanic emissions or the Smoking Hills' area of the Northwest Territories, Canada.


2017 ◽  
Author(s):  
W. Richard Leaitch ◽  
Lynn M. Russell ◽  
Jun Liu ◽  
Felicia Kolonjari ◽  
Desiree Toom ◽  
...  

2014 ◽  
Vol 14 (7) ◽  
pp. 3247-3276 ◽  
Author(s):  
R. Hommel ◽  
K.-U. Eichmann ◽  
J. Aschmann ◽  
K. Bramstedt ◽  
M. Weber ◽  
...  

Abstract. Record breaking loss of ozone (O3) in the Arctic stratosphere has been reported in winter–spring 2010/2011. We examine in detail the composition and transformations occurring in the Arctic polar vortex using total column and vertical profile data products for O3, bromine oxide (BrO), nitrogen dioxide (NO2), chlorine dioxide (OClO), and polar stratospheric clouds (PSC) retrieved from measurements made by SCIAMACHY (Scanning Imaging Absorption SpectroMeter for Atmospheric CHartography) on-board Envisat (Environmental Satellite), as well as total column ozone amount, retrieved from the measurements of GOME-2 (Global Ozone Monitoring Experiment) on MetOp-A (Meteorological Experimental Satellite). Similarly we use the retrieved data from DOAS (Differential Optical Absorption Spectroscopy) measurements made in Ny-Ålesund (78.55° N, 11.55° E). A chemical transport model (CTM) has been used to relate and compare Arctic winter–spring conditions in 2011 with those in the previous year. In late winter–spring 2010/2011 the chemical ozone loss in the polar vortex derived from SCIAMACHY observations confirms findings reported elsewhere. More than 70% of O3 was depleted by halogen catalytic cycles between the 425 and 525 K isentropic surfaces, i.e. in the altitude range ~16–20 km. In contrast, during the same period in the previous winter 2009/2010, a typical warm Arctic winter, only slightly more than 20% depletion occurred below 20 km, while 40% of O3 was removed above the 575 K isentrope (~23 km). This loss above 575 K is explained by the catalytic destruction by NOx descending from the mesosphere. In both Arctic winters 2009/2010 and 2010/2011, calculated O3 losses from the CTM are in good agreement to our observations and other model studies. The mid-winter 2011 conditions, prior to the catalytic cycles being fully effective, are also investigated. Surprisingly, a significant loss of O3 around 60%, previously not discussed in detail, is observed in mid-January 2011 below 500 K (~19 km) and sustained for approximately 1 week. The low O3 region had an exceptionally large spatial extent. The situation was caused by two independently evolving tropopause elevations over the Asian continent. Induced adiabatic cooling of the stratosphere favoured the formation of PSC, increased the amount of active chlorine for a short time, and potentially contributed to higher polar ozone loss later in spring.


2008 ◽  
Vol 8 (12) ◽  
pp. 3337-3367 ◽  
Author(s):  
G. B. Hedegaard ◽  
J. Brandt ◽  
J. H. Christensen ◽  
L. M. Frohn ◽  
C. Geels ◽  
...  

Abstract. The response of a selected number of chemical species is inspected with respect to climate change. The coupled Atmosphere-Ocean General Circulation Model ECHAM4-OPYC3 is providing meteorological fields for the Chemical long-range Transport Model DEHM. Three selected decades (1990s, 2040s and 2090s) are inspected. The 1990s are used as a reference and validation period. In this decade an evaluation of the output from the DEHM model with ECHAM4-OPYC3 meteorology input data is carried out. The model results are tested against similar model simulations with MM5 meteorology and against observations from the EMEP monitoring sites in Europe. The test results from the validation period show that the overall statistics (e.g. mean values and standard deviations) are similar for the two simulations. However, as one would expect the model setup with climate input data fails to predict correctly the timing of the variability in the observations. The overall performance of the ECHAM4-OPYC3 setup as meteorological input to the DEHM model is shown to be acceptable according to the applied ranking method. It is concluded that running a chemical long-range transport model on data from a "free run" climate model is scientifically sound. From the model runs of the three decades, it is found that the overall trend detected in the evolution of the chemical species, is the same between the 1990 decade and the 2040 decade and between the 2040 decade and the 2090 decade, respectively. The dominating impacts from climate change on a large number of the chemical species are related to the predicted temperature increase. Throughout the 21th century the ECHAM4-OPYC3 projects a global mean temperature increase of 3 K with local maxima up to 11 K in the Arctic winter based on the IPCC A2 emission scenario. As a consequence of this temperature increase, the temperature dependent biogenic emission of isoprene is predicted to increase significantly over land by the DEHM model. This leads to an increase in the O3 production and together with an increase in water vapor to an increase in the number of free OH radicals. Furthermore this increase in the number of OH radicals contributes to a significant change in the typical life time of many species, since OH are participating in a large number of chemical reactions. It is e.g. found that more SO42− will be present in the future over the already polluted areas and this increase can be explained by an enhanced conversion of SO2 to SO42−.


Complexity ◽  
2006 ◽  
Vol 11 (3) ◽  
pp. 9-10 ◽  
Author(s):  
Harold J. Morowitz ◽  
Vijayasarathy Srinivasan ◽  
Eric Smith

1969 ◽  
Vol 57 (4) ◽  
pp. 821-825 ◽  
Author(s):  
Walter L. Nazimowitz ◽  
T. S. Ma

2021 ◽  
Author(s):  
Ramina Alwarda ◽  
Kristof Bognar ◽  
Kimberly Strong ◽  
Martyn Chipperfield ◽  
Sandip Dhomse ◽  
...  

<p>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°N, 86.42°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<sub>2</sub> during spring, as well as enhanced reactive halogen species (OClO and BrO). Complementary measurements of HCl and ClONO<sub>2</sub> (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<sub>3</sub> 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.</p>


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