scholarly journals Tropospheric BrO column densities in the Arctic derived from satellite: retrieval and comparison to ground-based measurements

2012 ◽  
Vol 5 (11) ◽  
pp. 2779-2807 ◽  
Author(s):  
H. Sihler ◽  
U. Platt ◽  
S. Beirle ◽  
T. Marbach ◽  
S. Kühl ◽  
...  

Abstract. During polar spring, halogen radicals like bromine monoxide (BrO) play an important role in the chemistry of tropospheric ozone destruction. Satellite measurements of the BrO distribution have become a particularly useful tool to investigate this probably natural phenomenon, but the separation of stratospheric and tropospheric partial columns of BrO is challenging. In this study, an algorithm was developed to retrieve tropospheric vertical column densities of BrO from data of high-resolution spectroscopic satellite instruments such as the second Global Ozone Monitoring Experiment (GOME-2). Unlike recently published approaches, the presented algorithm is capable of separating the fraction of BrO in the activated troposphere from the total BrO column solely based on remotely measured properties. The presented algorithm furthermore allows to estimate a realistic measurement error of the tropospheric BrO column. The sensitivity of each satellite pixel to BrO in the boundary layer is quantified using the measured UV radiance and the column density of the oxygen collision complex O4. A comparison of the sensitivities with CALIPSO LIDAR observations demonstrates that clouds shielding near-surface trace-gas columns can be reliably detected even over ice and snow. Retrieved tropospheric BrO columns are then compared to ground-based BrO measurements from two Arctic field campaigns in the Amundsen Gulf and at Barrow in 2008 and 2009, respectively. Our algorithm was found to be capable of retrieving enhanced near-surface BrO during both campaigns in good agreement with ground-based data. Some differences between ground-based and satellite measurements observed at Barrow can be explained by both elevated and shallow surface layers of BrO. The observations strongly suggest that surface release processes are the dominating source of BrO and that boundary layer meteorology influences the vertical distribution.

2012 ◽  
Vol 5 (3) ◽  
pp. 3199-3270 ◽  
Author(s):  
H. Sihler ◽  
U. Platt ◽  
S. Beirle ◽  
T. Marbach ◽  
S. Kühl ◽  
...  

Abstract. During polar spring, halogen radicals like bromine monoxide (BrO) play an important role in the chemistry of tropospheric ozone destruction. Satellite measurements of the BrO-distribution have become a particularly useful tool to investigate this probably natural phenomenon, but the separation of stratospheric and tropospheric partial columns of BrO is challenging. In this study, an algorithm was developed to retrieve tropospheric vertical column densities of BrO from data of high-resolution spectroscopic satellite instruments such as the second Global Ozone Monitoring Experiment (GOME-2). Unlike recently published approaches, the presented algorithm is capable of separating the fraction of BrO in the activated troposphere from the total BrO column solely based on remotely measured properties. The sensitivity of each satellite pixel to BrO in the boundary-layer is quantified using the measured UV-radiance and the column density of the oxygen collision complex O4. A comparison of the sensitivities with CALIPSO LIDAR observations demonstrates that clouds shielding near-surface trace-gas columns can be reliably detected even over ice and snow. Retrieved tropospheric BrO columns are then compared to ground-based BrO measurements from two Arctic field campaigns in the Amundsen Gulf and at Barrow in 2008 and 2009, respectively. Our algorithm was found to be capable of retrieving enhanced near-surface BrO during both campaigns in good agreement to ground-based data. Some differences between ground-based and satellite measurements observed at Barrow can be explained by both, elevated and shallow surface layers of BrO. The observations strongly suggest that surface release processes are the dominating source of BrO and that boundary-layer meteorology influences the vertical distribution.


2008 ◽  
Vol 8 (3) ◽  
pp. 505-522 ◽  
Author(s):  
G. L. Manney ◽  
W. H. Daffer ◽  
K. B. Strawbridge ◽  
K. A. Walker ◽  
C. D. Boone ◽  
...  

Abstract. The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.


2011 ◽  
Vol 11 (4) ◽  
pp. 12411-12440 ◽  
Author(s):  
A. R. Russell ◽  
A. E. Perring ◽  
L. C. Valin ◽  
E. Bucsela ◽  
E. C. Browne ◽  
...  

Abstract. We present a new retrieval of tropospheric NO2 vertical column density from the Ozone Monitoring Instrument (OMI) based on high spatial and temporal resolution terrain and profile inputs. We find non-negligible impacts on the retrieved NO2 column for terrain pressure (±20%), albedo (±40%), and NO2 vertical profile (−75%–+10%). We compare our NO2 product, the Berkeley High-Resolution (BEHR) product, with operational retrievals and find that the operational retrievals are biased high (30%) over remote areas and biased low (8%) over urban regions. We validate the operational and BEHR products using boundary layer aircraft observations from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS-CA) field campaign which occurred in June 2008 in California. Results indicate that columns derived using our boundary layer extrapolation method show good agreement with satellite observations (R2 = 0.65–0.83; N = 68) and provide a more robust validation of satellite-observed NO2 column than those determined using full vertical spirals (R2 = 0.26; N = 5) as in previous work. Agreement between aircraft observations and the BEHR product (R2 = 0.83) is better than agreement with the operational products (R2 = 0.65–0.72). We also show that agreement between satellite and aircraft observations for all products can be further improved (e.g. BEHR: R2 = 0.91) using cloud information from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument instead of the OMI cloud product. These results indicate that much of the variance in the operational products can be attributed to coarse resolution terrain and profile parameters.


Author(s):  
Jason Welsh ◽  
Jack Fishman

We use a regional scale photochemical transport model to investigate the surface concentrations and column integrated amounts of ozone (O3) and nitrogen dioxide (NO2) during a pollution event that occurred in the St. Louis metropolitan region in 2012. These trace gases will be two of the primary constituents that will be measured by TEMPO, an instrument on a geostationary platform, which will result in a dataset that has hourly temporal resolution during the daytime and ~4 km spatial resolution. Although air quality managers are most concerned with surface concentrations, satellite measurements provide a quantity that reflects a column amount, which may or may not be directly relatable to what is measured at the surface. The model results provide good agreement with observed surface O3 concentrations, which is the only trace gas dataset that can be used for verification. The model shows that a plume of O3 extends downwind from St. Louis and contains an integrated amount of ozone of ~ 16 DU (1 DU = 2.69 x 1016 mol. cm-2), a quantity that is two to three times lower than what was observed by satellite measurements during two massive pollution episodes in the 1980s. Based on the smaller isolatable emissions coming from St. Louis, this quantity is not unreasonable, but may also reflect the reduction of photochemical ozone production due to the implementation of emission controls that have gone into effect in the past few decades.


2019 ◽  
Vol 59 ◽  
pp. 9.1-9.85 ◽  
Author(s):  
Margaret A. LeMone ◽  
Wayne M. Angevine ◽  
Christopher S. Bretherton ◽  
Fei Chen ◽  
Jimy Dudhia ◽  
...  

AbstractOver the last 100 years, boundary layer meteorology grew from the subject of mostly near-surface observations to a field encompassing diverse atmospheric boundary layers (ABLs) around the world. From the start, researchers drew from an ever-expanding set of disciplines—thermodynamics, soil and plant studies, fluid dynamics and turbulence, cloud microphysics, and aerosol studies. Research expanded upward to include the entire ABL in response to the need to know how particles and trace gases dispersed, and later how to represent the ABL in numerical models of weather and climate (starting in the 1970s–80s); taking advantage of the opportunities afforded by the development of large-eddy simulations (1970s), direct numerical simulations (1990s), and a host of instruments to sample the boundary layer in situ and remotely from the surface, the air, and space. Near-surface flux-profile relationships were developed rapidly between the 1940s and 1970s, when rapid progress shifted to the fair-weather convective boundary layer (CBL), though tropical CBL studies date back to the 1940s. In the 1980s, ABL research began to include the interaction of the ABL with the surface and clouds, the first ABL parameterization schemes emerged; and land surface and ocean surface model development blossomed. Research in subsequent decades has focused on more complex ABLs, often identified by shortcomings or uncertainties in weather and climate models, including the stable boundary layer, the Arctic boundary layer, cloudy boundary layers, and ABLs over heterogeneous surfaces (including cities). The paper closes with a brief summary, some lessons learned, and a look to the future.


2011 ◽  
Vol 11 (16) ◽  
pp. 8543-8554 ◽  
Author(s):  
A. R. Russell ◽  
A. E. Perring ◽  
L. C. Valin ◽  
E. J. Bucsela ◽  
E. C. Browne ◽  
...  

Abstract. We present a new retrieval of tropospheric NO2 vertical column density from the Ozone Monitoring Instrument (OMI) based on high spatial and temporal resolution terrain and profile inputs. We compare our NO2 product, the Berkeley High-Resolution (BEHR) product, with operational retrievals and find that the operational retrievals are biased high (30 %) over remote areas and biased low (8 %) over urban regions. Additionally, we find non-negligible impacts on the retrieved NO2 column for terrain pressure (±20 %), albedo (±40 %), and NO2 vertical profile (−75 %–+10 %). We validate the operational and BEHR products using boundary layer aircraft observations from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS-CA) field campaign which occurred in June 2008 in California. Results indicate that columns derived using our boundary layer extrapolation method show good agreement with satellite observations (R2 = 0.65–0.83; N = 68) and provide a more robust validation of satellite-observed NO2 column than those determined using full vertical spirals (R2 = 0.26; N = 5) as in previous work. Agreement between aircraft observations and the BEHR product (R2 = 0.83) is better than agreement with the operational products (R2 = 0.65–0.72). We also show that agreement between satellite and aircraft observations can be further improved (e.g. BEHR: R2 = 0.91) using cloud information from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument instead of the OMI cloud product. These results indicate that much of the variance in the operational products can be attributed to coarse resolution terrain pressure, albedo, and profile parameters implemented in the retrievals.


2012 ◽  
Vol 5 (5) ◽  
pp. 7641-7673 ◽  
Author(s):  
R. Sinreich ◽  
A. Merten ◽  
L. Molina ◽  
R. Volkamer

Abstract. We present a novel parameterization method to convert Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) differential Slant Column Densities (dSCDs) into near-surface box averaged volume mixing ratios. The approach is applicable inside the planetary boundary layer under conditions with significant aerosol load, does not require a-priori assumptions about the trace gas vertical distribution and builds on the increased sensitivity of MAX-DOAS near the instrument altitude. It parameterizes radiative transfer model calculations and significantly reduces the computational effort. The biggest benefit of this method is that the retrieval of an aerosol profile, which usually is necessary for deriving a trace gas concentration from MAX-DOAS dSCDs, is not needed. The method is applied to NO2 MAX-DOAS dSCDs recorded during the Mexico City Metropolitan Area 2006 (MCMA-2006) measurement campaign. The retrieved volume mixing ratios of two elevation angles (1° and 3°) are compared to volume mixing ratios measured by two long-path (LP)-DOAS instruments located at the same site. Measurements are found to agree well during times when vertical mixing is expected to be strong. However, inhomogeneities in the air mass above Mexico City can be detected by exploiting the different horizontal and vertical dimensions probed by MAX-DOAS measurements at different elevation angles, and by LP-DOAS. In particular, a vertical gradient in NO2 close to the ground can be observed in the afternoon, and is attributed to reduced mixing coupled with near surface emission. The existence of a vertical gradient in the lower 250 m during parts of the day shows the general challenge of sampling the boundary layer in a representative way and emphasizes the need of vertically resolved measurements.


2020 ◽  
Vol 20 (20) ◽  
pp. 11869-11892
Author(s):  
Ilias Bougoudis ◽  
Anne-Marlene Blechschmidt ◽  
Andreas Richter ◽  
Sora Seo ◽  
John Philip Burrows ◽  
...  

Abstract. Every polar spring, phenomena called bromine explosions occur over sea ice. These bromine explosions comprise photochemical heterogeneous chain reactions that release bromine molecules, Br2, to the troposphere and lead to tropospheric plumes of bromine monoxide, BrO. This autocatalytic mechanism depletes ozone, O3, in the boundary layer and troposphere and thereby changes the oxidizing capacity of the atmosphere. The phenomenon also leads to accelerated deposition of metals (e.g., Hg). In this study, we present a 22-year (1996 to 2017) consolidated and consistent tropospheric BrO dataset north of 70∘ N, derived from four different ultraviolet–visible (UV–VIS) satellite instruments (GOME, SCIAMACHY, GOME-2A and GOME-2B). The retrieval data products from the different sensors are compared during periods of overlap and show good agreement (correlations of 0.82–0.98 between the sensors). From our merged time series of tropospheric BrO vertical column densities (VCDs), we infer changes in the bromine explosions and thus an increase in the extent and magnitude of tropospheric BrO plumes during the period of Arctic warming. We determined an increasing trend of about 1.5 % of the tropospheric BrO VCDs per year during polar springs, while the size of the areas where enhanced tropospheric BrO VCDs can be found has increased about 896 km2 yr−1. We infer from comparisons and correlations with sea ice age data that the reported changes in the extent and magnitude of tropospheric BrO VCDs are moderately related to the increase in first-year ice extent in the Arctic north of 70∘ N, both temporally and spatially, with a correlation coefficient of 0.32. However, the BrO plumes and thus bromine explosions show significant variability, which also depends, apart from sea ice, on meteorological conditions.


Author(s):  
Jason Welsh ◽  
Jack Fishman

We use a regional scale photochemical transport model to investigate the surface concentrations and column integrated amounts of ozone (O3) and nitrogen dioxide (NO2) during a pollution event that occurred in the St. Louis metropolitan region in 2012. These trace gases will be two of the primary constituents that will be measured by TEMPO (Tropospheric Emissions: Monitoring of Pollution), an instrument on a geostationary platform, which will result in a dataset that has hourly temporal resolution during the daytime and ~4 km spatial resolution. Although air quality managers are most concerned with surface concentrations, satellite measurements provide a quantity that reflects a column amount, which may or may not be directly relatable to what is measured at the surface. Our model results provide reasonably good agreement with observed surface O3 concentrations (correlation coefficients ranging from 0.69 to 0.87 at each of the nine monitoring stations in the St. Louis region), which is the only trace gas dataset that can be used for verification. The model shows that a plume of O3 extends downwind from St. Louis and contains an integrated amount of ozone of ~ 16 Dobson Units (DU; 1 DU = 2.69 x 1016 molecules cm-2), an amount lower than what was observed during two massive pollution episodes in the 1980s. Based on the smaller isolatable emissions coming from St. Louis, this quantity is not unreasonable, but may also reflect the reduction of photochemical ozone production due to the implementation of emission controls that have gone into effect since the 1980s.


2003 ◽  
Vol 3 (6) ◽  
pp. 5755-5775 ◽  
Author(s):  
G. P. Gobbi ◽  
F. Barnaba

Abstract. A set of 813 lidar profiles of tropospheric aerosol and cirrus clouds extinction and depolarization observed at Rome, Italy, between February 2001 and February 2002 is analyzed and discussed. The yearly record reveals a meaningful contribution of both cirrus clouds (38%) and Saharan dust (12%) to the total optical thickness (OT) of 0.26, at 532 nm. Seasonal analysis shows the planetary boundary layer (PBL) aerosols to be confined below 2 km in winter and 3.8 km in summer, with relevant OT shifting from 0.08 to 0.16, respectively. Cirrus clouds maximize in spring and autumn, in both cases with average OT similar to the PBL aerosols one. With the exception of winter months, Saharan dust is found to represent an important third layer mostly residing between PBL aerosols and cirrus clouds, with yearly average OT~0.03. Saharan dust and cirrus clouds were detected in 20% and in 45% of the observational days, respectively. Validation of the lidar OT retrievals against collocated sunphotometer observations show very good agreement. These results represent one of the few yearly records of tropospheric aerosol vertical profiles available in the literature.


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