scholarly journals Airborne DOAS limb measurements of tropospheric trace gas profiles: case study on the profile retrieval of O<sub>4</sub> and BrO

2010 ◽  
Vol 3 (4) ◽  
pp. 3925-3969 ◽  
Author(s):  
C. Prados-Roman ◽  
A. Butz ◽  
T. Deutschmann ◽  
M. Dorf ◽  
L. Kritten ◽  
...  

Abstract. A novel limb scanning mini-DOAS spectrometer for the detection of UV/vis absorbing radicals (e.g., O3, BrO, IO, HONO) was deployed on the DLR-Falcon (Deutsches Zentrum für Luft- und Raumfahrt) aircraft and tested during the ASTAR 2007 campaign (Arctic Study of Tropospheric Aerosol, Clouds and Radiation) that took place at Svalbard (78° N) in spring 2007. Our main objectives during this campaign were to test the instrument, and to perform spectral and profile retrievals of tropospheric trace gases, with particular interest on investigating the distribution of halogen compounds (e.g., BrO) during the so-called ozone depletion events (ODEs). In the present work, a new method for the retrieval of vertical profiles of tropospheric trace gases from tropospheric DOAS limb observations is presented. Major challenges arise from modeling the radiative transfer in an aerosol and cloud particle loaded atmosphere, and from overcoming the lack of a priori knowledge of the targeted trace gas vertical distribution (e.g., unknown tropospheric BrO vertical distribution). Here, those challenges are tackled by a mathematical inversion of tropospheric trace gas profiles using a regularization approach constrained by a retrieved vertical profile of the aerosols extinction coefficient εM. The validity and limitations of the algorithm are tested with in situ measured εM, and with an absorber of known vertical profile (O4). The method is then used for retrieving vertical profiles of tropospheric BrO. Results indicate that, for aircraft ascent/descent observations, the limit for the BrO detection is roughly 1.5 pptv (pmol/mol), and the BrO profiles inferred from the boundary layer up to the upper troposphere and lower stratosphere have around 10 degrees of freedom. For the ASTAR 2007 deployments during ODEs, the retrieved BrO vertical profiles consistently indicate high BrO mixing ratios (~15 pptv) within the boundary layer, low BrO mixing ratios (≤1.5 pptv) in the free troposphere, occasionally enhanced BrO mixing ratios (~1.5 pptv) in the upper troposphere, and increasing BrO mixing ratios with altitude in the lowermost stratosphere. These findings are well in agreement with satellite and balloon-borne soundings of total and partial BrO atmospheric column densities.

2011 ◽  
Vol 4 (6) ◽  
pp. 1241-1260 ◽  
Author(s):  
C. Prados-Roman ◽  
A. Butz ◽  
T. Deutschmann ◽  
M. Dorf ◽  
L. Kritten ◽  
...  

Abstract. A novel limb scanning mini-DOAS spectrometer for the detection of UV/vis absorbing radicals (e.g., O3, BrO, IO, HONO) was deployed on the DLR-Falcon (Deutsches Zentrum für Luft- und Raumfahrt) aircraft and tested during the ASTAR 2007 campaign (Arctic Study of Tropospheric Aerosol, Clouds and Radiation) that took place at Svalbard (78° N) in spring 2007. Our main objectives during this campaign were to test the instrument, and to perform spectral and profile retrievals of tropospheric trace gases, with particular interest on investigating the distribution of halogen compounds (e.g., BrO) during the so-called ozone depletion events (ODEs). In the present work, a new method for the retrieval of vertical profiles of tropospheric trace gases from tropospheric DOAS limb observations is presented. Major challenges arise from modeling the radiative transfer in an aerosol and cloud particle loaded atmosphere, and from overcoming the lack of a priori knowledge of the targeted trace gas vertical distribution (e.g., unknown tropospheric BrO vertical distribution). Here, those challenges are tackled by a mathematical inversion of tropospheric trace gas profiles using a regularization approach constrained by a retrieved vertical profile of the aerosols extinction coefficient EM. The validity and limitations of the algorithm are tested with in situ measured EM, and with an absorber of known vertical profile (O4). The method is then used for retrieving vertical profiles of tropospheric BrO. Results indicate that, for aircraft ascent/descent observations, the limit for the BrO detection is roughly 1.5 pptv (pmol mol−1), and the BrO profiles inferred from the boundary layer up to the upper troposphere and lower stratosphere have around 10 degrees of freedom. For the ASTAR 2007 deployments during ODEs, the retrieved BrO vertical profiles consistently indicate high BrO mixing ratios (∼15 pptv) within the boundary layer, low BrO mixing ratios (&amp;leq;1.5 pptv) in the free troposphere, occasionally enhanced BrO mixing ratios (∼1.5 pptv) in the upper troposphere, and increasing BrO mixing ratios with altitude in the lowermost stratosphere. These findings agree reasonably well with satellite and balloon-borne soundings of total and partial BrO atmospheric column densities.


2020 ◽  
Author(s):  
Michael Revesz ◽  
Stefan F. Schreier ◽  
Philipp Weihs ◽  
Tim Bösch ◽  
Kezia Lange ◽  
...  

&lt;p&gt;Within the project VINDOBONA (VIenna horizontal aNd vertical Distribution OBservations Of Nitrogen dioxide and Aerosols), a method was developed to retrieve the spatial distribution of trace gases using data from three ground based MAX-DOAS instruments and was applied on the example of NO&lt;sub&gt;2&lt;/sub&gt;. At three different locations in Vienna (Austria) MAX-DOAS instruments were installed performing measurements in the visible and UV spectral range. Currently, each instrument is set up to determine the column densities in different azimuthal directions and low elevation angles within approximately a horizontal plane. The different lines of sight of the three instruments intersect horizontally and can be used to estimate the horizontal spatial distribution of trace gases. With the knowledge of vertical profiles, even the vertical distribution can be estimated using this method.&amp;#160;&lt;/p&gt;&lt;p&gt;The intersections of the different lines of sight define segments along the slant columns for which the mass concentrations can be estimated. Knowledge about the vertical profiles for a chosen trace gas can be used to correct the retrieved trace gas concentration to specific altitudes above ground. Such corrections are also required since the three instruments were set up at different heights above ground, at different altitudes relative to sea level and with different elevation angles of the lowest viewing direction. One open issue for the retrieval process is the terrain in Vienna in combination with the prevailing wind condition that impacts the horizontal and vertical trace gas distribution and make the retrieval challenging.&amp;#160;&lt;/p&gt;


2012 ◽  
Vol 5 (5) ◽  
pp. 7243-7292 ◽  
Author(s):  
S. Baidar ◽  
H. Oetjen ◽  
S. Coburn ◽  
B. Dix ◽  
I. Ortega ◽  
...  

Abstract. The University of Colorado Airborne Multi Axis Differential Optical Absorption Spectroscopy (CU AMAX-DOAS) instrument uses solar stray light remote sensing to detect and quantify multiple trace gases, including nitrogen dioxide (NO2), glyoxal (CHOCHO), formaldehyde (HCHO), water vapor (H2O), nitrous acid (HONO), iodine monoxide (IO), bromine monoxide (BrO), and oxygen dimers (O4) at multiple wavelengths (360 nm, 477 nm, 577 nm and 632 nm) simultaneously, and sensitively in the open atmosphere. The instrument is unique, in that it presents the first systematic implementation of MAX-DOAS on research aircraft, i.e. (1) includes measurements of solar stray light photons from nadir, zenith, and multiple elevation angles forward and below the plane by the same spectrometer/detector system, and (2) features a motion compensation system that decouples the telescope field of view (FOV) from aircraft movements in real-time (< 0.35° accuracy). Sets of solar stray light spectra collected from nadir to zenith scans provide some vertical profile information within 2 km above and below the aircraft altitude, and the vertical column density (VCD) below the aircraft is measured in nadir view. Maximum information about vertical profiles is derived simultaneously for trace gas concentrations and aerosol extinction coefficients over similar spatial scales and with a vertical resolution of typically 250 m during aircraft ascent/descent. The instrument is described, and data from flights over California during the CalNex and CARES air quality field campaigns is presented. Horizontal distributions of NO2 VCDs (below the aircraft) maps are sampled with typically 1 km resolution, and show good agreement with two ground based CU MAX-DOAS instruments (slope 0.95 ± 0.09, R2 = 0.86). As a case study vertical profiles of NO2, CHOCHO, HCHO, and H2O mixing ratios and aerosol extinction coefficients, ε, at 477nm calculated from O4 measurements from a low approach at Brackett airfield inside the South Coast Air Basin (SCAB) are presented. These profiles contain ~ 12 degrees of freedom (DOF) over a 3.5 km altitude range, independent of signal-to-noise at which the trace gas is detected. The boundary layer NO2 concentration, and the integral aerosol extinction over height (aerosol optical depth, AOD) agrees well with nearby ground-based in-situ NO2 measurement, and AERONET station. The detection limits of NO2, CHOCHO, HCHO, ε360, ε477 from 30 s integration time spectra recorded forward of the plane are 5 ppt, 3 ppt, 100 ppt, 0.004 km−1, 0.002 km−1 in the free troposphere (FT), and 30 ppt, 16 ppt, 540 ppt, 0.012 km−1, 0.006 km−1 inside the boundary layer (BL), respectively. Mobile column observations of trace gases and aerosols are complimentary to in-situ observations, and help bridge the spatial scales probed by ground-based observations, satellites, and predicted by atmospheric models.


2016 ◽  
Vol 16 (6) ◽  
pp. 4135-4146 ◽  
Author(s):  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
Nicola Pirrone ◽  
Johannes Bieser ◽  
Jan Bödewadt ◽  
...  

Abstract. The knowledge of the vertical distribution of atmospheric mercury (Hg) plays an important role in determining the transport and cycling of mercury. However, measurements of the vertical distribution are rare, because airborne measurements are expensive and labour intensive. Consequently, only a few vertical Hg profile measurements have been reported since the 1970s. Besides the Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) observations, the latest vertical profile over Europe was measured in 1996. Within the Global Mercury Observation System (GMOS) project, four vertical profiles were taken on board research aircraft (CASA-212) in August 2013 in background air over different locations in Slovenia and Germany. Each vertical profile consists of at least seven 5 min horizontal flight sections from 500 m above ground to 3000 m a.s.l. Gaseous elemental mercury (GEM) and total gaseous mercury (TGM) were measured with Tekran 2537X and Tekran 2537B analysers. In addition to the mercury measurements, SO2, CO, O3, NO, and NO2, basic meteorological parameters (pressure, temperature, relative humidity) have been measured. Additional ground-based mercury measurements at the GMOS master site in Waldhof, Germany and measurements onboard the CARIBIC passenger aircraft were used to extend the profile to the ground and upper troposphere respectively. No vertical gradient was found inside the well-mixed boundary layer (variation of less than 0.1 ng m−3) at different sites, with GEM varying from location to location between 1.4 and 1.6 ng m−3 (standard temperature and pressure, STP: T  =  273.15 K, p  =  1013.25 hPa). At all locations GEM dropped to 1.3 ng m−3 (STP) when entering the free troposphere and remained constant at higher altitudes. The combination of the vertical profile, measured on 21 August 2013 over Leipzig, Germany, with the CARIBIC measurements during ascent and descent to Frankfurt Airport, Germany, taken at approximately the same time, provide a unique central European vertical profile from inside the boundary layer (550 m a.s.l) to the upper free troposphere (10 500 m a.s.l.) and show a fairly constant free-tropospheric TGM concentration of 1.3 ng m−3 (STP).


2004 ◽  
Vol 4 (2) ◽  
pp. 351-359 ◽  
Author(s):  
G. P. Gobbi ◽  
F. Barnaba ◽  
L. Ammannato

Abstract. A set of 813 lidar profiles of tropospheric aerosol and cirrus clouds extinction and depolarization observed in 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 532nm. Seasonal analysis shows the planetary boundary layer (PBL) aerosols to be confined below 2km in winter and 3.8km in summer, with relevant OT shifting from 0.08 to 0.16, respectively. Cirrus clouds maximise 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 OT0.03. 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.


2011 ◽  
Vol 11 (2) ◽  
pp. 503-518 ◽  
Author(s):  
A. K. Baker ◽  
T. J. Schuck ◽  
F. Slemr ◽  
P. van Velthoven ◽  
A. Zahn ◽  
...  

Abstract. Between April and December 2008 the CARIBIC commercial aircraft conducted monthly measurement flights between Frankfurt, Germany and Chennai, India. These flights covered the period of the Asian summer monsoon (June–September), during which enhancements in a number of atmospheric species were observed in the upper troposphere over southwestern Asia. In addition to in situ measurements of trace gases and aerosols, whole air samples were collected during the flights, and these were subsequently analyzed for a suite of trace gases that included a number of C2–C8 non-methane hydrocarbons. Non-methane hydrocarbons are relatively short-lived compounds and the large enhancements in their mixing ratios in the upper troposphere over southwestern Asia during the monsoon, sometimes more than double their spring and fall means, provides qualitative evidence for the influence of convectively uplifted boundary layer air. The particularly large enhancements of the combustion tracers benzene and ethyne, along with the similarity of their ratios with carbon monoxide and emission ratios from the burning of household biofuels, indicate a strong influence of biofuel burning to NMHC emissions in this region. Conversely, the ratios of ethane and propane to carbon monoxide, along with the ratio between i-butane and n-butane, indicate a significant source of these compounds from the use of fossil fuels, and comparison to previous campaigns suggests that this source could be increasing. Photochemical aging patterns of NMHCs showed that the CARIBIC samples were collected in two distinctly different regions of the monsoon circulation: a southern region where air masses had been recently influenced by low level contact and a northern region, where air parcels had spent substantial time in transit in the upper troposphere before being probed. Estimates of age using ratios of individual NMHCs have ranges of 3–6 days in the south and 9–12 days in the north.


2015 ◽  
Vol 8 (6) ◽  
pp. 2473-2489 ◽  
Author(s):  
J. Ungermann ◽  
J. Blank ◽  
M. Dick ◽  
A. Ebersoldt ◽  
F. Friedl-Vallon ◽  
...  

Abstract. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 High Altitude LOng Range (HALO) research aircraft during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra that are spectrally sampled every 0.625 cm−1. A total of 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line of sight. Simultaneous in situ observations by the Basic Halo Measurement and Sensor System (BAHAMAS), the Fast In-situ Stratospheric Hygrometer (FISH), an ozone detector named Fairo, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in situ trace gas data, and discrepancies can to a large extent be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.


2017 ◽  
Author(s):  
Lisa K. Behrens ◽  
Andreas Hilboll ◽  
Andreas Richter ◽  
Enno Peters ◽  
Henk Eskes ◽  
...  

Abstract. In this study, we present a novel NO2 DOAS retrieval in the ultraviolet (UV) spectral range for satellite observations from the Global Ozone Monitoring Instrument 2 on board EUMETSAT’s MetOp-A (GOME-2A) satellite. We compare the results to those from an established NO2 retrieval in the visible (vis) spectral range from the same instrument and infer information about the NO2 vertical profile shape in the troposphere. As expected, radiative transfer calculations for satellite geometries show that the sensitivity close to the ground is higher in the vis than in the UV spectral range. Consequently, NO2 slant column densities (SCDs) in the vis are usually higher than in the UV, if the NO2 is close to the surface. Therefore, these differences in NO2 SCDs between the two spectral ranges contain information on the vertical distribution of NO2 in the troposphere. We combine these results with radiative transfer calculations and simulated NO2 fields from the TM5 chemistry transport model to evaluate the simulated NO2 vertical distribution. We investigate regions representative for both anthropogenic and biomass burning NO2 pollution. Anthropogenic air pollution is mostly located in the boundary layer close to the surface, which is reflected by the large differences between UV and vis SCDs of ~ 60 %. Biomass burning NO2 in contrast is often uplifted into elevated layers above the boundary layer. This is best seen in tropical Africa south of the equator, where the biomass burning NO2 is well observed in the UV, and the difference between the two spectral ranges is only ~ 36 %. In tropical Africa north of the equator, however, the biomass burning NO2 is located closer to the ground, reducing its visibility. While not enabling a full retrieval of the vertical NO2 profile shape in the troposphere, our results can help to constrain the vertical profile of NO2 in the lower troposphere and, when analyzed together with simulated NO2 fields, can help interpret the model output.


2021 ◽  
Author(s):  
Zoe Davis ◽  
Debora Griffin ◽  
Yue Jia ◽  
Susann Tegtmeier ◽  
Mallory Loria ◽  
...  

&lt;p&gt;A recent method uses satellite measurements to estimate lifetimes and emissions of trace-gases from point sources (Fioletov et al., 2015). Emissions are retrieved by fitting measured vertical column densities (VCDs) of trace-gases to a three-dimensional function of the wind speed and spatial coordinates. In this study, a plume model generated &amp;#8220;synthetic&amp;#8221; satellite observations of prescribed emissions to examine the accuracy of the retrieved emissions. The Lagrangian transport and dispersion model FLEXPART (v10.0) modelled the plume from a point source over a multi-day simulation period at a resolution much higher than current satellite observations. The study aims to determine how various assumptions in the retrieval method and local meteorological conditions affect the accuracy and precision of emissions. These assumptions include that the use of a vertical mean of the wind profile is representative of the transport of the plume&amp;#8217;s vertical column. In the retrieval method, the VCDs&amp;#8217; pixel locations are rotated around the source based on wind direction so that all plumes have a common wind direction. Retrievals using a vertical mean wind for rotation will be compared to retrievals using VCDs determined by rotating each altitude of the vertical profile of trace-gas using the respective wind-direction. The impact of local meteorological factors on the two approaches will be presented, including atmospheric mixing, vertical wind shear, and boundary layer height. The study aims to suggest which altitude(s) of the vertical profile of winds results in the most accurate retrievals given the local meteorological conditions. The study will also examine the impact on retrieval accuracy due to satellite resolution, trace-gas lifetime, plume source altitude, number of overpasses, and random and systematic errors. Sensitivity studies repeated using a second, &amp;#8220;line-density&amp;#8221;, retrieval method will also be presented (Adams et al., 2019; Goldberg et al., 2019).&lt;/p&gt;


2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  

&lt;p&gt;Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt;, CO, and O&lt;sub&gt;3&lt;/sub&gt; conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM&lt;sub&gt;2.5 &lt;/sub&gt;chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt; and O&lt;sub&gt;3&lt;/sub&gt; mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O&lt;sub&gt;3&lt;/sub&gt; levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM&lt;sub&gt;2.5 &lt;/sub&gt;composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&lt;strong&gt;REFERENCES&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172&amp;#8211;1187 (2019).&lt;/p&gt;&lt;p&gt;[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.&lt;/p&gt;


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