Vertical Profiles of Long Lived Trace Gases

Author(s):  
Melanie Müller ◽  
Martin Strunk ◽  
Andreas Engel ◽  
Ulrich Schmidt
1989 ◽  
Vol 94 (D12) ◽  
pp. 14879-14892 ◽  
Author(s):  
Kenneth E. Pickering ◽  
Russell R. Dickerson ◽  
Winston T. Luke ◽  
Linda J. Nunnermacker

2018 ◽  
Author(s):  
Yang Wang ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Sebastian Böhnke ◽  
Isabelle De Smedt ◽  
...  

Abstract. A Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18° N, 114.36° E) in the suburban area of Xingtai (one of the most polluted cities in China) during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ~ 3.5 ppb. Underestimates of MAX-DOAS results compared to in situ measurements of NO2 (~ 60 %), SO2 (~ 20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2, SO2 are reasonably consistent with those measured by a collocated Raman Lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO, and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ~ 1.4 km) than did NO2, SO2, and HONO (with 75 % integrated column below ~ 0.5 km) under polluted condition. Lifted layers were systematically observed for all species, (except HONO), indicating accumulation, secondary formation, or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2, SO2, and HONO, but around noon for aerosols, HCHO, and CHOCHO, mainly dominated by photochemistry, characteristic upslope/downslope circulation and PBL dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution from the southern areas such as industrialized Wuan. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases, and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations of HCHO, CHOCHO and aerosols.


2011 ◽  
Vol 11 (9) ◽  
pp. 4491-4503 ◽  
Author(s):  
J. Worden ◽  
D. Noone ◽  
J. Galewsky ◽  
A. Bailey ◽  
K. Bowman ◽  
...  

Abstract. The Aura satellite Tropospheric Emission Spectrometer (TES) instrument is capable of measuring the HDO/H2O ratio in the lower troposphere using thermal infrared radiances between 1200 and 1350 cm−1. However, direct validation of these measurements is challenging due to a lack of in situ measured vertical profiles of the HDO/H2O ratio that are spatially and temporally co-located with the TES observations. From 11 October through 5 November 2008, we undertook a campaign to measure HDO and H2O at the Mauna Loa observatory in Hawaii for comparison with TES observations. The Mauna Loa observatory is situated at 3.1 km above sea level or approximately 680 hPa, which is approximately the altitude where the TES HDO/H2O observations show the most sensitivity. Another advantage of comparing in situ data from this site to estimates derived from thermal IR radiances is that the volcanic rock is heated by sunlight during the day, thus providing significant thermal contrast between the surface and atmosphere; this thermal contrast increases the sensitivity to near surface estimates of tropospheric trace gases. The objective of this inter-comparison is to better characterize a bias in the TES HDO data, which had been previously estimated to be approximately 5 % too high for a column integrated value between 850 hPa and 500 hPa. We estimate that the TES HDO profiles should be corrected downwards by approximately 4.8 % and 6.3 % for Versions 3 and 4 of the data respectively. These corrections must account for the vertical sensitivity of the TES HDO estimates. We estimate that the precision of this bias correction is approximately 1.9 %. The accuracy is driven by the corrections applied to the in situ HDO and H2O measurements using flask data taken during the inter-comparison campaign and is estimated to be less than 1 %. Future comparisons of TES data to accurate vertical profiles of in situ measurements are needed to refine this bias estimate.


2013 ◽  
Vol 6 (3) ◽  
pp. 719-739 ◽  
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 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 (absorption bands at 360, 477, 577, 632 nm) simultaneously in the open atmosphere. The instrument is unique as it (1) features a motion compensation system that decouples the telescope field of view from aircraft movements in real time (<0.35° accuracy), and (2) 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. 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 (California Research at the Nexus of Air Quality and Climate Change) and CARES (Carbonaceous Aerosols and Radiative Effects Study) air quality field campaigns is presented. Horizontal distributions of NO2 VCD (below the aircraft) maps are sampled with typically 1 km resolution, and show good agreement with two ground-based MAX-DOAS instruments (slope = 0.95 ± 0.09, R2 = 0.86). As a case study vertical profiles of NO2, CHOCHO, HCHO, and H2O concentrations and aerosol extinction coefficients, ε, at 477 nm 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, an independent information approximately every 250 m. 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, H2O442, &amp;varepsilon;360, &amp;varepsilon;477 for 30 s integration time spectra recorded forward of the plane are 5 ppt, 3 ppt, 100 ppt, 42 ppm, 0.004 km−1, 0.002 km−1 in the free troposphere (FT), and 30 ppt, 16 ppt, 540 ppt, 252 ppm, 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 that are probed by satellites and ground-based observations, and predicted by atmospheric models.


2013 ◽  
Vol 13 (5) ◽  
pp. 12287-12336 ◽  
Author(s):  
M. Michael ◽  
A. Yadav ◽  
S. N. Tripathi ◽  
V. P. Kanawade ◽  
A. Gaur ◽  
...  

Abstract. The "online" meteorological and chemical transport Weather Research and Forecasting/Chemistry (WRF-Chem) model has been implemented over the Indian subcontinent for three consecutive summers in 2008, 2009 and 2010 to study the aerosol properties over the domain. The initial and boundary conditions are obtained from NCAR reanalysis data. The emission rates of sulfur dioxide, black carbon, organic carbon and PM2.5, which are developed over India at a grid resolution of 0.25° × 0.25° have been used in the present study. The remaining emissions are obtained from global inventories (RETRO and EDGAR). The model simulated the meteorological parameters, trace gases and particulate matter. Predicted mixing ratios of trace gases (Ozone, carbon monoxide and sulfur dioxide) are compared with ground based observations over Kanpur. Simulated aerosol optical depth are compared with those observed at nine Aerosol Robotic Network stations (AERONET). The simulations show that the aerosol optical depth of the less polluted regions is better simulated compared to that of the locations where the aerosol loading is very high. The vertical profiles of extinction coefficient observed at Kanpur Micropulse Lidar Network (MPLNET) station is in agreement with the simulated values for altitudes greater than 1.5 km and qualitatively simulate the elevated layers of aerosols. The simulated mass concentration of black carbon shows very good correlation with observations, due to the better local emission inventory used. The vertical profiles of black carbon at various locations have also been compared with observations from aircraft campaign held during pre-monsoon period of 2008 and 2009 resulting in good agreement. This study shows that WRF-Chem model captures many important features of the observations and therefore can be used for understanding and predicting regional atmospheric composition over Indian subcontinent.


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;


2014 ◽  
Vol 7 (1) ◽  
pp. 431-482 ◽  
Author(s):  
M. Michael ◽  
A. Yadav ◽  
S. N. Tripathi ◽  
V. P. Kanawade ◽  
A. Gaur ◽  
...  

Abstract. The "online" meteorological and chemical transport Weather Research and Forecasting/Chemistry (WRF-Chem) model has been implemented over the Indian subcontinent for three consecutive summers in 2008, 2009 and 2010 to study the aerosol properties over the domain. The model simulated the meteorological parameters, trace gases and particulate matter. Predicted mixing ratios of trace gases (Ozone, carbon monoxide and sulfur dioxide) are compared with ground based observations over Kanpur. Simulated aerosol optical depth are compared with those observed at nine Aerosol Robotic Network stations (AERONET). The simulations show that the aerosol optical depth of the less polluted regions is better simulated compared to that of the locations where the aerosol loading is very high. The vertical profiles of extinction coefficient observed at the Kanpur Micropulse Lidar Network (MPLNET) station is underpredicted by the model by 10 to 50% for altitudes greater than 1.5 km and qualitatively simulate the elevated layers of aerosols. The simulated mass concentration of black carbon shows a correlation coefficient of 0.4 with observations. Vertical profiles of black carbon at various locations have also been compared with observations from an aircraft campaign held during pre-monsoon period of 2008 and 2009. This study shows that WRF-Chem model captures many important features of the observed atmospheric composition during the pre-monsoon season in India.


2015 ◽  
Vol 15 (6) ◽  
pp. 8283-8328 ◽  
Author(s):  
C. Di Biagio ◽  
L. Doppler ◽  
C. Gaimoz ◽  
N. Grand ◽  
G. Ancellet ◽  
...  

Abstract. In this study we present airborne observations of aerosol and trace gases obtained over the sea in the Western Mediterranean Basin during the TRAQA (TRansport and Air QuAlity) and SAFMED (Secondary Aerosol Formation in the MEDiterranean) campaigns in summers 2012 and 2013. A total of 23 vertical profiles were measured up to 5000 m a.s.l. over an extended area (40–45° N latitude and 2° W–12° E longitude) including the Gulf of Genoa, Southern France, the Gulf of Lion, and the Spanish coast. TRAQA and SAFMED successfully measured a wide range of meteorological conditions which favoured the pollution export from different sources located around the basin. Also, several events of dust outflows were measured during the campaigns. Observations from the present study indicate that continental pollution largely affects the Western Mediterranean both close to coastal regions and in the open sea as far as ~250 km from the coastline. Aerosol layers not specifically linked with Saharan dust outflows are distributed ubiquitously which indicates quite elevated levels of background pollution throughout the Western Basin. The measured aerosol scattering coefficient varies between ~20 and 120 M m−1, while carbon monoxide (CO) and ozone (O3) mixing ratios are in the range of 60–170 and 30–85 ppbv, respectively. Pollution reaches 3000–4000 m in altitude and presents a very complex and highly stratified structure characterized by fresh and aged layers both in the boundary layer and in the free troposphere. Within pollution plumes the measured particle concentration in the Aitken (0.004–0.1 μm) and accumulation (0.1–1.0 μm) modes is between $\\sim 100$ and 5000–6000 s cm−3 (standard cm−3), which is comparable to the aerosol concentration measured in continental urban areas. Additionally, our measurements indicate the presence of highly concentrated Aitken layers (10 000–15 000 s cm−3) observed both close to the surface and in the free troposphere, possibly linked to the influence of new particle formation (NPF) episodes over the basin.


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.


1998 ◽  
Vol 103 (D17) ◽  
pp. 22015-22037 ◽  
Author(s):  
G. A. Isaac ◽  
C. M. Banic ◽  
W. R. Leaitch ◽  
K. G. Anlauf ◽  
M. D. Couture ◽  
...  

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