scholarly journals Investigation of NO<sub>2</sub> vertical distribution using two DOAS retrievals for GOME-2A measurements in the UV and vis spectral range

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.

2018 ◽  
Vol 11 (5) ◽  
pp. 2769-2795 ◽  
Author(s):  
Lisa K. Behrens ◽  
Andreas Hilboll ◽  
Andreas Richter ◽  
Enno Peters ◽  
Henk Eskes ◽  
...  

Abstract. In this study, we present a novel nitrogen dioxide (NO2) differential optical absorption spectroscopy (DOAS) retrieval in the ultraviolet (UV) spectral range for 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 investigate how differences between the two are linked to 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-MP chemistry transport model to evaluate the simulated NO2 vertical distribution.We investigate regions representative of 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 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 SCD 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 in the UV.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 analysed together with simulated NO2 fields, can help to better interpret the model output.


2020 ◽  
Author(s):  
Mo Wang ◽  
Baiqing Xu ◽  
Song Yang ◽  
Jing Gao ◽  
Taihua Zhang ◽  
...  

&lt;p&gt;Black carbon (BC) can change the energy budget of the earth system by strongly absorbing solar radiation: both suspended in the atmosphere, incorporated into cloud droplets, or deposited onto high-albedo surfaces. BC&amp;#8217;s direct radiative forcing is highly dependent on its vertical distribution. However, due to large variabilities and the small number of vertical profile measurements, there is still large uncertainty in this forcing value. Moreover, the vertical profile of BC and its relative elevation to clouds determine BC&amp;#8217;s lifetime in the atmosphere and its transport and removal processes. In November-December 2017, a series of tethered balloon flights was launched at the Southeast Tibet Observation and Research Station for the Alpine Environment of the Chinese Academy of Sciences. A cylindrical balloon with a diameter of 7.9 m and maximum volume of 1250 m&lt;sup&gt;3&lt;/sup&gt; was used. A 7-channel Aethalometer was installed in the gondola attached to the balloon, together with several other instruments including a GPS for altitude, and sensors for temperature and relative humidity. The airborne Aethalometer measured BC mass concentration (ng/m&lt;sup&gt;3&lt;/sup&gt;) on a on a 1-second timebase at 7 wavelengths ranging from 370 nm to 950 nm. Meanwhile, another Aethalometer was used to monitor BC mass concentration near the surface, at a height of about 10 m above the ground. From the tethered balloon flights, we derived three profiles designated as &amp;#8216;F1&amp;#8217;, &amp;#8216;F3-ASC&amp;#8217;, and &amp;#8216;F3-DES&amp;#8217;. The maximum height for the F1 flight was 500 m a.g.l., namely 3800 m a.s.l.; while the maximum height for the F3 flight was 1950 m a.g.l., namely 5250 m a.s.l. Based on the potential temperature and relative humidity data, the profiles were divided into three layers: the stable boundary layer (SBL), the residual layer (RL), and the free troposphere (FT). The vertical distribution of BC shows a prominent peak within the SBL. The mean BC concentration in SBL (1000&amp;#177;750 ng/m&lt;sup&gt;3&lt;/sup&gt;) was one order of magnitude higher than in RL and FT, which were 140&amp;#177;40 ng/m&lt;sup&gt;3&lt;/sup&gt; and 120&amp;#177;40 ng/m&lt;sup&gt;3&lt;/sup&gt;, respectively. The BC concentration measured in the present study in FT over the southeastern Tibetan Plateau is comparable to measurements in Arctic regions, but lower than values in South Asia. Analysis of the wavelength dependence of the data yields an estimate of the biomass burning contribution. This showed a maximum value in SBL of 44&amp;#177;37%, and was 16&amp;#177;6% in RL and 13&amp;#177;5% in FT. Analysis of 24-hour isentropic back trajectories showed that BC in SBL and RL was dominated by local sources, while in the FT, BC is mainly influenced by mid- to long-distant transport by the westerlies. In addition, analysis of the variations of BC concentration and biomass burning contribution on a high-resolution time scale showed that BC concentrations and the nature of their sources are largely influenced by air mass origins and transport. To our knowledge, this is the first ever in situ measurement of BC concentration over the Tibetan Plateau in the atmospheric boundary layer and free troposphere up to 5000 m a.s.l.&lt;/p&gt;


2015 ◽  
Vol 8 (4) ◽  
pp. 1657-1671 ◽  
Author(s):  
L. Haszpra ◽  
Z. Barcza ◽  
T. Haszpra ◽  
Zs. Pátkai ◽  
K. J. Davis

Abstract. Planetary boundary layer (PBL) CO2 mole fraction data are needed by transport models and carbon budget models as both input and reference for validation. The height of in situ CO2 mole fraction measurements is usually different from that of the model levels where the data are needed; data from short towers, in particular, are difficult to utilize in atmospheric models that do not simulate the surface layer well. Tall-tower CO2 mole fraction measurements observed at heights ranging from 10 to 115 m above ground level at a rural site in Hungary and regular airborne vertical mole fraction profile measurements (136 vertical profiles) above the tower allowed us to estimate how well a tower of a given height could estimate the CO2 mole fraction above the tower in the PBL. The statistical evaluation of the height-dependent bias between the real PBL CO2 mole fraction profile (measured by the aircraft) and the measurement at a given elevation above the ground was performed separately for the summer and winter half years to take into account the different dynamics of the lower troposphere and the different surface CO2 flux in the different seasons. The paper presents (1) how accurately the vertical distribution of CO2 in the PBL can be estimated from the measurements on the top of a tower of height H; (2) how tall of a tower would be needed for the satisfaction of different requirements on the accuracy of the estimation of the CO2 vertical distribution; (3) how accurate of a CO2 vertical distribution estimation can be expected from the existing towers; and (4) how much improvement can be achieved in the accuracy of the estimation of CO2 vertical distribution by applying the virtual tall-tower concept.


2021 ◽  
Vol 2 (1-4) ◽  
Author(s):  
Gabriele Fasano ◽  
Henri Diémoz ◽  
Ilias Fountoulakis ◽  
Claudio Cassardo ◽  
Rei Kudo ◽  
...  

AbstractAtmospheric aerosols play an important role in Earth’s radiative balance, directly interacting with solar radiation or influencing cloud formation and properties. In order to assess their radiative impact, it is necessary to accurately characterise their optical properties, together with their spatial and vertical distribution. The information on aerosol vertical profile is often scarce, in particular in mountainous, complex terrains. This study presents the first attempt to evaluate the shortwave aerosol direct radiative effect in the Aosta Valley, a mountainous region in the Northwestern Italian Alps. Ground-based, remote sensing instruments (a sky radiometer and an Automated Lidar Ceilometer) are used to derive two descriptions of the aerosol properties and vertical distribution: a first, more accurate description, which includes the whole spectral information about the aerosol extinction coefficient, phase function and single scattering albedo; a second, more approximate one, which only relies on spectrally constant values of aerosol single scattering albedo and asymmetry factor. This information is used as input for radiative transfer simulations, which allow to estimate, in cloudless conditions, the shortwave aerosol direct radiative effect and the vertical profile of the instantaneous heating rates in the lower layers of the atmosphere. The simulations obtained with the two descriptions do not differ significantly: they highlight a strong surface dimming (between − 25 and − 50 W m− 2) due to the presence of aerosol, with a considerable radiative absorption inside the atmospheric column (around + 30 W m− 2), and an overall small cooling effect for the Earth-atmospheric system. The absorption of solar radiation within the atmospheric column due to aerosol leads to instantaneous heating rates up to 1.5 K day− 1 in the tropospheric layers below 6 km a.s.l. These results show that, in some conditions, the shortwave aerosol direct radiative effect can be considerable even in this Alpine environment, usually considered as relatively pristine (yearly average PM10 concentration about 20 μg m− 3).


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.


2021 ◽  
Vol 21 (6) ◽  
pp. 4979-5014
Author(s):  
Ananth Ranjithkumar ◽  
Hamish Gordon ◽  
Christina Williamson ◽  
Andrew Rollins ◽  
Kirsty Pringle ◽  
...  

Abstract. Understanding the vertical distribution of aerosol helps to reduce the uncertainty in the aerosol life cycle and therefore in the estimation of the direct and indirect aerosol forcing. To improve our understanding, we use measurements from four deployments of the Atmospheric Tomography (ATom) field campaign (ATom1–4) which systematically sampled aerosol and trace gases over the Pacific and Atlantic oceans with near pole-to-pole coverage. We evaluate the UK Earth System Model (UKESM1) against ATom observations in terms of joint biases in the vertical profile of three variables related to new particle formation: total particle number concentration (NTotal), sulfur dioxide (SO2) mixing ratio and the condensation sink. The NTotal, SO2 and condensation sink are interdependent quantities and have a controlling influence on the vertical profile of each other; therefore, analysing them simultaneously helps to avoid getting the right answer for the wrong reasons. The simulated condensation sink in the baseline model is within a factor of 2 of observations, but the NTotal and SO2 show much larger biases mainly in the tropics and high latitudes. We performed a series of model sensitivity tests to identify atmospheric processes that have the strongest influence on overall model performance. The perturbations take the form of global scaling factors or improvements to the representation of atmospheric processes in the model, for example by adding a new boundary layer nucleation scheme. In the boundary layer (below 1 km altitude) and lower troposphere (1–4 km), inclusion of a boundary layer nucleation scheme (Metzger et al., 2010) is critical to obtaining better agreement with observations. However, in the mid (4–8 km) and upper troposphere (> 8 km), sub-3 nm particle growth, pH of cloud droplets, dimethyl sulfide (DMS) emissions, upper-tropospheric nucleation rate, SO2 gas-scavenging rate and cloud erosion rate play a more dominant role. We find that perturbations to boundary layer nucleation, sub-3 nm growth, cloud droplet pH and DMS emissions reduce the boundary layer and upper tropospheric model bias simultaneously. In a combined simulation with all four perturbations, the SO2 and condensation sink profiles are in much better agreement with observations, but the NTotal profile still shows large deviations, which suggests a possible structural issue with how nucleation or gas/particle transport or aerosol scavenging is handled in the model. These perturbations are well-motivated in that they improve the physical basis of the model and are suitable for implementation in future versions of UKESM.


2020 ◽  
Author(s):  
Ananth Ranjithkumar ◽  
Hamish Gordon ◽  
Christina Williamson ◽  
Andrew Rollins ◽  
Kirsty J. Pringle ◽  
...  

Abstract. Understanding the vertical distribution of aerosol helps to reduce the uncertainty in the aerosol lifecycle and therefore in the estimation of the direct and indirect aerosol forcing. To improve our understanding, we use measurements from four deployments of the Atmospheric Tomography (ATom) field campaign (ATom1-4) which systematically sampled data over the Pacific and Atlantic Oceans with near pole-to-pole coverage. We evaluate the UK Earth system model (UKESM1) against ATom observations in terms of joint biases in the vertical profile of three variables related to new particle formation: total particle number concentration (NTotal), sulphur dioxide (SO2) mixing ratio and the condensation sink. The NTotal, SO2 and condensation sink are interdependent quantities and have a controlling influence on the vertical profile of each other. Improving only one of these quantities in comparison with observations can lead to a misleading impression that overall model performance has improved. Analysing NTotal, SO2 and condensation sink simultaneously helps reduce the probability of getting the right answer for the wrong reasons. The model's condensation sink is within a factor of 2 of observations, but the NTotal and SO2 shows larger biases mainly in the tropics and high latitudes. Algorithmic improvements to the model and perturbations to key atmospheric processes help reduce tropospheric model biases consistently. We performed a series of model sensitivity tests to identify atmospheric processes that have the strongest influence on overall model performance (NTotal, SO2 and condensation sink simultaneously). In the boundary layer (which we define in this study as below 1 km altitude) and lower troposphere (1–4 km) inclusion of a boundary layer nucleation scheme (Metzger et al., 2010), which is switched off in the default version of UKESM, is critical to obtaining better agreement with observations. However, in the mid (4–8 km) and upper troposphere (> 8 km), sub-3 nm particle growth, pH of cloud droplets, DMS emissions, upper tropospheric nucleation rate, SO2 gas scavenging rate and cloud erosion rate are found to play a more dominant role. Analysing the data with altitude, we find that perturbations to boundary layer nucleation, sub 3 nm growth, cloud droplet pH and DMS emissions reduces the boundary layer and upper tropospheric model bias. We performed a combined simulation with all 4 perturbations included and found that the model's NTotal, SO2 and condensation sink biases were reduced in most cases (up to a 50 % reduction) in both the boundary layer and upper troposphere simultaneously. These perturbations are well-motivated in that they improve the physical basis of the model and are suitable for implementation in future versions of UKESM.


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.


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).


2014 ◽  
Vol 7 (12) ◽  
pp. 12249-12282 ◽  
Author(s):  
L. Haszpra ◽  
Z. Barcza ◽  
T. Haszpra ◽  
Z. Pátkai ◽  
K. J. Davis

Abstract. Planetary boundary layer (PBL) CO2 mole fraction data are needed by transport models and carbon budget models as both input and reference for validation. The height of in situ CO2 mole fraction measurements is usually different from that of the model levels where the data are needed; data from short towers, in particular, are difficult to utilize in atmospheric models that do not simulate the surface layer well. Tall tower CO2 mole fraction measurements observed at heights ranging from 10 to 115 m a.g.l. at a rural site in Hungary and regular airborne vertical mole fraction profile measurements (136 vertical profiles) above the tower allowed us to estimate how well a tower of a given height could estimate the CO2 mole fraction above the tower in the PBL. The statistical evaluation of the height-dependent bias between the real PBL CO2 mole fraction profile (measured by the aircraft) and the measurement at a given elevation above the ground was performed separately for the summer and winter half years to take into account the different dynamics of the lower troposphere and the different surface CO2 flux in the different seasons. The paper presents: (1) how accurately the vertical distribution of CO2 in the PBL can be estimated from the measurements on the top of a tower of height H, (2) how tall a tower would be needed for the satisfaction of different requirements on the accuracy of the estimation of the CO2 vertical distribution, (3) how accurate a CO2 vertical distribution estimation can be expected from the existing towers; and (4) how much improvement can be achieved in the accuracy of the estimation of CO2 vertical distribution applying the virtual tall tower concept.


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