scholarly journals Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone

2007 ◽  
Vol 7 (3) ◽  
pp. 815-838 ◽  
Author(s):  
B. Sauvage ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
X. Liu ◽  
K. Chance ◽  
...  

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS satellite instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning NOx and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flashes improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 6±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger than the bottom-up inventory by a factor of 2 for HCHO and alkenes, and by a factor of 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv, reflecting enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols increases O3 by 5 ppbv in biomass burning regions, reducing a model bias versus MOZAIC aircraft measurements.

2006 ◽  
Vol 6 (6) ◽  
pp. 11465-11520 ◽  
Author(s):  
B. Sauvage ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
X. Liu ◽  
K. Chance ◽  
...  

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.


2020 ◽  
Vol 12 (22) ◽  
pp. 3823
Author(s):  
Katherine T. Junghenn Noyes ◽  
Ralph A. Kahn ◽  
James A. Limbacher ◽  
Zhanqing Li ◽  
Marta A. Fenn ◽  
...  

Although the characteristics of biomass burning events and the ambient ecosystem determine emitted smoke composition, the conditions that modulate the partitioning of black carbon (BC) and brown carbon (BrC) formation are not well understood, nor are the spatial or temporal frequency of factors driving smoke particle evolution, such as hydration, coagulation, and oxidation, all of which impact smoke radiative forcing. In situ data from surface observation sites and aircraft field campaigns offer deep insight into the optical, chemical, and microphysical traits of biomass burning (BB) smoke aerosols, such as single scattering albedo (SSA) and size distribution, but cannot by themselves provide robust statistical characterization of both emitted and evolved particles. Data from the NASA Earth Observing System’s Multi-Angle Imaging SpectroRadiometer (MISR) instrument can provide at least a partial picture of BB particle properties and their evolution downwind, once properly validated. Here we use in situ data from the joint NOAA/NASA 2019 Fire Influence on Regional to Global Environments Experiment-Air Quality (FIREX-AQ) field campaign to assess the strengths and limitations of MISR-derived constraints on particle size, shape, light-absorption, and its spectral slope, as well as plume height and associated wind vectors. Based on the satellite observations, we also offer inferences about aging mechanisms effecting downwind particle evolution, such as gravitational settling, oxidation, secondary particle formation, and the combination of particle aggregation and condensational growth. This work builds upon our previous study, adding confidence to our interpretation of the remote-sensing data based on an expanded suite of in situ measurements for validation. The satellite and in situ measurements offer similar characterizations of particle property evolution as a function of smoke age for the 06 August Williams Flats Fire, and most of the key differences in particle size and absorption can be attributed to differences in sampling and changes in the plume geometry between sampling times. Whereas the aircraft data provide validation for the MISR retrievals, the satellite data offer a spatially continuous mapping of particle properties over the plume, which helps identify trends in particle property downwind evolution that are ambiguous in the sparsely sampled aircraft transects. The MISR data record is more than two decades long, offering future opportunities to study regional wildfire plume behavior statistically, where aircraft data are limited or entirely lacking.


2013 ◽  
Vol 13 (5) ◽  
pp. 2487-2505 ◽  
Author(s):  
S. Groß ◽  
M. Esselborn ◽  
B. Weinzierl ◽  
M. Wirth ◽  
A. Fix ◽  
...  

Abstract. During four aircraft field experiments with the DLR research aircraft Falcon in 1998 (LACE), 2006 (SAMUM-1) and 2008 (SAMUM-2 and EUCAARI), airborne High Spectral Resolution Lidar (HSRL) and in situ measurements of aerosol microphysical and optical properties were performed. Altogether, the properties of six different aerosol types and aerosol mixtures – Saharan mineral dust, Saharan dust mixtures, Canadian biomass burning aerosol, African biomass burning mixture, anthropogenic pollution aerosol, and marine aerosol have been studied. On the basis of this extensive HSRL data set, we present an aerosol classification scheme which is also capable to identify mixtures of different aerosol types. We calculated mixing lines that allowed us to determine the contributing aerosol types. The aerosol classification scheme was supported by backward trajectory analysis and validated with in-situ measurements. Our results demonstrate that the developed aerosol mask is capable to identify complex stratifications with different aerosol types throughout the atmosphere.


2002 ◽  
Vol 107 (D5) ◽  
pp. SOL 47-1-SOL 47-6 ◽  
Author(s):  
A. A. Viggiano ◽  
D. E. Hunton ◽  
Thomas M. Miller ◽  
John O. Ballenthin

2010 ◽  
Vol 3 (3) ◽  
pp. 1359-1421
Author(s):  
R. Hommel ◽  
C. Timmreck ◽  
H. F. Graf

Abstract. In this paper we investigate results from a middle-atmosphere aerosol-climate model which has been developed to study the evolution of stratospheric aerosols. Here we focus on the stratospheric background period and evaluate several key quantities of the global dispersion of stratospheric aerosols and their precursors with observations and other model studies. It is shown that the model fairly well reproduces in situ observations of the aerosol size and number concentrations in the upper troposphere and lower stratosphere (UT/LS). Compared to measurements from the limb-sounding SAGE II satellite instrument, modelled integrated aerosol quantities are more biased the lower the moment of the aerosol population. Both findings are consistent with earlier work analysing the quality of SAGE II retrieved e.g. aerosol surface area densities from the volcanically unperturbed stratosphere (SPARC/ASAP, 2006; Thomason et al., 2008; Wurl et al., 2010). The model suggests that new particles are formed over large areas of the LS, albeit nucleation rates in the upper troposphere are at least one order of magnitude larger than those in the stratosphere. Hence, we suggest that both tropospheric sulphate aerosols and particles formed in situ in the LS are maintaining the stability of the stratospheric aerosol layer also in the absence of direct stratospheric emissions from volcanoes. Particle size distributions are clearly bimodal, except in the upper branches of the stratospheric aerosol layer where aerosols evaporate. Modelled concentrations of condensation nuclei (CN) are lesser than measured in regions of the aerosol layer where aerosol mixing ratios are largest, due to an overpredicted particle growth by coagulation. Transport regimes of tropical stratospheric aerosol have been identified from modelled aerosol mixing ratios and correspond to those deduced from satellite extinction measurements. We found that convective updraft in the Asian Monsoon region significantly contributes to both stratospheric aerosol load and size. The timing of formation and descend of layers of fine mode particles in the winter and spring polar stratosphere (CN layer) are reproduced by the model. Far above the tropopause where nucleation is inhibited due to with height increasing stratospheric temperatures, planetary wave mixing transports significant amounts of fine mode particles from the polar stratosphere to mid-latitudes. In those regions enhanced condensation rates of sulphuric acid vapour counteracts the evaporation of aerosols, hence prolonging the aerosol lifetime in the upper branches of the stratospheric aerosol layer. Measurements of the aerosol precursors SO2 and sulphuric acid vapour are fairly well reproduced by the model throughout the stratosphere.


2009 ◽  
Vol 48 (6) ◽  
pp. 1199-1216 ◽  
Author(s):  
Otto Hyvärinen ◽  
Kalle Eerola ◽  
Niilo Siljamo ◽  
Jarkko Koskinen

Abstract Snow cover has a strong effect on the surface and lower atmosphere in NWP models. Because the progress of in situ observations has stalled, satellite-based snow analyses are becoming increasingly important. Currently, there exist several products that operationally map global or continental snow cover. In this study, satellite-based snow cover analyses from NOAA, NASA, and the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT), and NWP snow analyses from the High-Resolution Limited-Area Model (HIRLAM) and ECMWF, were compared using data from January to June 2006. Because no analyses were independent and since available in situ measurements were already used in the NWP analyses, no independent ground truth was available and only the consistency between analyses could be compared. Snow analyses from NOAA, NASA, and ECMWF were similar, but the analysis from NASA was greatly hampered by clouds. HIRLAM and EUMETSAT deviated most from other analyses. Even though the analysis schemes of HIRLAM and ECMWF were quite similar, the resulting snow analyses were quite dissimilar, because ECMWF used the satellite information of snow cover in the form of NOAA analyses, while HIRLAM used none. The differences are especially prominent in areas around the snow edge where few in situ observations are available. This suggests that NWP snow analyses based only on in situ measurements would greatly benefit from inclusion of satellite-based snow cover information.


2020 ◽  
Author(s):  
Shoma Yamanouchi ◽  
Camille Viatte ◽  
Kimberly Strong ◽  
Dylan B. A. Jones ◽  
Cathy Clerbaux ◽  
...  

<div> <div> <div> <p>Ammonia (NH<sub>3</sub>) is a major source of nitrates in the atmosphere, and a major source of fine particulate matter. As such, there have been increasing efforts to monitor NH<sub>3</sub>. This study examines long-term measurements of NH<sub>3</sub> around Toronto, Canada, derived from three multiscale datasets: 16 years of total column measurements using ground-based Fourier transform infrared (FTIR) spectroscopy, three years of surface in-situ measurements, and ten years of total columns from the Infrared Atmospheric Sounding Interferometer (IASI) sensor onboard the Metop satellites. These datasets were used to quantify NH<sub>3</sub> temporal variabilities (trends, inter-annual, seasonal) over Toronto to assess the observational footprint of the FTIR measurements, and two case studies of pollution events due to transport of biomass burning plumes.</p> <p>All three timeseries showed increasing trends in NH<sub>3</sub> over Toronto: 3.34 ± 0.44 %/year from 2002 to 2018 in the FTIR columns, 8.88 ± 2.49 %/year from 2013 to 2017 in the surface in-situ data, and 8.78 ± 0.84 %/year from 2008 to 2018 in the IASI columns. To assess the observational footprint of the FTIR NH<sub>3</sub> columns, correlations between the datasets were examined. The best correlation between FTIR and IASI was found for coincidence criterion of ≤ 50 km and ≤ 20 minutes, with r = 0.66 and a slope of 0.988 ± 0.058. The FTIR column and in-situ measurements were standardized and correlated, with 24-day averages and monthly averages yielding correlation coefficients of r = 0.72 and r = 0.75, respectively.<br>FTIR and IASI were also compared against the GEOS-Chem model, run at 2° by 2.5° resolution, to assess model performance and investigate correlation of the model output with local column measurements (FTIR) and measurements on a regional scale (IASI). Comparisons on a regional scale (domain spanning from 35°N to 53°N, and 93.75°W to 63.75°W) resulted in r = 0.62, and thus a coefficient of determination, which is indicative of the predictive capacity of the model, of r<sup>2</sup> = 0.38, but comparing a single model grid point against the FTIR resulted in a poorer correlation, with r<sup>2</sup> = 0.26, indicating that a finer spatial resolution is needed to adequately model the variability of NH<sub>3</sub>. This study also examines two case studies of NH<sub>3</sub> enhancements due to biomass burning plumes, in August 2014 and May 2016. In these events, enhancements in both the total columns and surface NH3, were observed.</p> </div> </div> </div>


2006 ◽  
Vol 6 (6) ◽  
pp. 11727-11743 ◽  
Author(s):  
N. A. D. Richards ◽  
Q. Li ◽  
K. W. Bowman ◽  
J. R. Worden ◽  
S. S. Kulawik ◽  
...  

Abstract. We present results from the first assimilation of carbon monoxide (CO) observations from the Tropospheric Emission Spectrometer (TES) into a global three-dimensional (3-D) chemistry and transport model (CTM). A sequential sub-optimal Kalman filter assimilation scheme (Khattatov et al., 2000) was applied to assimilate TES CO profiles during November 2004 into the GEOS-Chem global 3-D CTM. The assimilation results were compared with MOPITT and MOZAIC observations. The assimilation significantly improves model simulation of CO in the middle to upper troposphere, where the MOPITT versus model bias was reduced by up to two-thirds. Assimilation results show higher levels of CO in the southern tropics, consistent with MOPITT observations. We find good agreement between the TES assimilated model estimates of CO and in situ measurements from the MOZAIC program, which shows a negative bias of up to 10 ppbv in middle and upper tropospheric TES CO. The results demonstrate how assimilation can be used for non-coincident validation of TES CO profile retrievals.


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