Examining the accuracy of satellite retrievals of trace-gas emissions and lifetimes using high-resolution plume modelling.

2021 ◽  
Author(s):  
Zoe Davis ◽  
Debora Griffin ◽  
Yue Jia ◽  
Susann Tegtmeier ◽  
Mallory Loria ◽  
...  
Keyword(s):  
Wind Direction ◽  
Vertical Profile ◽  
Trace Gases ◽  
Meteorological Conditions ◽  
Point Sources ◽  
Satellite Observations ◽  
Trace Gas ◽  
Vertical Column ◽  
Retrieval Method ◽  
The Impact

<p>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 “synthetic” 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’s vertical column. In the retrieval method, the VCDs’ 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, “line-density”, retrieval method will also be presented (Adams et al., 2019; Goldberg et al., 2019).</p>

Estimating wildfire emissions of ammonia using Cross-track Infrared Sounder (CrIS) profile information

2021 ◽  
Author(s):  
Ellen Eckert ◽  
Zoe Y. W. Davis ◽  
Mark W. Shephard ◽  
Chris A. McLinden ◽  
Debora Griffin ◽  
...  
Keyword(s):  
Wind Direction ◽  
Vertical Profile ◽  
Three Dimensional ◽  
Emission Rates ◽  
Aerosol Formation ◽  
Satellite Measurements ◽  
Vertical Column ◽  
Fire Emissions ◽  
Cross Track ◽  
The Impact

<p>Ammonia plays an important role for air, soil and water quality, as well as aerosol formation and plant growth. Accurate estimates of emission rates of ammonia from wildfires are crucial to understand the impact on human health and ecosystems. However, ground-based measurements of ammonia are sporadic. Satellite measurements can help address this monitoring gap. The Cross-track Infrared Sounder (CrIS) product provides a unique tool because some information on the vertical distribution of ammonia is derived from the profile retrievals in addition to vertical column densities (VCDs). Emission rates are retrieved by fitting measured vertical column densities (VCDs) to a three-dimensional function of the wind speed and spatial coordinates. This method requires VCDs to be rotated given the wind-direction to remove wind-direction as a fitting variable. The vertical information given by CrIS provides the potential for more accurate emission estimates as wind-direction and -speed at each profile level can be taken into account. The application of the vertical profile of wind also allows more accurate estimates of plume width, which can vary significantly in the traditional VCD rotation depending on the altitudes of wind used for the rotation. This approach was developed and validated using synthetic satellite measurements of plumes simulated by the FLEXPART (v10.0) model to better understand the impact of variability in the vertical profile of the wind. The methodology was then applied using CrIS satellite observations to estimate forest fire emissions of NH3. Preliminary results of this study will be presented.</p>

scholarly journals Recommendations for HCHO and SO2 Retrieval Settings from MAX-DOAS Observations under Different Meteorological Conditions

2021 ◽  
Vol 13 (12) ◽  
pp. 2244
Author(s):  
Zeeshan Javed ◽  
Aimon Tanvir ◽  
Muhammad Bilal ◽  
Wenjing Su ◽  
Congzi Xia ◽  
...  
Keyword(s):  
Column Density ◽  
Trace Gases ◽  
Meteorological Conditions ◽  
Optical Absorption Spectroscopy ◽  
Chemical Production ◽  
Vertical Column ◽  
Phase Oxidation ◽  
Fog Days ◽  
Rms Errors ◽  
Optimal Settings

Recently, the occurrence of fog and haze over China has increased. The retrieval of trace gases from the multi-axis differential optical absorption spectroscopy (MAX-DOAS) is challenging under these conditions. In this study, various reported retrieval settings for formaldehyde (HCHO) and sulfur dioxide (SO2) are compared to evaluate the performance of these settings under different meteorological conditions (clear day, haze, and fog). The dataset from 1st December 2019 to 31st March 2020 over Nanjing, China, is used in this study. The results indicated that for HCHO, the optimal settings were in the 324.5–359 nm wavelength window with a polynomial order of five. At these settings, the fitting and root mean squared (RMS) errors for column density were considerably improved for haze and fog conditions, and the differential slant column densities (DSCDs) showed more accurate values compared to the DSCDs between 336.5 and 359 nm. For SO2, the optimal settings for retrieval were found to be at 307–328 nm with a polynomial order of five. Here, root mean square (RMS) and fitting errors were significantly lower under all conditions. The observed HCHO and SO2 vertical column densities were significantly lower on fog days compared to clear days, reflecting a decreased chemical production of HCHO and aqueous phase oxidation of SO2 in fog droplets.

scholarly journals Air quality impacts of COVID-19 lockdown measures detected from space using high spatial resolution observations of multiple trace gases from Sentinel-5P/TROPOMI

2021 ◽  
Author(s):  
Pieternel F. Levelt ◽  
Deborah C. Stein Zweers ◽  
Ilse Aben ◽  
Maite Bauwens ◽  
Tobias Borsdorff ◽  
...  
Keyword(s):  
Air Quality ◽  
Spatial Resolution ◽  
High Spatial Resolution ◽  
Trace Gases ◽  
Trace Gas ◽  
Joint Analysis ◽  
Anthropogenic Emissions ◽  
China And India ◽  
Societal Relevance ◽  
The Impact

Abstract. The aim of this paper is two-fold: to provide guidance on how to best interpret TROPOMI trace gas retrievals and to highlight how TROPOMI trace gas data can be used to understand event-based impacts on air quality from regional to city-scales around the globe. For this study, we present the observed changes in the atmospheric column amounts of five trace gases (NO2, SO2, CO, HCHO and CHOCHO) detected by the Sentinel-5P TROPOMI instrument, driven by reductions of anthropogenic emissions due to COVID-19 lockdown measures in 2020. We report clear COVID-19-related decreases in NO2 concentrations on all continents. For megacities, reductions in column amounts of tropospheric NO2 range between 14 % and 63 %. For China and India supported by NO2 observations, where the primary source of anthropogenic SO2 is coal-fired power generation, we were able to detect sector-specific emission changes using the SO2 data. For HCHO and CHOCHO, we consistently observe anthropogenic changes in two-week averaged column amounts over China and India during the early phases of the lockdown periods. That these variations over such a short time scale are detectable from space, is due to the high resolution and improved sensitivity of the TROPOMI instrument. For CO, we observe a small reduction over China which is in concert with the other trace gas reductions observed during lockdown, however large, interannual differences prevent firm conclusions from being drawn. The joint analysis of COVID-19 lockdown-driven reductions in satellite observed trace gas column amounts, using the latest operational and scientific retrieval techniques for five species concomitantly is unprecedented. However, the meteorologically and seasonally driven variability of the five trace gases does not allow for drawing fully quantitative conclusions on the reduction of anthropogenic emissions based on TROPOMI observations alone. We anticipate that in future, the combined use of inverse modelling techniques with the high spatial resolution data from S5P/TROPOMI for all observed trace gases presented here, will yield a significantly improved sector-specific, space-based analysis of the impact of COVID-19 lockdown measures as compared to other existing satellite observations. Such analyses will further enhance the scientific impact and societal relevance of the TROPOMI mission.

Impact of 3D cloud structures on tropospheric NO2 column measurements from UV-VIS sounders

2020 ◽  
Author(s):  
Huan Yu ◽  
Arve Kylling ◽  
Claudia Emde ◽  
Bernhard Mayer ◽  
Kerstin Stebel ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Mitigation Strategies ◽  
Trace Gas ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Vertical Column ◽  
Ice Clouds ◽  
Cloud Data ◽  
One Step ◽  
The Impact

<p>Operational retrievals of tropospheric trace gases from space-borne spectrometers are made using 1D radiative transfer models. To minimize cloud effects generally only partially cloudy pixels are analysed using simplified cloud contamination treatments based on radiometric cloud fraction estimates and photon path length corrections based on oxygen collision pair (O<sub>2</sub>-O<sub>2</sub>) or O<sub>2</sub>A-absorption band measurements. In reality, however, the impact of clouds can be much more complex, involving scattering of clouds in neighbouring pixels and cloud shadow effects. Therefore, to go one step further, other correction methods may be envisaged that use sub-pixel cloud information from co-located imagers. Such methods require an understanding of the impact of clouds on the real 3D radiative transfer. We quantify this impact using the MYSTIC 3D radiative transfer model. The generation of realistic 3D input cloud fields, needed by MYSTIC (or any other 3D radiative transfer model), is non-trivial. We use cloud data generated by the ICOsahedral Non-hydrostatic (ICON) atmosphere model for a region including Germany, the Netherlands and parts of other surrounding countries. The model simulates realistic liquid and ice clouds with a horizontal spatial resolution of 156 m and it has been validated against ground-based and satellite-based observational data.</p><p>As a trace gas example, we study NO<sub>2</sub>, a key tropospheric trace gas measured by the atmospheric Sentinels. The MYSTIC 3D model simulates visible spectra, which are ingested in standard DOAS retrieval algorithms to retrieve the NO<sub>2</sub> column amount. Spectra are simulated for a number of realistic cloud scenarios, snow free surface albedos, and solar and satellite geometries typical of low-earth and geostationary orbits. The retrieved NO<sub>2</sub> vertical column densities (VCD) are compared with the true values to identify conditions where 3D cloud effects lead to significant biases on the NO<sub>2</sub> VCDs. A variety of possible mitigation strategies for such pixels are then explored.</p>

scholarly journals Impacts of updated spectroscopy on thermal infrared retrievals of methane evaluated with HIPPO data

2014 ◽  
Vol 7 (9) ◽  
pp. 10059-10107
Author(s):  
M. J. Alvarado ◽  
V. H. Payne ◽  
K. E. Cady-Pereira ◽  
J. D. Hegarty ◽  
S. S. Kulawik ◽  
...  
Keyword(s):  
Nitrous Oxide ◽  
Trace Gases ◽  
Thermal Infrared ◽  
Trace Gas ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Spectroscopic Parameters ◽  
Mixing Ratios ◽  
Aircraft Observations ◽  
The Impact

Abstract. Errors in the spectroscopic parameters used in the forward radiative transfer model can introduce altitude-, spatially-, and temporally-dependent biases in trace gas retrievals. For well-mixed trace gases such as methane, where the variability of tropospheric mixing ratios is relatively small, reducing such biases is particularly important. We use aircraft observations from all five missions of the HIAPER Pole-to-Pole Observations (HIPPO) of the Carbon Cycle and Greenhouse Gases Study to evaluate the impact of updates to spectroscopic parameters for methane (CH4), water vapor (H2O), and nitrous oxide (N2O) on thermal infrared retrievals of methane from the NASA Aura Tropospheric Emission Spectrometer (TES). We find that updates to the spectroscopic parameters for CH4 result in a substantially smaller mean bias in the retrieved CH4 when compared with HIPPO observations. After an N2O-based correction, the bias in TES methane upper tropospheric representative values for measurements between 50° S and 50° N decreases from 56.9 to 25.7 ppbv, while the bias in the lower tropospheric representative value increases only slightly (from 27.3 to 28.4 ppbv). For retrievals with less than 1.6 DOFS, the bias is reduced from 26.8 to 4.8 ppbv. We also find that updates to the spectroscopic parameters for N2O reduce the errors in the retrieved N2O profile.

scholarly journals Versatile soil gas concentration and isotope monitoring: optimization and integration of novel soil gas probes with online trace gas detection

2022 ◽  
Vol 19 (1) ◽  
pp. 165-185
Author(s):  
Juliana Gil-Loaiza ◽  
Joseph R. Roscioli ◽  
Joanne H. Shorter ◽  
Till H. M. Volkmann ◽  
Wei-Ren Ng ◽  
...  
Keyword(s):  
Real Time ◽  
Trace Gases ◽  
Soil Gas ◽  
Redox Conditions ◽  
Trace Gas ◽  
Soil System ◽  
Isotopic Signatures ◽  
Gas Measurements ◽  
The Impact

Abstract. Gas concentrations and isotopic signatures can unveil microbial metabolisms and their responses to environmental changes in soil. Currently, few methods measure in situ soil trace gases such as the products of nitrogen and carbon cycling or volatile organic compounds (VOCs) that constrain microbial biochemical processes like nitrification, methanogenesis, respiration, and microbial communication. Versatile trace gas sampling systems that integrate soil probes with sensitive trace gas analyzers could fill this gap with in situ soil gas measurements that resolve spatial (centimeters) and temporal (minutes) patterns. We developed a system that integrates new porous and hydrophobic sintered polytetrafluoroethylene (sPTFE) diffusive soil gas probes that non-disruptively collect soil gas samples with a transfer system to direct gas from multiple probes to one or more central gas analyzer(s) such as laser and mass spectrometers. Here, we demonstrate the feasibility and versatility of this automated multiprobe system for soil gas measurements of isotopic ratios of nitrous oxide (δ18O, δ15N, and the 15N site preference of N2O), methane, carbon dioxide (δ13C), and VOCs. First, we used an inert silica matrix to challenge probe measurements under controlled gas conditions. By changing and controlling system flow parameters, including the probe flow rate, we optimized recovery of representative soil gas samples while reducing sampling artifacts on subsurface concentrations. Second, we used this system to provide a real-time window into the impact of environmental manipulation of irrigation and soil redox conditions on in situ N2O and VOC concentrations. Moreover, to reveal the dynamics in the stable isotope ratios of N2O (i.e., 14N14N16O, 14N15N16O, 15N14N16O, and 14N14N18O), we developed a new high-precision laser spectrometer with a reduced sample volume demand. Our integrated system – a tunable infrared laser direct absorption spectrometry (TILDAS) in parallel with Vocus proton transfer reaction mass spectrometry (PTR-MS), in line with sPTFE soil gas probes – successfully quantified isotopic signatures for N2O, CO2, and VOCs in real time as responses to changes in the dry–wetting cycle and redox conditions. Broadening the collection of trace gases that can be monitored in the subsurface is critical for monitoring biogeochemical cycles, ecosystem health, and management practices at scales relevant to the soil system.

scholarly journals Atmospheric transport and chemistry of trace gases in LMDz5B: evaluation and implications for inverse modelling

2015 ◽  
Vol 8 (2) ◽  
pp. 129-150 ◽  
Author(s):  
R. Locatelli ◽  
P. Bousquet ◽  
F. Hourdin ◽  
M. Saunois ◽  
A. Cozic ◽  
...  
Keyword(s):  
Greenhouse Gas Emissions ◽  
Greenhouse Gas ◽  
Atmospheric Transport ◽  
Trace Gases ◽  
Inverse Modelling ◽  
Trace Gas ◽  
Vertical Resolution ◽  
Tracer Transport ◽  
Gas Emissions ◽  
The Impact

Abstract. Representation of atmospheric transport is a major source of error in the estimation of greenhouse gas sources and sinks by inverse modelling. Here we assess the impact on trace gas mole fractions of the new physical parameterizations recently implemented in the atmospheric global climate model LMDz to improve vertical diffusion, mesoscale mixing by thermal plumes in the planetary boundary layer (PBL), and deep convection in the troposphere. At the same time, the horizontal and vertical resolution of the model used in the inverse system has been increased. The aim of this paper is to evaluate the impact of these developments on the representation of trace gas transport and chemistry, and to anticipate the implications for inversions of greenhouse gas emissions using such an updated model. Comparison of a one-dimensional version of LMDz with large eddy simulations shows that the thermal scheme simulates shallow convective tracer transport in the PBL over land very efficiently, and much better than previous versions of the model. This result is confirmed in three-dimensional simulations, by a much improved reproduction of the radon-222 diurnal cycle. However, the enhanced dynamics of tracer concentrations induces a stronger sensitivity of the new LMDz configuration to external meteorological forcings. At larger scales, the inter-hemispheric exchange is slightly slower when using the new version of the model, bringing them closer to observations. The increase in the vertical resolution (from 19 to 39 layers) significantly improves the representation of stratosphere/troposphere exchange. Furthermore, changes in atmospheric thermodynamic variables, such as temperature, due to changes in the PBL mixing modify chemical reaction rates, which perturb chemical equilibriums of reactive trace gases. One implication of LMDz model developments for future inversions of greenhouse gas emissions is the ability of the updated system to assimilate a larger amount of high-frequency data sampled at high-variability stations. Others implications are discussed at the end of the paper.

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

2011 ◽  
Vol 4 (6) ◽  
pp. 1241-1260 ◽  
Author(s):  
C. Prados-Roman ◽  
A. Butz ◽  
T. Deutschmann ◽  
M. Dorf ◽  
L. Kritten ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Vertical Distribution ◽  
Vertical Profile ◽  
Trace Gases ◽  
Trace Gas ◽  
Vertical Profiles ◽  
Cloud Particle ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Tropospheric Aerosol

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.

scholarly journals The impacts of ocean acidification on marine trace gases and the implications for atmospheric chemistry and climate

2020 ◽  
Vol 476 (2237) ◽  
pp. 20190769 ◽  
Author(s):  
Frances E. Hopkins ◽  
Parvadha Suntharalingam ◽  
Marion Gehlen ◽  
Oliver Andrews ◽  
Stephen D. Archer ◽  
...  
Keyword(s):  
Ocean Acidification ◽  
Atmospheric Chemistry ◽  
Process Model ◽  
Trace Gases ◽  
Gas Production ◽  
Trace Gas ◽  
Model Organisms ◽  
Gas Fluxes ◽  
Trace Gas Fluxes ◽  
The Impact

Surface ocean biogeochemistry and photochemistry regulate ocean–atmosphere fluxes of trace gases critical for Earth's atmospheric chemistry and climate. The oceanic processes governing these fluxes are often sensitive to the changes in ocean pH (or p CO 2 ) accompanying ocean acidification (OA), with potential for future climate feedbacks. Here, we review current understanding (from observational, experimental and model studies) on the impact of OA on marine sources of key climate-active trace gases, including dimethyl sulfide (DMS), nitrous oxide (N 2 O), ammonia and halocarbons. We focus on DMS, for which available information is considerably greater than for other trace gases. We highlight OA-sensitive regions such as polar oceans and upwelling systems, and discuss the combined effect of multiple climate stressors (ocean warming and deoxygenation) on trace gas fluxes. To unravel the biological mechanisms responsible for trace gas production, and to detect adaptation, we propose combining process rate measurements of trace gases with longer term experiments using both model organisms in the laboratory and natural planktonic communities in the field. Future ocean observations of trace gases should be routinely accompanied by measurements of two components of the carbonate system to improve our understanding of how in situ carbonate chemistry influences trace gas production. Together, this will lead to improvements in current process model capabilities and more reliable predictions of future global marine trace gas fluxes.

scholarly journals Investigating the impact of regional transport on PM<sub>2.5</sub> formation using vertical observation during APEC 2014 Summit in Beijing

2016 ◽  
Vol 16 (24) ◽  
pp. 15451-15460 ◽  
Author(s):  
Yang Hua ◽  
Shuxiao Wang ◽  
Jiandong Wang ◽  
Jingkun Jiang ◽  
Tianshu Zhang ◽  
...  
Keyword(s):  
Relative Humidity ◽  
Fine Particulate Matter ◽  
Ground Level ◽  
Meteorological Conditions ◽  
Point Sources ◽  
Asia Pacific ◽  
Rural Site ◽  
Regional Transport ◽  
Observation Methods ◽  
The Impact

Abstract. During the APEC (Asia-Pacific Economic Cooperation) Economic Leaders' 2014 Summit in Beijing, strict regional air emission controls were implemented, providing a unique opportunity to investigate the transport and formation mechanism of fine particulate matter (PM2.5). This study explores the use of vertical observation methods to investigate the influence of regional transport on PM2.5 pollution in Beijing before and during the APEC Summit. Vertical profiles of extinction coefficient, wind, temperature and relative humidity were monitored at a rural site on the border of Beijing and Hebei Province. Three PM2.5 pollution episodes were analyzed. In episode 1 (27 October to 1 November), regional transport accompanied by the accumulation of pollutants under unfavorable meteorological conditions led to the pollution. In episode 2 (2–5 November), pollutants left from episode 1 were retained in the boundary layer of the region for 2 days and then settled down to the surface, leading to an explosive increase of PM2.5. The regional transport of aged aerosols played a crucial role in the heavy PM2.5 pollution. In episode 3 (6–11 November), emissions from large point sources had been controlled for several days while primary emissions from diesel vehicles might have led to the pollution. It is found that ground-level observation of meteorological conditions and air quality could not fully explain the pollution process, while vertical parameters (aerosol optical properties, winds, relative humidity and temperature) improved the understanding of regional transport influence on heavy pollution processes. Future studies may consider including vertical observations to aid investigation of pollutant transport, especially during episodic events of rapidly increasing concentrations.

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