Biomass burning is a major source of pollution in the tropical Southern Hemisphere, and fine mode carbonaceous particles are produced by the same combustion processes that emit carbon monoxide (CO). ...In this paper we examine these emissions with data from the Terra satellite, CO profiles from the Measurement of Pollution in the Troposphere (MOPITT) instrument, and fine‐mode aerosol optical depth (AOD) from the Moderate‐Resolution Imaging Spectroradiometer (MODIS). The satellite measurements are used in conjunction with calculations from the MOZART chemical transport model to examine the 2003 Southern Hemisphere burning season with particular emphasis on the months of peak fire activity in September and October. Pollutant emissions follow the occurrence of dry season fires, and the temporal variation and spatial distributions of MOPITT CO and MODIS AOD are similar. We examine the outflow from Africa and South America with emphasis on the impact of these emissions on clean remote regions. We present comparisons of MOPITT observations and ground‐based interferometer data from Lauder, New Zealand, which indicate that intercontinental transport of biomass burning pollution from Africa often determines the local air quality. The correlation between enhancements of AOD and CO column for distinct biomass burning plumes is very good with correlation coefficients greater than 0.8. We present a method using MOPITT and MODIS data for estimating the emission ratio of aerosol number density to CO concentration which could prove useful as input to modeling studies. We also investigate decay of plumes from African fires following export into the Indian Ocean and compare the MOPITT and MODIS measurements as a way of estimating the regional aerosol lifetime. Vertical transport of biomass burning emissions is also examined using CO profile information. Low‐altitude concentrations are very high close to source regions, but further downwind of the continents, vertical mixing takes place and results in more even CO vertical distributions. In regions of significant convection, particularly in the equatorial Indian Ocean, the CO mixing ratio is greater at higher altitudes, indicating vertical transport of biomass burning emissions to the upper troposphere.
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 summer 2012 and 2013. A total of 23 vertical profiles were measured up to 5000 m above sea level over an extended area (40-45 degree N and 2 degree W-12 degree E) including the Gulf of Genoa, southern France, the Gulf of Lion, and the Spanish coast. During TRAQA and SAFMED the study area experienced a wide range of meteorological conditions which favoured 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 show 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. The measured aerosol scattering coefficient varies between ~ 20 and 120 Mm-1, while carbon monoxide (CO) and ozone (O3) mixing ratios are in the range of 60-165 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 mu m) and accumulation (0.1-1.0 mu m) modes is between ~ 30 and 5000-6000 scm-3 (standard cm-3), which is comparable to the aerosol concentration measured in continental areas under pollution conditions. Additionally, our measurements indicate the presence of highly concentrated Aitken layers (10 000-15 000 scm-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.
Measurements of Pollution in the Troposphere (MOPITT) is a new remote sensing instrument aboard the Earth Observing System (EOS) “Terra” satellite which exploits gas correlation radiometry principles ...to quantify tropospheric concentrations of carbon monoxide (CO) and methane (CH4). The MOPITT CO retrieval algorithm employs a nonlinear optimal estimation method to iteratively solve for the CO profile which is statistically most consistent with both the satellite‐measured radiances and a priori information. The algorithm's theoretical basis is described in terms of the observed radiances and their weighting functions, the a priori information, and the retrieval averaging kernels. Examples of actual CO retrievals over scenes with contrasting pollution conditions are demonstrated, and interpreted in the context of the retrieval averaging kernels and a priori.
We use satellite sensor measurements to obtain a broad picture of the processes affecting tropical tropospheric O3 production over Africa and the Atlantic in the early part of the year. Terra/MOPITT ...CO retrievals correlate well with biomass burning fire counts observed by the TRMM/VIRS instrument in Northern Hemisphere savanna regions and allow investigation of the subsequent convection of the biomass burning plume at the intertropical convergence zone and interhemispheric transport. Measurements of NO2 from the ERS‐2/GOME instrument enable identification of two important tropical sources of this O3 precursor, biomass burning and lightning. Good correlation is seen between NO2 retrievals and TRMM/LIS lightning flash observations in southern African regions free of biomass burning, thus indicating a probable lightning source of NOx. The combination of MOPITT CO, GOME NO2, and TRMM fire and lightning flash counts provides a powerful tool for investigating the tropospheric production of O3 precursors. These data are used in conjunction with the MOZART‐2 chemical transport model to investigate the early year tropical Atlantic tropospheric O3 distribution using January 2001 as a case study. Inconsistencies between the various tropical tropospheric O3 column products obtained from EP/TOMS data, and between these products, in situ measurements, and modeling, have led to questions about how the Northern Hemisphere biomass burning is connected to the TOMS derived O3 maximum in the tropical southern Atlantic. We show that the early year tropical O3 distribution is actually characterized by two maxima. The first arises due to biomass burning emissions, is located near the Northern Hemisphere fires, and is most evident in the lower troposphere. The second is located in the southern tropical Atlantic midtroposphere, and results from NOx produced by lightning over southern Africa and South America.
We study the carbon monoxide (CO) variability in the last decade measured by NASA's Atmospheric InfraRed Sounder (AIRS) on the Earth Observing System (EOS)/Aqua satellite. The focus of this study is ...to analyze CO variability and short-term trends separately for background CO and fresh CO emissions based on a new statistical approach. The AIRS Level 2 (L2) retrieval algorithm utilizes cloud clearing to treat cloud contaminations in the signals, and this increases the data coverage significantly to a yield of more than 50% of the total measurements. We first study if the cloud clearing affects CO retrievals and the subsequent trend studies by using the collocated Moderate Resolution Imaging Spectroradiometer (MODIS) cloud mask to identify AIRS clear sky scenes. We then carry out a science analysis using AIRS CO data individually for the clear and cloud-cleared scenes to identify any potential effects due to cloud clearing. We also introduce a new technique to separate background and recently emitted CO observations, which aims to constrain emissions using only satellite CO data. We validate the CO variability of the recent emissions estimated from AIRS against other emission inventory databases (i.e., Global Fire Emissions Database - GFED3 and the MACC/CityZEN UE - MACCity) and calculate that the correlation coefficients between the AIRS CO recently emitted and the emission inventory databases are 0.726 for the Northern Hemisphere (NH) and 0.915 for the Southern Hemisphere (SH). The high degree of agreement between emissions identified using only AIRS CO and independent inventory sources demonstrates the validity of this approach to separate recent emissions from the background CO using one satellite data set.
This study tests a novel methodology to add value to satellite data sets. This methodology, data fusion, is similar to data assimilation, except that the background model-based field is replaced by a ...satellite data set, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these data sets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS-TES and AIRS-MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20-30% and above 20%, respectively) as compared with AIRS-only version 5 CO retrievals, and improved daily coverage compared with TES and MLS CO data.
We conduct analyses to assess how characteristics of observations of ozone and its precursors affect air quality forecasting and research. To carry out this investigation, we use a photochemical box ...model and its adjoint integrated with a Lagrangian 4D-variational data assimilation system. Using this framework in conjunction with pseudo-observations, we perform an ozone precursor source inversion and estimate surface emissions. We then assess the resulting improvement in ozone air quality prediction. We use an analytical model to conduct uncertainty analyses. Using this analytical tool, we address some key questions regarding how the characteristics of observations affect ozone precursor emission inversion and in turn ozone prediction. These questions include what the effect is of choosing which species to observe, of varying amounts of observation noise, of changing the observing frequency and the observation time during the diurnal cycle, and of how these different scenarios interact with different photochemical regimes. In our investigation we use three observed species scenarios: CO and NO2; ozone, CO, and NO2; and HCHO, CO and NO2. The photochemical model was set up to simulate a range of summertime polluted environments spanning NOx-(NO and NO2)-limited to volatile organic compound (VOC)-limited conditions. We find that as the photochemical regime changes, here is a variation in the relative importance of trace gas observations to be able to constrain emission estimates and to improve the subsequent ozone forecasts. For example, adding ozone observations to an NO2 and CO observing system is found to decrease ozone prediction error under NOx- and VOC-limited regimes, and complementing the NO2 and CO system with HCHO observations would improve ozone prediction in the transitional regime and under VOC-limited conditions. We found that scenarios observing ozone and HCHO with a relative observing noise of lower than 33 % were able to achieve ozone prediction errors of lower than 5 ppbv (parts per billion by volume). Further, only observing intervals of 3 h or shorter were able to consistently achieve ozone prediction errors of 5 ppbv or lower across all photochemical regimes. Making observations closer to the prediction period and either in the morning or afternoon rush hour periods made greater improvements for ozone prediction: 0.2–0.3 ppbv for the morning rush hour and from 0.3 to 0.8 ppbv for the afternoon compared to only 0–0.1 ppbv for other times of the day. Finally, we made two complementary analyses that show that our conclusions are insensitive to the assumed diurnal emission cycle and to the choice of which VOC species emission to estimate using our framework. These questions will address how different types of observing platform, e.g. geostationary satellites or ground monitoring networks, could support future air quality research and forecasting.
Validation of the Measurements of Pollution in the Troposphere (MOPITT) retrievals of carbon monoxide (CO) has been performed with a varied set of correlative data. These include in situ observations ...from a regular program of aircraft observations at five sites ranging from the Arctic to the tropical South Pacific Ocean. Additional in situ profiles are available from several short‐term research campaigns situated over North and South America, Africa, and the North and South Pacific Oceans. These correlative measurements are a crucial component of the validation of the retrieved CO profiles and columns from MOPITT. The current validation results indicate good quantitative agreement between MOPITT and in situ profiles, with an average bias less than 20 ppbv at all levels. Comparisons with measurements that were timed to sample profiles coincident with MOPITT overpasses show much less variability in the biases than those made by various groups as part of research field experiments. The validation results vary somewhat with location, as well as a change in the bias between the Phase 1 and Phase 2 retrievals (before and after a change in the instrument configuration due to a cooler failure). During Phase 1, a positive bias is found in the lower troposphere at cleaner locations, such as over the Pacific Ocean, with smaller biases at continental sites. However, the Phase 2 CO retrievals show a negative bias at the Pacific Ocean sites. These validation comparisons provide critical assessments of the retrievals and will be used, in conjunction with ongoing improvements to the retrieval algorithms, to further reduce the retrieval biases in future data versions.
The space and time variabilities of methane (CH4) total column and upper tropospheric mixing ratios are analysed above the Mediterranean Basin (MB) as part of the Chemical and Aerosol Mediterranean ...Experiment (ChArMEx) programme. Since the analysis of the mid-to-upper tropospheric CH4 distribution from spaceborne sensors and model outputs is challenging, we have adopted a climatological approach and have used a wide variety of data sets. We have combined spaceborne measurements from the Thermal And Near infrared Sensor for carbon Observations – Fourier Transform Spectrometer (TANSO-FTS) instrument on the Greenhouse gases Observing SATellite (GOSAT) satellite, the Atmospheric InfraRed Spectrometer (AIRS) on the AURA platform and the Infrared Atmospheric Sounder Interferometer (IASI) instrument aboard the MetOp-A platform with model results from the Chemical Transport Model (CTM) MOCAGE, and the Chemical Climate Models (CCMs) CNRM-AOCCM and LMDz-OR-INCA (according to different emission scenarios). In order to minimize systematic errors in the spaceborne measurements, we have only considered maritime pixels over the MB. The period of interest spans from 2008 to 2011 considering satellite and MOCAGE data and, regarding the CCMs, from 2001 to 2010. Although CH4 is a long-lived tracer with lifetime of ~12 years and is supposed to be well mixed in the troposphere, an east–west gradient in CH4 is observed and modelled in the mid-to-upper troposphere with a maximum in the Western MB in all seasons except in summer when CH4 accumulates above the Eastern MB. The peak-to-peak amplitude of the east–west seasonal variation in CH4 above the MB in the upper troposphere (300 hPa) is weak but almost twice as great in the satellite measurements (~25 ppbv) as in the model data (~15 ppbv). The maximum of CH4 in summer above the eastern MB can be explained by a series of dynamical processes only occurring in summer. The Asian monsoon traps and uplifts high amounts of CH4 to the upper troposphere where they build up. The Asian Monsoon Anticyclone redistributes these elevated CH4 amounts towards North Africa and the Middle East to finally reach and descend in the eastern MB. In the lower troposphere, the CH4 variability is mainly driven by the local sources of emission in the vicinity of the MB.
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