We have previously demonstrated a pulsed direct detection IPDA lidar to measure range and the column concentration of atmospheric CO2. The lidar measures the atmospheric backscatter profiles and ...samples the shape of the 1,572.33 nm CO2 absorption line. We participated in the ASCENDS science flights on the NASA DC-8 aircraft during August 2011 and report here lidar measurements made on four flights over a variety of surface and cloud conditions near the US. These included over a stratus cloud deck over the Pacific Ocean, to a dry lake bed surrounded by mountains in Nevada, to a desert area with a coal-fired power plant, and from the Rocky Mountains to Iowa, with segments with both cumulus and cirrus clouds. Most flights were to altitudes >12 km and had 5-6 altitude steps. Analyses show the retrievals of lidar range, CO2 column absorption, and CO2 mixing ratio worked well when measuring over topography with rapidly changing height and reflectivity, through thin clouds, between cumulus clouds, and to stratus cloud tops. The retrievals shows the decrease in column CO2 due to growing vegetation when flying over Iowa cropland as well as a sudden increase in CO2 concentration near a coal-fired power plant. For regions where the CO2 concentration was relatively constant, the measured CO2 absorption lineshape (averaged for 50 s) matched the predicted shapes to better than 1% RMS error. For 10 s averaging, the scatter in the retrievals was typically 2-3 ppm and was limited by the received signal photon count. Retrievals were made using atmospheric parameters from both an atmospheric model and from in situ temperature and pressure from the aircraft. The retrievals had no free parameters and did not use empirical adjustments, and >70% of the measurements passed screening and were used in analysis. The differences between the lidar-measured retrievals and in situ measured average CO2 column concentrations were <1.4 ppm for flight measurement altitudes >6 km.
Many soil‐derived particles dominated by insoluble material, including Saharan dusts, are known to act as ice nuclei. If, however, dust particles can compete with other atmospheric particle types to ...form liquid cloud droplets, they have a greater potential to change climate through indirect effects on cloud radiative properties and to affect the hydrological cycle through precipitation changes. By directly collecting and analyzing the residual nuclei of small cloud droplets, we demonstrate that Saharan dust particles do commonly act as cloud condensation nuclei (CCN) in the eastern North Atlantic. Droplet activation calculations support the measurements by showing that due to its slightly hygroscopic nature, even submicron dust can be important as CCN. Given the dual nature of Saharan dust particles as CCN and ice nuclei, this infusion of dust is expected to impact not only droplet size and albedo in small clouds, but ice formation in deep convective clouds.
Satellite observations of carbon monoxide (CO) from the Measurements of Pollution in the Troposphere (MOPITT) instrument are combined with measurements from the Transport and Chemical Evolution Over ...the Pacific (TRACE-P) aircraft mission over the northwest Pacific and with a global three-dimensional chemical transport model (GEOS-CHEM) to quantify Asian pollution outflow and its trans-Pacific transport during spring 2001. Global CO column distributions in MOPITT and GEOS-CHEM are highly correlated (R(exp 2) = 0.87), with no significant model bias. The largest regional bias is over Southeast Asia, where the model is 18% too high. A 60% decrease of regional biomass burning emissions in the model (to 39 Tg/yr) would correct the discrepancy; this result is consistent with TRACE-P observations. MOPITT and TRACE-P also give consistent constraints on the Chinese source of CO from fuel combustion (181 Tg CO/yr). Four major events of trans-Pacific transport of Asian pollution in spring 2001 were seen by MOPITT, in situ platforms, and GEOS-CHEM. One of them was sampled by TRACE-P (26-27 February) as a succession of pollution layers over the northeast Pacific. These layers all originated from one single event of Asian outflow that split into northern and southern plumes over the central Pacific. The northern plume (sampled at 6-8 km off California) had no ozone enhancement. The southern subsiding plume (sampled at 2-4 km west of Hawaii) contained a 8 - 17 ppbv ozone enhancement, driven by decomposition of peroxyacetylnitrate (PAN) to nitrogen oxides (NOx). This result suggests that PAN decomposition in trans-Pacific pollution plumes subsiding over the United States could lead to significant enhancements of surface ozone.
Our knowledge about synoptic‐scale variations of atmospheric‐CO2 produced by interactions between midlatitude cyclones and regional‐scale surface fluxes remains limited due to the scarcity of ...observations. We synthesized observations of greenhouse gases (GHGs) with respect to frontal passages to understand how GHG distributions change vertically and horizontally during a synoptic event. We use the airborne in situ measurements of GHGs collected during the Atmospheric Carbon and Transport‐America summer 2016 field campaign. Using these measurements, we defined three metrics, (1) the differences in the GHG mole fractions across frontal boundaries in the atmospheric boundary layer (BL) and free troposphere (FT), (2) differences in the vertical contrasts in GHGs in warm and cold sectors, and (3) the size and magnitude of enhanced CO2 in the vicinity of frontal boundary. We found that frontal structures are clearly associated with spatially coherent and significant changes in GHG composition. Warm sector CO2 mole fractions CO2 are higher than those in the cold sector. The cross‐frontal CO2 contrasts are largest in the BL (5–30 ppm) with smaller differences in the FT (3–5 ppm). We found higher CH4 in the BL in the warm sector than in the cold sector for 5 out of 11 cases. Analyses of vertical profiles revealed higher CO2 in the FT than in the BL in the cold sector while opposite pattern in the warm sector. Average BL‐to‐FT CO2 differences are 12 and −6 ppm in the warm and cold sectors, respectively. The observational analyses presented define new metrics involving horizontal and vertical GHG contrasts across fronts during summer which will be used to evaluate simulations of GHG transport.
Key Points
We report the first comprehensive airborne observations of the horizontal and vertical variability in atmospheric greenhouse gases (CO2, CH4) associated with midlatitude cyclones
Cold fronts contain coherent CO2 structures including cross‐frontal contrasts at all levels in the troposphere and a narrow band of enhanced CO2 along the frontal boundary
Fronts showed lower CO2 in the cold sector (north/west) and higher CO2 in the warm sector (south/east), with larger contrasts in boundary layer than in free troposphere
The Atmospheric Carbon and Transport (ACT)-America NASA Earth Venture Suborbital Mission set out to improve regional atmospheric greenhouse gas (GHG) inversions by exploring the intersection of the ...strong GHG fluxes and vigorous atmospheric transport that occurs within the midlatitudes. Two research aircraft instrumented with remote and in situ sensors to measure GHG mole fractions, associated trace gases, and atmospheric state variables collected 1,140.7 flight hours of research data, distributed across 305 individual aircraft sorties, coordinated within 121 research flight days, and spanning five 6-week seasonal flight campaigns in the central and eastern United States. Flights sampled 31 synoptic sequences, including fair-weather and frontal conditions, at altitudes ranging from the atmospheric boundary layer to the upper free troposphere. The observations were complemented with global and regional GHG flux and transport model ensembles. We found that midlatitude weather systems contain large spatial gradients in GHG mole fractions, in patterns that were consistent as a function of season and altitude. We attribute these patterns to a combination of regional terrestrial fluxes and inflow from the continental boundaries. These observations, when segregated according to altitude and air mass, provide a variety of quantitative insights into the realism of regional CO2 and CH4 fluxes and atmospheric GHG transport realizations. The ACT-America dataset and ensemble modeling methods provide benchmarks for the development of atmospheric inversion systems. As global and regional atmospheric inversions incorporate ACT-America’s findings and methods, we anticipate these systems will produce increasingly accurate and precise subcontinental GHG flux estimates.
Ozone measurements by various platforms during the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) operations in the summer of 2004 are assimilated into the ...STEM regional chemical transport model (CTM). Under the four‐dimensional variational data assimilation (4D‐Var) framework, the model forecast (background) error covariance matrix is constructed using both the so‐called NMC (National Meteorological Center, now National Centers for Environmental Prediction) method and the observational (Hollingworth‐Lönnberg) method. The inversion of the covariance matrix is implemented using truncated singular value decomposition (TSVD) approach. The TSVD approach is numerically stable even with severely ill conditioned vertical correlation covariance matrix and large horizontal correlation distances. Ozone observations by different platforms (aircraft, surface, and ozonesondes) are first assimilated separately. The impacts of the various measurements are evaluated on their ability to improve the predictions, defined as the information content of the observations under the current framework. In the end, all observations are assimilated into the CTM. The final analysis matches well with observations from all platforms. Assessed with all the observations throughout the boundary layer and midtroposphere, the model bias is reduced from 11.3 ppbv for the base case to −1.5 ppbv. A reduction of 10.3 ppbv in root mean square error is also seen. In addition, the potential of improving air quality forecasts by chemical data assimilation is demonstrated. The effect of assimilating ozone observations on model predictions of other species is also shown.
The Tropospheric Emission Spectrometer (TES) is an infrared instrument that was launched on board NASA's Aura satellite in 2004. TES is the first instrument to provide vertical information on ...tropospheric ozone while simultaneously measuring CO on a global basis. Before they may be used for scientific study, TES profiles must first be validated to determine if there are any systematic biases present. In this study we present a validation of TES tropospheric ozone using airborne differential absorption lidar (DIAL) profiles obtained during the Intercontinental Chemical Transport Experiment–B (INTEX‐B) campaign, which took place during March–May 2006. During INTEX‐B the NASA DC‐8 aircraft conducted several flights, which allowed the DIAL instrument to obtain ozone profile measurements that were spatially coincident with TES special observations in three different geographical regions. Here we present comparisons of TES and DIAL tropospheric ozone profiles that show that, on average, TES exhibits a small positive bias in the troposphere of 5–15%. We also examine the use of in situ profile observations for the validation of TES tropospheric ozone, and we find these to be of most use in clean regions where the background ozone field is homogeneous.
This work describes aircraft‐based lidar observations of thin cirrus clouds at the tropical tropopause in the central Pacific obtained during the Tropical Ozone Transport Experiment/Vortex Ozone ...Transport Experiment (TOTE/VOTE) in December 1995 and February 1996. Thin cirrus clouds were found at the tropopause on each of the four flights which penetrated within 15° of the equator at 200–210 east longitude. South of 15°N, thin cirrus were detected above the aircraft about 65% of the time that data were available. The altitudes of these clouds exceeded 18 km at times. The cirrus observations could be divided into two basic types: thin quasi‐laminar wisps and thicker, more textured structures. On the basis of trajectory analyses and temperature histories, these two types were usually formed respectively by (1) in situ cooling on both a synoptic scale and mesoscale and (2) recent (a few days) outflow from convection. There is evidence from one case that the thicker clouds can also be formed by in situ cooling. The actual presence or absence of thin cirrus clouds was also consistent with the temperature and convective histories derived from back trajectory calculations. Notably, at any given time, only a relatively small portion (at most 25%) of the west central tropical Pacific has been influenced by convection within the previous 10 days. The structures of some of the thin cirrus clouds formed in situ strongly resembled long‐wavelength (500–1000 km) gravity waves observed nearly simultaneously by the ER‐2 on one of the flights. Comparison with in situ water vapor profiles made by the NASA ER‐2 aircraft provide some observational support for the hypothesis that thin cirrus clouds play an important role in dehydrating tropospheric air as it enters the stratosphere.
Lidar observations collected during the Lidar In-space Technology Experiment experiment in conjunction with the Meteosat and European Centre for Medium-Range Weather Forecasts data have been used not ...only to validate the Saharan dust plume conceptual model constructed from the GARP (Global Atmospheric Research Programme) Atlantic Tropical Experiment data, but also to examine the vicissitudes of the Saharan aerosol including their optical depths across the west Africa and east Atlantic regions. Optical depths were evaluated from both the Meteosat and lidar data. Back trajectory calculations were also made along selected lidar orbits to verify the characteristic anticyclonic rotation of the dust plume over the eastern Atlantic as well as to trace the origin of a dust outbreak over West Africa.
A detailed synoptic analysis including the satellite-derived optical depths, vertical lidar backscattering cross section profiles, and back trajectories of the 16–19 September 1994 Saharan dust outbreak over the eastern Atlantic and its origin over West Africa during the 12–15 September period have been presented. In addition, lidar-derived backscattering profiles and optical depths were objectively analyzed to investigate the general features of the dust plume and its geographical variations in optical thickness. These analyses validated many of the familiar characteristic features of the Saharan dust plume conceptual model such as (i) the lifting of the aerosol over central Sahara and its subsequent transport to the top of the Saharan air layer (SAL), (ii) the westward rise of the dust layer above the gradually deepening marine mixed layer and the sinking of the dust-layer top, (iii) the anticyclonic gyration of the dust pulse between two consecutive trough axes, (iv) the dome-shaped structure of the dust-layer top and bottom, (v) occurrence of a middle-level jet near the southern boundary of the SAL, (vi) transverse–vertical circulations across the SAL front including their possible role in the initiation of a squall line to the southside of the jet that ultimately developed into a tropical storm, and (vii) existence of satellite-based high optical depths to the north of the middle-level jet in the ridge region of the wave.
Furthermore, the combined analyses reveal a complex structure of the dust plume including its origin over North Africa and its subsequent westward migration over the Atlantic Ocean. The dust plume over the west African coastline appears to be composed of two separate but narrow plumes originating over the central Sahara and Lake Chad regions, in contrast to one single large plume shown in the conceptual model. Lidar observations clearly show that the Saharan aerosol over North Africa not only consist of background dust (Harmattan haze) but also wind-blown aerosol from fresh dust outbreaks. They further exhibit maximum dust concentration near the middle-level jet axis with downward extension of heavy dust into the marine boundary layer including a clean dust-free trade wind inversion to the north of the dust layer over the eastern Atlantic region. The lidar-derived optical depths show a rapid decrease of optical depths away from land with maximum optical depths located close to the midlevel jet, in contrast to north of the jet shown by satellite estimates and the conceptual model. To reduce the uncertainties in estimating extinction-to-backscattering ratio for optical depth calculations from lidar data, direct aircraft measurements of optical and physical properties of the Saharan dust layer are needed.