In situ evidence for renitrification in the Arctic lower stratosphere during the polar aura validation experiment (PAVE)

In-situ measurements of nitric acid (HNO3), ozone (O3), and nitrous oxide (N2O) were made from the NASA DC-8 during the Polar Aura Validation Experiment in January/February 2005. In the lower stratosphere (9–12.5 km, potential temperature 300–350 K) characteristic compact relationships were observed between all three gases. The ratio HNO3/O3 averaged 3.5 (±0.7) ppt/ppb. Samples with enhanced HNO3/O3 (\u3e4.0) were most abundant under the edge of the Arctic Polar vortex in airmasses with enhanced mixing ratios of both gases (\u3e400 ppb O3 and \u3e2000 ppt HNO3) and reduced mixing ratios of N2O (\u3c305 ppb), indicating air from higher levels in the stratosphere. Relationships to N2O in the anomalous samples under the vortex edge indicate that increases in HNO3/O3 reflect renitrification at DC-8 flight levels, with no indication of significant O3 loss. Renitrified air was only observed at potential temperatures above 340 K, and was most abundant on the PAVE flights on 27 and 29 January

Aerosol chemical composition in Asian continental outflow during the TRACE-P campaign: Comparison with PEM-West B

Aerosol associated soluble ions and the radionuclide tracers 7Be and 210Pb were quantified in 414 filter samples collected in spring 2001 from the DC-8 during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign. Binning the data into near Asia (flights from Hong Kong and Japan) and remote Pacific (all other flights) revealed large enhancements of NO3−, SO4=, C2O4=, NH4+, K+, Mg2+, and Ca2+ near Asia. The boundary layer and lower troposphere were most strongly influenced by continental outflow, and the largest enhancements were seen in Ca2+ (a dust tracer) and NO3− (reflecting uptake of HNO3 onto the dust). Comparing the TRACE P near Asia bin with earlier results from the same region during PEM-West B (in 1994) shows at least twofold enhancements during TRACE P in most of the ions listed above. Calcium and NO3− were most enhanced in this comparison as well (more than sevenfold higher in the boundary layer and threefold higher in the lower troposphere). Independent estimation of Asian emissions of gaseous precursors of the aerosol-associated ions suggest only small changes between the two missions, and precipitation fields do not suggest any significant difference in the efficiency of the primary sink, precipitation scavenging. It thus appears that with the possible exception of dust, the enhancements of aerosol-associated species during TRACE P cannot be explained by stronger sources or weaker sinks. We argue that the enhancements largely reflect the fact that TRACE P focused on characterizing Asian outflow, and thus the DC-8 was more frequently flown into regions that were influenced by well-organized flow off the continent

Impact of multiscale dynamical processes and mixing on the chemical composition of the upper troposphere and lower stratosphere during the Intercontinental Chemical Transport Experiment–North America

We use high-frequency in situ observations made from the DC8 to examine fine-scale tracer structure and correlations observed in the upper troposphere and lower stratosphere during INTEX-NA. Two flights of the NASA DC-8 are compared and contrasted. Chemical data from the DC-8 flight on 18 July show evidence for interleaving and mixing of polluted and stratospheric air masses in the vicinity of the subtropical jet in the upper troposphere, while on 2 August the DC-8 flew through a polluted upper troposphere and a lowermost stratosphere that showed evidence of an intrusion of polluted air. We compare data from both flights with RAQMS 3-D global meteorological and chemical model fields to establish dynamical context and to diagnose processes regulating the degree of mixing on each day. We also use trajectory mapping of the model fields to show that filamentary structure due to upstream strain deformation contributes to tracer variability observed in the upper troposphere. An Eulerian measure of strain versus rotation in the large-scale flow is found useful in predicting filamentary structure in the vicinity of the jet. Higher-frequency (6–24 km) tracer variability is attributed to buoyancy wave oscillations in the vicinity of the jet, whose turbulent dissipation leads to efficient mixing across tracer gradients

Chemical data assimilation estimates of continental U.S. ozone and nitrogen budgets during the Intercontinental Chemical Transport Experiment-North America

Global ozone analyses, based on assimilation of stratospheric profile and ozone column measurements, and NOy predictions from the Real-time Air Quality Modeling System (RAQMS) are used to estimate the ozone and NOy budget over the continental United States during the July-August 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during INTEX-A show that RAQMS captures the main features of the global and continental U.S. distribution of tropospheric ozone, carbon monoxide, and NOy with reasonable fidelity. Assimilation of stratospheric profile and column ozone measurements is shown to have a positive impact on the RAQMS upper tropospheric/lower stratosphere ozone analyses, particularly during the period when SAGE III limb scattering measurements were available. Eulerian ozone and NOy budgets during INTEX-A show that the majority of the continental U.S. export occurs in the upper troposphere/lower stratosphere poleward of the tropopause break, a consequence of convergence of tropospheric and stratospheric air in this region. Continental U.S. photochemically produced ozone was found to be a minor component of the total ozone export, which was dominated by stratospheric ozone during INTEX-A. The unusually low photochemical ozone export is attributed to anomalously cold surface temperatures during the latter half of the INTEX-A mission, which resulted in net ozone loss during the first 2 weeks of August. Eulerian NOy budgets are shown to be very consistent with previously published estimates. The NOy export efficiency was estimated to be 24%, with NOx + PAN accounting for 54% of the total NOy export during INTEX-A. Copyright 2007 by the American Geophysical Union

The View from the Top: CALIOP Ice Water Content in the Uppermost Layer of Tropical Cyclones

NASA's CALIPSO satellite carries both the Cloud and Aerosol Lidar with Orthogonal Polarization (CALIOP) and the Imaging Infrared Radiometer (IIR). The lidar is ideally suited to viewing the very top of tropical cyclones, and the IIR provides critical optical and microphysical information. The lidar and the IIR data work together to understand storm clouds since they are perfectly co-located, and big tropical cyclones provide an excellent complex target for comparing the observations. There is a lot of information from these case studies for understanding both the observations and the tropical cyclones, and we are just beginning to scratch the surface of what can be learned. Many tropical cyclone cloud particle measurements are focused on the middle and lower regions of storms, but characterization of cyclone interaction with the lowermost stratosphere at the upper storm boundary may be important for determining the total momentum and moisture transport budget, and perhaps for predicting storm intensity as well. A surprising amount of cloud ice is to be found at the very top of these big storms

Reactive nitrogen in Asian continental outflow over the western Pacific: Results from the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) airborne mission

We present here results for reactive nitrogen species measured aboard the NASA DC-8 aircraft during the Transport and Chemical Evolution over the Pacific (TRACE-P) mission. The large-scale distributions total reactive nitrogen (NOy,sum = NO + NO2 + HNO3 + PAN + C1–C5alkyl nitrates) and O3 and CO were better defined in the boundary layer with significant degradation of the relationships as altitude increased. Typically, NOy,sum was enhanced over background levels of ∼260 pptv by 20-to-30-fold. The ratio C2H2/CO had values of 1–4 at altitudes up to 10 km and as far eastward as 150°E, implying significant vertical mixing of air parcels followed by rapid advection across the Pacific. Analysis air parcels originating from five principal Asian source regions showed that HNO3 and PAN dominated NOy,sum. Correlations of NOy,sum with C2Cl4 (urban tracer) were not well defined in any of the source regions, and they were only slightly better with CH3Cl (biomass tracer). Air parcels over the western Pacific contained a complex mixture of emission sources that are not easily resolvable as shown by analysis of the Shanghai mega-city plume. It contained an intricate mixture of pollution emissions and exhibited the highest mixing ratios of NOy,sum species observed during TRACE-P. Comparison of tropospheric chemistry between the earlier PEM-West B mission and the recent TRACE-P data showed that in the boundary layer significant increases in the mixing ratios of NOy,sum species have occurred, but the middle and upper troposphere seems to have been affected minimally by increasing emissions on the Asian continent over the last 7 years

Carbonyl sulfide and carbon disulfide: Large-scale distributions over the western Pacific and emissions from Asia during TRACE-P

An extensive set of carbonyl sulfide (OCS) and carbon disulfide (CS2) observations were made as part of the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) project, which took place in the early spring 2001. TRACE-P sampling focused on the western Pacific region but in total included the geographic region 110°E to 290°E longitude, 5°N to 50°N latitude, and 0–12 km altitude. Substantial OCS and CS2 enhancements were observed for a great many air masses of Chinese and Japanese origin during TRACE-P. Over the western Pacific, mean mixing ratios of long-lived OCS and shorter-lived CS2 showed a gradual decrease by about 10% and a factor of 5–10, respectively, from the surface to 8–10 km altitude, presumably because land-based sources dominated their distribution during February through April 2001. The highest mean OCS and CS2levels (580 and 20 pptv, respectively, based on 2.5° × 2.5° latitude bins) were observed below 2 km near the coast of Asia, at latitudes between 25°N and 35°N, where urban Asian outflow was strongest. Ratios of OCS versus CO for continental SE Asia were much lower compared to Chinese and Japanese signatures and were strongly associated with biomass burning/biofuel emissions. We present a new inventory of anthropogenic Asian emissions (including biomass burning) for OCS and CS2 and compare it to emission estimates based on regional relationships of OCS and CS2 to CO and CO2. The OCS and CS2 results for the two methods compare well for continental SE Asia and Japan plus Korea and also for Chinese CS2 emissions. However, it appears that the inventory underestimates Chinese emissions of OCS by about 30–100%. This difference may be related to the fact that we did not include natural sources such as wetland emissions in our inventory, although the contributions from such sources are believed to be at a seasonal low during the study period. Uncertainties in OCS emissions from Chinese coal burning, which are poorly characterized, likely contribute to the discrepancy

Adapting CALIPSO Climate Measurements for Near Real Time Analyses and Forecasting

The Cloud-Aerosol Lidar and Infrared Pathfinder satellite Observations (CALIPSO) mission was originally conceived and designed as a climate measurements mission, with considerable latency between data acquisition and the release of the level 1 and level 2 data products. However, the unique nature of the CALIPSO lidar backscatter profiles quickly led to the qualitative use of CALIPSO?s near real time (i.e., ? expedited?) lidar data imagery in several different forecasting applications. To enable quantitative use of their near real time analyses, the CALIPSO project recently expanded their expedited data catalog to include all of the standard level 1 and level 2 lidar data products. Also included is a new cloud cleared level 1.5 profile product developed for use by operational forecast centers for verification of aerosol predictions. This paper describes the architecture and content of the CALIPSO expedited data products. The fidelity and accuracy of the expedited products are assessed via comparisons to the standard CALIPSO data products

Strategies for Improved CALIPSO Aerosol Optical Depth Estimates

In the spring of 2010, the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) project will be releasing version 3 of its level 2 data products. In this paper we describe several changes to the algorithms and code that yield substantial improvements in CALIPSO's retrieval of aerosol optical depths (AOD). Among these are a retooled cloud-clearing procedure and a new approach to determining the base altitudes of aerosol layers in the planetary boundary layer (PBL). The results derived from these modifications are illustrated using case studies prepared using a late beta version of the level 2 version 3 processing code

Quantifying the Amount of Ice in Cold Tropical Cirrus Clouds

How much ice is there in the Tropical Tropopause layer, globally? How does one begin to answer that question? Clouds are currently the largest source of uncertainty in climate models, and the ice water content (IWC) of cold cirrus clouds is needed to understand the total water and radiation budgets of the upper troposphere and lower stratosphere (UT/LS). The Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, originally a "pathfinder" mission only expected to last for three years, has now been operational for more than eight years. Lidar data from CALIPSO can provide information about how IWC is vertically distributed in the UT/LS, and about inter-annual variability and seasonal changes in cloud ice. However, cloud IWC is difficult to measure accurately with either remote or in situ instruments because IWC from cold cirrus clouds is derived from the particle cross-sectional area or visible extinction coefficient. Assumptions must be made about the relationship between the area, volume and density of ice particles with various crystal habits. Recently there have been numerous aircraft field campaigns providing detailed information about cirrus ice water content from cloud probes. This presentation evaluates the assumptions made when creating the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) global IWC data set, using recently reanalyzed aircraft particle probe measurements of very cold, thin TTL cirrus from the 2006 CR-AVE