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NASA NTRS1998

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (theta about 450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(sub y)) had also been removed, with layers of enhanced (sub y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (about 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 micron) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range of theta is estimated to have been dehydrated in this event.

Hintsa, E. J.↗
NASA NTRS1998

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (0-450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(y)) had also been removed, with layers of enhanced NO(y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approximately 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 microns) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range of 0 is estimated to have been dehydrated in this event.

Hintsa, E. J.↗
NASA NTRS1999

[Global Atmospheric Chemistry/Transport Modeling and Data-Analysis]

This grant supported a global atmospheric chemistry/transport modeling and data- analysis project devoted to: (a) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for trace gases; (b) utilization of these inverse methods which use either the Model for Atmospheric Chemistry and Transport (MATCH) which is based on analyzed observed winds or back- trajectories calculated from these same winds for determining regional and global source and sink strengths for long-lived trace gases important in ozone depletion and the greenhouse effect; (c) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple "titrating" gases; and (d) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3D models. Important ultimate goals included determination of regional source strengths of important biogenic/anthropogenic trace gases and also of halocarbons restricted by the Montreal Protocol and its follow-on agreements, and hydrohalocarbons now used as alternatives to the above restricted halocarbons.

Prinn, Ronald G.↗
NASA NTRS1998

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (theta approximately 450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(y)) had also been removed, with layers of enhanced NO(y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approximately 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 micrometers) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range Transport of theta is estimated to have been dehydrated in this event.

Hintsa, E. J.↗
NASA NTRS1999

Impact of Aircraft Emissions on Reactive Nitrogen over the North Atlantic Flight Corridor Region

The impact of aircraft emissions on reactive nitrogen in the upper troposphere (UT) and lowermost stratosphere (LS) was estimated using the NO(y)-O3 correlation obtained during the SASS Ozone and NO(x) Experiment (SONEX) carried out over the US continent and North Atlantic Flight Corridor (NAFC) region in October and November 1997. To evaluate the large scale impact, we made a reference NO(y)-O3 relationship in air masses, upon which aircraft emissions were considered to have little impact. For this purpose, the integrated input of NO(x) from aircraft into an air mass along a 10-d back trajectory (DELTA-NO(y)) was calculated based on the ANCAT/EC2 emission inventory. The excess NO(y) (dNO(y)) was calculated from the observed NO(y) and the reference NO(y)-O3 relationship. As a result, a weak positive correlation was found between the dNO(y) and DELTA-NO(y), and dNO(y) and NO(x)/NO(y) values, while no positive correlation between the dNO(y) and CO values was found, suggesting that dNO(y) values can be used as a measure of the NO(x) input from aircraft emissions. The excess NO(y) values calculated from another NO(y)-O3 reference relationship made using in-situ CN data also agreed with these dNO(y) values, within the uncertainties. At the NAFC region (45 N - 60 N), the median value of dNO(y) in the troposphere increased with altitude above 9 km and reached 70 pptv (20% of NO(y)) at 11 km. The excess NO(x) was estimated to be about half of the dNO(y) values, corresponding to 30% of the observed NO(x) level. Higher dNO(y) values were generally found in air masses where O3 = 75 - 125 ppbv, suggesting a more pronounced effect around the tropopause. The median value of dNO(y) in the stratosphere at the NAFC region at 8.5 - 11.5 km was about 120 pptv. The higher dNO(y) values in the LS were probably due to the accumulated effect of aircraft emissions, given the long residence time of affected air in the LS. Similar dNO(y) values were also obtained in air masses sampled over the US continent.

Koike, M.↗
NASA NTRS1997

Nitrogen Oxides and Ozone from B-747 Measurements (NOXAR) During POLINAT-2 and SONEX: Overview and Case Studies on Continental and Marine Convection

In the framework of the project POLINAT 2 (Pollution in the North Atlantic Flight Corridor) we measured NO(x) (NO and NO2) and ozone on 85 flights through the North Atlantic Flight Corridor (NAFC) with a fully automated system permanently installed aboard an in-service Swissair B-747 airliner in the period of August to November 1997. The averaged NO(x) concentrations both in the NAFC and at the U.S. east coast were similar to that measured in autumn 1995 with the same system. The patchy occurrence of NO(x) enhancements up to 3000 pptv over several hundred kilometers (plumes), predominately found over the U.S. east coast lead to a log-normal NO(x) probability density function. In three case studies we examine the origins of such plumes by combining back-trajectories with brightness temperature enhanced (IR) satellite imagery, lightning observations from the U.S. National Lightning Detection Network (NLDN) and the Optical Transient Detector (OTD) satellite. We demonstrate that the location of NO(x) plumes can be well explained with maps of convective influence. We show that the number of lightning flashes in cluster of marine thunderstorms is proportional to the NO(x) concentrations observed several hundred kilometers downwind of the anvil outflows. From the fact that in autumn the NO(x) maximum was found several hundred kilometers off the U.S. east coast, it can be inferred that thunderstorms triggered over the warm Gulf Stream current are major sources for the regional upper tropospheric NO(x) budget in autumn.

Jeker, Dominique P.↗
NASA NTRS1999

Model Calculations of the Impact of NO(x) from Air Traffic, Lightning and Surface Emissions, Compared with Measurements

The impact of NO(x) from aircraft emissions, lightning and surface contributions on atmospheric nitrogen oxides and ozone has been investigated with the three-dimensional global chemistry transport model TM3 by partitioning the nitrogen oxides and ozone according to source category. The results have been compared with POLINAT II and SONEX airborne measurements in the North Atlantic flight corridor in 1997. Various cases have been investigated: measurements during a stagnant anti-cyclone and an almost cut-off low, both with expected high aircraft contributions, a southward bound flight with an expected strong flight corridor gradient and lightning contributions in the South, and a transatlantic flight with expected boundary layer pollution near the U.S. coast. The agreement between modeled results and measurements is reasonably good for NO and ozone. Also, the calculated impact of the three defined sources were consistent with the estimated exposure of the sampled air to these sources, obtained by specialized back-trajectory model products.

Meijer, E. W.↗
NASA NTRS1999

Impact of Aircraft Emissions on NO(x) in the Lowermost Stratosphere at Northern Midlatitudes

Airborne measurements of NO(x) total reactive nitrogen (NO(y)), O3 and condensation nuclei (CN) were made within air traffic corridors over the U.S. and North Atlantic regions (35-60 deg N) in the fall of 1997. NO(x) and NO(y) data obtained in the lowermost stratosphere (LS) were examined using the calculated increase in NO(y) ((delta)NO(y)) along five-day back trajectories as a parameter to identify possible effects of aircraft on reactive nitrogen. It is very likely that aircraft emissions had a significant impact on the NO(x) levels in the LS inasmuch as the NO(s), mixing ratios at 8.5-12 km were significantly correlated with the independent parameters of aircraft emissions, i.e., (delta)NO(y) levels and CN values. In order to estimate quantitatively the impact of aircraft emissions on NO(x), and CN, the background levels of CN and NO(x) at O3 = 100-200 ppbv were derived from the correlations of these quantities with (delta)NO(y)). On average, the aircraft emissions are estimated to have increased the NO(x) and CN values by 130 pptv and 400 STP,cc, respectively, which corresponds to 70 -/+ 30 % and 30 -/+ 20 % of the observed median values.

Kondo, Y.↗
NASA NTRS1999

Infrared Solar Spectroscopic Measurements of Free Tropospheric CO, C2H6, and HCN above Mauna Loa, Hawaii: Seasonal Variations and Evidence for Enhanced Emissions from the Southeast Asian Tropical Fires of 1997-1998

High spectral resolution (0.003 per cm) infrared solar absorption measurements of CO, C2H6, and HCN have been recorded at the Network for the Detection of Stratospheric Change station on Mauna Loa, Hawaii, (19.5N, 155.6W, altitude 3.4 km). The observations were obtained on over 250 days between August 1995 and February 1998. Column measurements are reported for the 3.4-16 km altitude region, which corresponds approximately to the free troposphere above the station. Average CO mixing ratios computed for this layer have been compared with flask sampling CO measurements obtained in situ at the station during the same time period. Both show asymmetrical seasonal cycles superimposed on significant variability. The first 2 years of observations exhibit a broad January-April maximum and a sharper CO minimum during late summer. The C2H6 and CO 3.4-16 km columns were highly correlated throughout the observing period with the C2H6/CO slope intermediate between higher and lower values derived from similar infrared spectroscopic measurements at 32'N and 45'S latitude, respectively. Variable enhancements in CO, C2H6, and particularly HCN were observed beginning in about September 1997. The maximum HCN free tropospheric monthly mean column observed in November 1997 corresponds to an average 3.4-16 km mixing ratio of 0.7 ppbv (1 ppbv = 10(exp -9) per unit volume), more than a factor of 3 above the background level. The HCN enhancements continued through the end of the observational series. Back-trajectory calculations suggest that the emissions originated at low northern latitudes in southeast Asia. Surface CO mixing ratios and the C2H6 tropospheric columns measured during the same time also showed anomalous autumn 1997 maxima. The intense and widespread tropical wild fires that burned during the strong El Nino warm phase of 1997- 1998 are the likely source of the elevated emission products.

Rinsland, C. P.↗
NASA NTRS1999

Infrared Solar Spectroscopic Measurements of Free Tropospheric CO, C2H6, and HCN above Mauna Loa, Hawaii: Seasonal Variations and Evidence for Enhanced Emissions from the Southeast Asian Fires of 1997-1998

High spectral resolution (0.003/ cm) infrared solar absorption measurements of CO, C2H6, and HCN have been recorded at the Network for the Detection of Stratospheric Change station on Mauna Loa, Hawaii, (19.5 deg N, 155.6 deg W, altitude 3.4 km). The observations were obtained on over 250 days between August 1995 and February 1998. Column measurements are reported for the 3.4 - 16 km altitude region, which corresponds approximately to the free troposphere above the station. Average CO mixing ratios computed for this layer have been compared with flask sampling CO measurements obtained in situ at the station during the same time period. Both show asymmetrical seasonal cycles superimposed on significant variability. The first two years of observations exhibit a broad January-April maximum and a sharper CO minimum during late summer. The C2H6 and CO 3.4 - 16 km columns were highly correlated throughout the observing period with the C2H6/CO slope intermediate between higher and lower values derived from similar infrared spectroscopic measurements at 32 deg N and 45 deg S latitude, respectively. Variable enhancements in CO, C2H6, and particularly HCN were observed beginning in about September 1997. The maximum HCN free tropospheric monthly mean column observed in November 1997 corresponds to an average 3.4 - 16 km mixing ratio of 0.7 ppbv (1 ppbv = 10(exp -9) per unit volume), more than a factor of 3 above the background level. The HCN enhancements continued through the end of the observational series. Back-trajectory calculations suggest that the emissions originated at low northern latitudes in southeast Asia. Surface CO mixing ratios and the C2H6 tropospheric columns measured during the same time also showed anomalous autumn 1997 maxima. The intense and widespread tropical wild fires that burned during 3 the strong El Nino warm phase of 1997-1998 are the likely source of the elevated emission products.

Rinsland, C. P.↗
NASA NTRS1999

Processes Affecting Tropospheric Ozone Inferred from Ozonesonde and Other Tracer Data from the R/V R H Brown Atlantic Cruise (37N-34S) in January-February 1999

During the Aerosols-99 trans-Atlantic cruise from Norfolk, VA, to Cape Town, South Africa, 22 ozonesondes were launched from the NOAA R/V R H Brown between 17 Jan and 6 Feb 1999, with all sondes but one reaching 30 km. A composite of ozone profiles along the transect shows high free tropospheric ozone (up to 100 ppbv at 9 km) between 5N and 20S, a coherent feature straddling either side of the ITCZ. Latitudinal variations of tropospheric ozone are interpreted using correlative measurements of surface ozone, CO, water vapor, and aerosol optical thickness (column absorbance) measured from the ship. Elevated ozone in the lower troposphere results from photochemical reactions of precursors emitted by biomass burning north of the ITCZ. However, the greatest ozone mixing ratios are in the mid-troposphere south of the ITCZ, which gives evidence of interhemispheric transport. Column-integrated tropospheric ozone, 35 DU from 0-16 km, agrees with that derived from the TOMS satellite by the modified-residual method [Thompson and Hudson, 1999]. NCEP wind fields, ship-launched radiosondes and back trajectories are consistent with a picture of recirculating air parcels centered in the tropical Atlantic region which is identified with the maximum wave-one amplitude in total ozone seen in sondes and by satellite.

Thompson, Anne M.↗
NASA NTRS1999

Shipboard and Satellite Views of Elevated Tropospheric Ozone over the Tropical Atlantic in January-February 1999

During the Aerosols99 trans-Atlantic cruise from Norfolk, VA, to Cape Town, South Africa, daily ozonesondes were launched from the NOAA R/V Ronald H Brown between 17 January and 6 February l999. A composite of tropospheric ozone profiles along the latitudinal transect shows 4 zones, which are interpreted using correlative shipboard ozone, CO, water vapor, and overhead aerosol optical thickness measurements. Elevated ozone associated with biomass burning north of the ITCZ (Intertropical Convergence Zone) is prominent at 3-5 km from 10-0N, but even higher ozone (100 ppbv, 7-10 km) occurred south of the ITCZ, where it was not burning. Column-integrated tropospheric ozone was 44 Dobson Units (DU) in one sounding, 10 DU lower than the maximum in a January-February 1993 Atlantic cruise with ozonesondes [Weller et al., 1996]. TOMS tropospheric ozone shows elevated ozone extending throughout the tropical Atlantic in January 1999. Several explanations are considered. Back trajectories, satellite aerosol observations and shipboard tracers suggest a combination of convection and interhemispheric transport of ozone and/or ozone precursors, probably amplified by a lightning NO source over Africa.

Thompson, Anne M.↗
NASA NTRS1999

Biomass Burning Influences on the Composition of the Remote South Pacific Troposphere: Analysis Based on Observations from PEM Tropics-A

Airborne, in-situ measurements from PEM-Tropics-A (September/October 1996) are analyzed to show the presence of distinct pollution plumes in the middle-tropical troposphere of the remote South Pacific (10-30degS). These elevated plumes cause a relative maximum at about 5-7km attitude in the vertical distribution of primary and secondary species characteristic of fuel combustion and biomass burning (CO, C2H2, C2H6, CH3Cl, PAN, O3). Similar plumes were also observed at mid-latitudes in the middle troposphere during three flights east of New Zealand (40-45degS). In all, pollution plumes with CO larger than 100 ppb were observed 24 times on 7 separate flight days south of the equator. The observed plumes were generally embedded in very dry air. Ten-day back trajectory analysis supports the view that these originated from the biomass burning regions of South Africa (and South America) and were transported to the South Pacific along long-distance subsiding trajectories. The chemical composition of the southern Pacific troposphere analyzed from the PEM-Tropics-A data is compared with data from the tropical regions of the northern Pacific (PEM-West-A) and southern Atlantic (TRACE-A) during the same Sept/Oct time period. Sizable perturbations in the abundance of ozone and its key precursors, resulting from the transport of pollution originating from biomass burning sources, are observed in much of the Southern Hemispheric troposphere.

Singh, H. B.↗
NASA NTRS2001

Summer Antarctic Ozone Behavior and Laminae

The ADEOS/ILAS solar occultation instrument measured the vertical distribution of ozone during the southern polar summer of 1997. A range of latitudes was sampled from 65 to 79 degrees south. Ozone profiles are characterized by laminae, which are confined to the 20 to 50 mb pressure altitude region. For a single day not all longitudes exhibit such structures. Using back trajectory calculations, it is shown that laminae are caused by lower latitude air being transported toward the pole by winds in the 20 to 50 mb region. These winds are not present above this pressure region. The existence of such structures implies that other constituents must also be transported by the winds. Other constituent distributions will be examined to determine the extent to which they are affected by wind transport. The effects on the TOMS total ozone distributions are also examined.

Aikin, A. C.↗
NASA NTRS1998

Dehydration and Denitrification in the Arctic Polar Vortex During the 1995-1996 Winter

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (theta = 450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NOy) had also been removed, with layers of enhanced NOy at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approx. 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 micrometers) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range of theta is estimated to have been dehydrated in this event.

Hintsa, E. J.↗
NASA NTRS2000

Aerosol Radiative Forcing in Asian Continental Outflow

Aerosols in elevated layers were sampled with FSSP-probes and wire impactors over the Pacific ocean aboard the NASA DC-8 aircraft. Analyses of particle size and morphology identifies two distinctly different aerosol types for cases when the mid-visible extinctions exceed 0.2/km. Smaller sizes (effective radii of 0.2 um) and moderate absorption (mid-visible single scattering albedo of.935) are typical for urban-industrial pollution. Larger sizes (effective radii of 0.7 um) and weak absorption (mid-visible single scattering albedo of 0.985) identify dust. This aerosol classification is in agreement with its origin as determined by airmass back trajectory analysis. Based on lidar vertical profiling, aerosol dominated by dust and urban-industrial pollution above 3km were assigned mid-visible optical depths of 0.50 and 0.27, respectively. Radiative transfer simulations, considering a 50% cloud-cover below the aerosol layers, suggest (on a daily tP C)C> basis) small reductions (-4W/m2) to the energy budget at the top of the atmosphere for both aerosol types. For c' 0 dust, more backscattering of sunlight (weaker solar absorption) is compensated by a stronger greenhouse effect due to larger sizes. Forced reductions to the energy budget at the surface are 12W/m2 for both aerosol types. In contrast, impacts on heating rates within the aerosol layers are quite different: While urban-industrial aerosol warms the layer (at +0.6K/day as solar heating dominates), dust cools (at -0.5K/day as infrared cooling dominates). Sensitivity tests show the dependence of the aerosol climatic impact on the optical depth, particle size, absorptivity, and altitude of the layers, as well as clouds and surface properties. Climatic cooling can be eliminated (1) for the urban-industrial aerosol if absorption is increased to yield a mid-visible single scattering albedo of 0.89, or if the ocean is replaced by a land surface; (2) for the dust aerosol if the effective radius is increased from 0.7 to 1.2 um. The removal of low-level clouds doubles the cooling at the top of the atmosphere to about -8W/m2.

Pueschel, R.↗
NASA NTRS2001

Photolysis Rate Coefficient Calculations in Support of SOLVE Campaign

The objectives for this SOLVE project were 3-fold. First, we sought to calculate a complete set of photolysis rate coefficients (j-values) for the campaign along the ER-2 and DC-8 flight tracks. En route to this goal, it would be necessary to develop a comprehensive set of input geophysical conditions (e.g., ozone profiles), derived from various climatological, aircraft, and remotely sensed datasets, in order to model the radiative transfer of the atmosphere accurately. These j-values would then need validation by comparison with flux-derived j-value measurements. The second objective was to analyze chemistry along back trajectories using the NASA/Goddard chemistry trajectory model initialized with measurements of trace atmospheric constituents. This modeling effort would provide insight into the completeness of current measurements and the chemistry of Arctic wintertime ozone loss. Finally, we sought to coordinate stellar occultation measurements of ozone (and thus ozone loss) during SOLVE using the Midcourse Space Experiment(MSX)/Ultraviolet and Visible Imagers and Spectrographic Imagers (UVISI) satellite instrument. Such measurements would determine ozone loss during the Arctic polar night and represent the first significant science application of space-based stellar occultation in the Earth's atmosphere.

Lloyd, Steven A.↗
NASA NTRS2001

Evidence of Stratosphere-to-Troposphere Transport Within a Mesoscale Model and TOMS Total Ozone

We present evidence for stratospheric mass transport into, and remaining in, the troposphere in an intense midlatitude cyclone. Mesoscale forecast model analysis fields from the Mesoscale Analysis and Prediction System (MAPS) were compared with total ozone observations from the Total Ozone Measurement Spectrometer (TOMS). Coupled with parcel back-trajectory calculations, the analyses suggest two mechanisms contributed to the mass exchange: (1) A region of dynamical ly-induced exchange occurred on the cyclone's southern edge. Parcels originally in the stratosphere crossed the jet core and experienced dilution by turbulent mixing with tropospheric air. (2) Diabatic effects reduced parcel potential vorticity (PV) for trajectories traversing precipitation regions, resulting in a "PV-hole" signature in the cyclone center. Air with lower-stratospheric values of ozone and water vapor was left in the troposphere. The strength of the latter process may be atypical. These results, combined with other research, suggest that precipitation-induced diabatic effects can significantly modify, (either decreasing or increasing) parcel potential vorticity, depending on parcel trajectory configuration with respect to jet core and maximum heating regions. In addition, these results underscore the importance of using not only PV but also chemical constituents for diagnoses of stratosphere-troposphere exchange (STE).

Olsen, Mark A.↗