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NASA NTRS2018

Ocean Circulation Causes Strong Variability in the Mid-Atlantic Bight Nitrogen Budget

Understanding of nitrogen cycling on continental shelves, a critical component of global nutrient cycling, is hampered by limited observations compared to the strong variability on a wide range of time and space scales. Numerical models have the potential to partially alleviate this issue by filling spatio-temporal data gaps and hence resolving annual area-integrated nutrient fluxes. In this study, a three-dimensional bio geo chemical-circulation model was implemented to simulate the Mid-Atlantic Bight (MAB) nitrogen budget. Model results demonstrate that, on average, MAB net community production (NCP) was positive (plus 0.27 teragrams (Tg) Nitrogen per year), indicating net autotrophy. Inter-annual variability in NCP was strong, with annual values ranging between 0.19 and 0.41 Tg N/year. Along-shelf and across-shelf horizontal transport fluxes were the other dominant terms in the nitrogen budget and were primarily responsible for this NCP variability. The along-shelf current transported nitrogen from the north (0.65 Tg N/year) into the MAB, supplementing the nitrogen entering from terrestrial inputs (0.27 Tg N/year). However, NCP was highest in the year when total water volume transport and inorganic nitrogen input was strongest across the continental slope in the southern MAB, rather than when terrestrial inputs were greatest. Inter-annual variability of NCP appears to be linked to changes in the positions of the Gulf Stream and Slope Water Gyre. Overall, the strong spatio temporal variability of the nitrogen fluxes highlights the importance of observations throughout all seasons and multiple years in order to accurately resolve the current status and future changes of the MAB nitrogen budget.

Friedrichs, Marjorie A. M.↗
NASA NTRS1985

LIMS data - Inferred stratospheric distribution of NOx and HOx trace constituents and the calculated odd nitrogen budget

LIMS, SAMS, SBUV and in-situ data have been used to infer species not measured but which are of photochemical interest, e.g., O(3P), O(1D), NO, N2O5, OH, HO2, ClO and HCl. (LIMS = limb infrared monitor of the stratosphere; SAMS = stratospheric and mesospheric sounder; and SBUV = solar backscattered ultraviolet instrument.) Production and loss of odd nitrogen have been calculated and estimates have been made of the odd nitrogen transport due to adiabatically driven circulation derived from LIMS data. Data used from LIMS include O3, NO2, HNO3, H2O and T. CH4 and N2O were taken from SAMS and the UV solar flux from the SBUV instrument. Species were inferred for periods in October, December, March and May. Results for December are discussed. Results indicate: (1) maximum stratospheric odd nitrogen levels of 25 ppbv; (2) evidence of odd nitrogen transport from the mesosphere appearing at 25 km in the wintertime polar latitudes; (3) the polar night build-up of high levels of N2O5 beginning after the autumnal equinox; and (4) the possibility of large downward fluxes of odd nitrogen into the troposphere during the winter at latitudes poleward of 60 degrees.

Callis, L. B.↗
NASA NTRS2007

Chemical Data Assimilation Estimates of Continental US Ozone and Nitrogen Budgets during INTEX-A

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 US during the July-August 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during the INTEX-A show that RAQMS captures the main features of the global and Continental US 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 US 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 US 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 percent, with NOx+PAN accounting for 54 percent of the total NOy export during INTEX-A.

Pierce, Robert B.↗
NASA NTRS1990

Biomass production and nitrogen dynamics in an integrated aquaculture/agriculture system

A combined aquaculture/agriculture system that brings together the three major components of a Controlled Ecological Life Support System (CELSS) - biomass production, biomass processing, and waste recycling - was developed to evaluate ecological processes and hardware requirements necessary to assess the feasibility of and define design criteria for integration into the Kennedy Space Center (KSC) Breadboard Project. The system consists of a 1 square meter plant growth area, a 500 liter fish culture tank, and computerized monitoring and control hardware. Nutrients in the hydrophonic solution were derived from fish metabolites and fish food leachate. In five months of continuous operation, 27.0 kg of lettuce tops, 39.9 kg of roots and biofilm, and 6.6 kg of fish (wet weights) were produced with 12.7 kg of fish food input. Based on dry weights, a biomass conversion index of 0.52 was achieved. A nitrogen budget was derived to determine partitioning of nitrogen within various compartments of the system. Accumulating nitrogen in the hypoponic solution indicated a need to enlarge the plant growth area, potentially increasing the biomass production and improving the biomass conversion index.

Owens, L. P.↗
NASA NTRS1990

Stratospheric constituent distributions from balloon-based limb thermal emission measurements

This research task deals with an analysis of infrared thermal emission observations of the Earth's atmosphere for determination of trace constituent distributions. Infrared limb thermal emission spectra in the 700-2000 cm(exp -1) region were obtained with a liquid nitrogen cooled Michelson interferometer-spectrometer (SIRIS) on a balloon flight launched from Palestine, Texas, at nighttime on September 15-16, 1986. An important objective of this work is to obtain simultaneously measured vertical mixing ratio profiles of O3, H2O, N2O, NO2, N2O5, HNO3 and ClONO2 and compare with measurements made with a variety of techniques by other groups as well as with photochemical model calculations. A portion of the observed spectra obtained by SIRIS from the balloon flight on September 15-16, 1986, has been analyzed with a focus on calculation of the total nighttime odd nitrogen budget from the simultaneously measured profiles of important members of the NO(sub x) family. The measurements permit first direct determination of the nighttime total odd nitrogen concentrations NO(sub y) and the partitioning of the important elements of the NO(sub x) family.

Abbas, Mian M.↗
NASA NTRS1994

Summertime distribution of PAN and other reactive nitrogen species in the northern high-latitude atmosphere of eastern Canada

Aircraft measurements of key reactive nitrogen species (NO, NO2, HNO3, PAN, PPN, NO3(-), NO(y)), C1 to C6 hydrocarbons, acetone, O3, chemical tracers (C2Cl4, CO), and important meteorological parameters were performed over eastern Canada during July to August 1990 at altitudes between 0 and 6 km as part of an Arctic Boundary Layer Expedition (ABLE3B). In the free troposphere, PAN was found to be the single most abundant reactive nitrogen species constituting a major fraction of NO(y) and was significantly more abundant than NO(x) and HNO3. PAN and O3 were well correlated both in their fine and gross structures. Compared to data previously collected in the Arctic/subarctic atmosphere over Alaska (ABLE3A), the lower troposphere (0-4 km) over eastern Canada was found to contain larger reactive nitrogen and anthropogenic tracer concentrations. At higher altitudes (4-6 km) the atmospheric composition was in many ways similar to what was seen over Alaska and supports the view that a large-scale reservoir of PAN (and NO(y)) is present in the upper troposphere over the entire Arctic/subarctic region. The reactive nitrogen budget based on missions conducted from the North Bay site (missions 2-10) showed a small shortfall, whereas the budget for data collected from the Goose Bay operation (missions 11-19) showed essential balance. It is calculated that 15-20 ppt of the observed NO(x) may find its source from the available PAN reservoir. Meteorological considerations as well as relationships between reactive nitrogen and tracer species suggest that the atmosphere over eastern Canada during summer is greatly influenced by forest fires and transported industrial pollution.

Singh, H. B.↗
NASA NTRS1979

The influence of ionization events on atmospheric ozone

Atmospheric ionization events can modify the concentration of neutral species in the stratosphere and mesosphere. In particular, ozone is destroyed because of the production of significant quantities of odd nitrogen and hydrogen compounds which react photochemically to destroy ozone. Direct evidence of ozone depletion comes from data taken during and following two solar flares generating large fluxes of 10-100 Mev protons, which bombarded the polar stratosphere and mesosphere. Observations of ozone taken during X-ray emission by solar flares and energetic electron precipitation during aurorae indicates ozone destruction above 50 km by ionization produced odd hydrogen. Lightning is apparently a large contributor to the tropospheric odd nitrogen budget. Ion propulsion induced dumping of the inner proton radiation belt represents a human activity which may influence stratospheric NOx.

Aikin, A. C.↗
NASA NTRS1978

Tropospheric ozone

Photochemical equilibrium models have been used to study the effect of recent revisions in important chemical reaction rates on the calculated tropospheric ozone concentration. Reasonable agreement with observed values is obtained if the NO(x) background is approximately 0.02 to 0.03 ppb, about an order of magnitude less than used in many previous model studies, but consistent with present nitrogen budget considerations and with observations of NO2. Chemical production and loss of ozone may dominate transport terms depending on values of key chemical rate constants and of the NO(x) background. This is consistent with the structure observed in the mean annual latitudinal distribution of ozone since ozone is its own chemical precursor and regions of enhanced stratosphere-troposphere exchange are also regions of enhanced photochemical activity.

Stewart, R. W.↗
NASA NTRS1983

The photochemistry of anthropogenic nonmethane hydrocarbons in the troposphere

A lumped, nonmethane hydrocarbon (NMHC) chemical mechanism is presently applied to a one-dimensional photochemical model of the troposphere. The profiles of OH, HO2, NO(x), and HNO3, showed only slight changes when NMHC chemistry was added. The integrated column of peroxyacetylnitrate (PAN), when NMHC chemistry was included, comprised 17 percent of the odd nitrogen budget. Advection is noted as an important possible mechanism for the removal of PAN at midlatitudes. The inclusion of such intermediate lifetime species as aldehydes and olefins has both provided additional sources of short-lived NMHC radicals, such as the peroxyacetyl radical that is the radical precursor of PAN, and offered a more detailed description of the concentrations of short-lived species and the overall NMHC chemistry.

Brewer, D. A.↗
NASA NTRS1991

Nighttime reactive nitrogen measurements from stratospheric infrared thermal emission observations

IR thermal emission spectra of the earth's atmosphere in the 700-2000/cm region were obtained with a cryogenically cooled high-resolution interferometer spectrometer on a balloon flight from Palestine, Texas, on September 15-16, 1986. The observations exhibit spectral features of a number of stratospheric constituents, including important species of the reactive nitrogen family. An analysis of the observed data for simultaneously measured vertical distributions of O3, H2O, N2O, NO2, N2O5, HNO3, and ClONO2 is presented. These measurements permit the first direct determination of the nighttime total reactive nitrogen concentrations, and the partitioning of the important elements of the NO(x) family. Comparisons of the total reactive nitrogen budget are made with the measurements by the ATMOS experiment and with the predictions of one-dimensional and two-dimensional photochemical models.

Abbas, Mian M.↗
NASA NTRS1990

Diagnostic studies of the HxOy-NxOy-O3 photochemical system using data from NASA GTE field expeditions

The research effort supported in part by the subject grant focused on three related topics. Our major effort was concentrated on the analysis of data gathered during GTE field expeditions. Ancillary efforts were directed at: the development and application of a Global Chemical Transport Model for the study of the atmospheric reactive nitrogen budget; the development and application of a one-dimensional, time dependent cloud model for the study of the impact of in-cloud aqueous phase chemistry on the atmospheric sulfur budget; and mechanistic studies of the chemical processes involved in dry deposition of ozone to vegetative surfaces. In the sections below, we briefly summarize the central conclusions of each of these efforts. These discussions are followed by a listing of the papers completed during the granting period and the graduate students supported by funds from the grant. Reprints and preprints of all papers completed with support from the grant are attached as appendices.

Chameides, W. L.↗
NASA NTRS1994

Summertime distribution and relations of reactive odd nitrogen species and NO(y) in the troposphere over Canada

We report here large-scale features of the distribution of NO(x), HNO3, PAN, particle NO3, and NO(y) in the troposphere from 0.15 to 6 km altitude over central Canada. These measurements were conducted in July - August 1990 from the NASA Wallops Electra aircraft as part of the joint United States-Canadian Arctic Boundary Layer Expedition (ABLE) 3B-Northern Wetlands Study. Our findings show that this region is generally NO(x) limited, with NO(x) mixing ratios typically 20-30 parts per trillion by volume (pptv). We found little direct evidence for anthropogenic enhancement of mixing ratios of reactive odd nitrogen species and NO(y) above those in 'background' air. Instead, it appears that enhancements in the mixing ratios of these species were primarily due to emissions from several day old or CO-rich-NO(x)-poor smoldering local biomass-burning fires. NO(x) mixing ratios in biomass-burning impacted air masses were usually less than 50 pptv, but those of HNO3 and PAN were typically 100-300 pptv representing a twofold-threefold enhancement over 'background' air. During our study period, inputs of what appeared to be aged tropical air were a major factor influencing the distribution of reactive odd nitrogen in the midtroposphere over northeastern North America. These air masses were quite depleted in NO(y) (generally less than 150 pptv), and a frequent summertime occurrence of such air masses over this region would imply a significant influence on the reactive odd nitrogen budget. Our findings show that the chemical composition of aged air masses over subarctic Canada and those documented in the Arctic during ABLE 3A have strikingly similar chemistries, suggesting large-scale connection between the air masses influencing these regions.

Talbot, R. W.↗
NASA NTRS1997

Upper Tropospheric/Lower Stratospheric Distribution of Reactive Nitrogen and Ozone

In-situ measurements of a large number of trace chemicals from upper troposphere/lower stratosphere (UT/LS) were performed with the NASA DC-8 aircraft during February/March 1994 over the Pacific Ocean (10 S to 60 N). Mixing ratios in the UT were relatively low in the warm tropical and subtropical air south of the polar jetstream (approx. =28 N) but increased sharply with latitude in the cold polar air north of the jetstream. At about 45 N, high concentrations of PAN (300 ppt) coexisted with extremely low (approx. = 20 ppt) concentrations of NOx. Elevated NOx levels in the UT did not always correspond to continental outflow conditions. Deepest penetrations into the stratosphere (550 ppb O3, 279 ppb NOx, and 350 K potential temperature) corresponded to a region that has been defined as the 'lowermost stratosphere' (LS) by Holton et al. Analysis of data shows that the mixing ratios of long-lived tracer species (e.g., CH4, HNO3, NOy, CFCs, HCFCs) are linearly correlated with those of O3 and N2O. A delta-NOY/delta-O3 of 0.0054 ppb/ppb and delta-NOy/delta-N2O of -0.081 ppb/ppb is in good agreement with other reported measurements from the DC-8. These slopes are however, somewhat steeper than those reported from the ER-2 studies. We find that the reactive nitrogen budget in the UT/LS is largely balanced with shortfalls that are no greater than 15%. A number of oxygenated species (e.g., acetone, H2O2) are present and may provide an important in-situ source of HOx in the UT/LS region.

Singh, H. S.↗
NASA NTRS1992

Relationship of peroxyacetyl nitrate to active and total odd nitrogen at northern high latitudes: influence of reservoir species on NOx and O3

Measurements of peroxyacetyl nitrate (PAN), NO, NO2, HNO3, NOy (total odd nitrogen), and O3 were made in the high-latitude troposphere over North America and Greenland (35 degrees to 82 degrees N) during the Arctic Boundary Layer Expedition (ABLE 3A) (July-August 1988) throughout 0-to 6-km altitudes. These data are analyzed to quantitatively describe the relationships between various odd nitrogen species and assess their significance to global tropospheric chemistry. In the free troposphere, PAN was as much as 25 times more abundant than NOx. PAN to NOx ratio increased with increasing altitude and latitude. PAN was found to be the single most abundant reactive nitrogen species in the free troposphere and constituted a major fraction of NOy, PAN to NOy ratios were about 0.1 in the boundary layer and increased to 0.4 in the free troposphere. A 2-D global photochemical model with C1-C3 hydrocarbon chemistry is used to compare model predictions with measured results. A sizable portion (approximately 50%) of the gaseous reactive nitrogen budget is unaccounted for, and unknown organic nitrates and pernitrates are expected to be present. Model calculations (August 1, 70 degrees N) show that a major fraction of the observed NOx (50 to 70% of median) may find its source in the available PAN reservoir. PAN and the unknown reservoir species may have the potential to control virtually the entire NOx availability of the high latitude troposphere. It is predicted that the summer NOx and O3 mixing ratios in the Arctic/sub-Arctic troposphere would be considerably lower in the absence of the ubiquitous PAN reservoir. Conversely, this PAN reservoir may be responsible for the observed temporal increase in tropospheric O3 at high latitudes.

NASA Center ARC↗
NASA NTRS2016

Interdecadal Trichodesmium Variability in Cold North Atlantic Waters

Studies of the nitrogen cycle in the ocean generally assume that the distribution of the marine diazotroph, Trichodesmium, is restricted to warm, tropical, and subtropical oligotrophic waters. Here we show evidence that Trichodesmium are widely distributed in the North Atlantic. We report an approximately vefold increase during the 1980s and 1990s in Trichodesmium presence near the British Isles with respect to the average over the last 50 years. A potential explanation is an increase in the Saharan dust source starting in the 1980s, coupled with changes in North Atlantic winds that opened a pathway for dust transport. Results from a coarse-resolution model in which winds vary but iron deposition is climatologically fixed suggest frequent nitrogen limitation in the region and reversals of the Portugal current, but it does not simulate the observed changes in Trichodesmium. Our results suggest that Trichodesmium may be capable of growth at temperatures below 20C and challenge assumptions about their latitudinal distribution. Therefore, we need to reevaluate assumptions about the temperature limitations of Trichodesmium and the dinitrogen (N2) xation capabilities of extratropical strains, which may have important implications for the global nitrogen budget.

Rivero-Calle, Sara↗
NASA NTRS1990

Budgets of reactive nitrogen, hydrocarbons, and ozone over the Amazon forest during the wet season

The atmospheric composition over the Amazon forest during the wet season is simulated with a one-dimensional photochemical model for the planetary boundary layer (PBL) extending from the ground to 2000-m altitude. The model is constrained and evaluated using observations from the Amazon Boundary Layer Experiment 2B field expedition. Results indicate that only about 20 percent of NO(x) emitted by soils is exported to the atmosphere above the forest canopy. The balance is deposited to vegetation before leaving the canopy layer. The small NO(x) flux that escapes from the canopy is nevertheless sufficient to account for the low NO concentrations observed in the PBL. Soil emission can account for only a portion of NO(y) observed over the forest. Organic nitrates of nonbiogenic origin likely account for the balance of NO(y). Enhancements of CO observed in the PBL appear to reflect direct emission of CO by the forest ecosystem. Concentrations of O3 in the PBL are regulated largely by transport from aloft and deposition to the canopy, with little net influence from photochemistry. Ozone is photochemically produced immediately above the forest where NO concentrations are relatively high, but is photochemically consumed in the upper portion of the PBL.

Jacob, Daniel J.↗
NASA NTRS1983

Nitrogen oxides in the troposphere - Global and regional budgets

The cycle of nitrogen oxides in the troposphere is discussed from both global and regional perspectives. Global sources for NO(x) are estimated to be of magnitude 50 (+ or - 25) x 10 to the 12th gm N/yr. Nitrogen oxides are derived from combustion of fossil fuels (40 percent) and biomass burning (25 percent) with the balance from lightning and microbial activity in soils. Estimates for the rate of removal of NOx based on recent atmospheric and precipitation chemistry data are consistent with global source strengths derived here. Industrial and agricultural activities provide approximately two thirds of the global source for NOx. In North America, sources from combustion of fossil fuels exceed natural sources by a factor of 3-13. Wet deposition removes about one third of the combustion source of NOx over North America, while dry deposition removes a similar amount. The balance is exported from the continent. Deposition of nitrate in precipitation over eastern Canada and the western Atlantic is clearly influenced by sources of NOx in the eastern United States.

Logan, J. A.↗
NASA NTRS1999

Measurements of Nitric Acid and Aerosol Species Aboard the NASA DC-8 Aircraft During the SASS Ozone and Nitrogen Oxide Experiment (SONEX)

The SASS Ozone and Nitrogen Oxides Experiment (SONEX) over the North Atlantic during October/November 1997 offered an excellent opportunity to examine the budget of total reactive nitrogen (NO(sub y)) in the upper troposphere (8 - 12 km altitude). The median measured NO(sub y) mixing ratio was 425 parts per trillion by volume (pptv). Two different methods were used to measure HNO3: (1) the mist chamber technique and, (2) chemical ionization mass spectrometry. Two merged data sets using these HNO3 measurements were used to calculate NO(sub y) by summing the reactive nitrogen species (a combination of measured plus modeled results) and comparing the resultant values to measured NO(sub y) (gold catalytic reduction method). Both comparisons showed good agreement in the two quantities (slope > 0.9 and r(exp 2) > 0.9). Thus, the total reactive nitrogen budget in the upper troposphere over the North Atlantic can be explained in a general manner as a simple mixture of NO(sub x). (NO + NO2), HNO3, and PAN. Median values of NO(sub x)/NO(sub y) were approximately equal to 0.25, HNO3/NO(sub y) were approximately equal to 0.35 and Peroxyacetyl Nitrate (PAN)/NO(sub y) were approximately equal to 0. 17. Particulate NO3 and alkyl nitrates together composed <10 % of NO(sub y), while model estimated HNO4 averaged 12%.

Talbot, Robert W.↗