Technical note: a new method for the Lagrangian tracking of pollution plumes from source to receptor using gridded model output

Lagrangian particle dispersion models (LPDMs) are powerful and popular tools used for the analysis of atmospheric trace gas measurements. However, it can be difficult to determine the transport pathway of emissions from their source to a receptor using the standard gridded model output, particularly during complex meteorological scenarios. In this paper we present a method to clearly and easily identify the pathway taken by only those emissions that arrive at a receptor at a particular time, by combining the standard gridded output from forward (e.g., concentration) and backward (e.g., residence time) LPDM simulations. By comparing the pathway determined from this method with particle trajectories from both the forward and backward models, we show that this method successfully restores much of the Lagrangian information that is lost when the data are gridded. A sample analysis is presented, demonstrating that the sourceto-receptor pathway determined from this method is more accurate and easier to use than existing methods using standard LPDM products (gridded fields of, e.g., concentrations and residence time). As demonstrated in an evaluation and an example application, the method requires agreement between the transport described by the forward and backward simulations and thus provides a means to assess the quality and reversibility of the simulation. Finally, we discuss the potential for combining the backward LPDM simulation with gridded data from other sources (e.g., chemical transport models) to obtain a Lagrangian sampling of the air that will eventually arrive at a receptor. Based on the advantages presented here, this new method can complement or even replace many of the standard uses of backward LPDM simulations

Release of NO(x) from sunlight-irradiated midlatitude snow

Photochemical production and release of gas-phase NO(x) (NO + NO2) from the natural snowpack at a remote site in northern Michigan were investigated during the Snow Nitrogen and Oxidants in Winter study in January 1999. Snow was collected in an open 34 L chamber, which was then sealed with a transparent Teflon cover and used as an outdoor flow and reaction chamber. Significant increases in NO(x) mixing ratio were observed in synthetic and ambient air pulled through the sunlit chamber. [NO(x)] enhancements were correlated to ultraviolet sunlight intensity, reaching ~300 pptv under partially overcast midday, mid-winter conditions. These findings are consistent with NO(x) production from photolysis of snowpack NO3 -; the observed NO(x) release implies production of significant amounts of OH within the snow. Snowpack NO3 - photolysis may therefore significantly alter boundary layer levels of both NO(x) and oxidized compounds over wide regions of the atmosphere

Multibody aircraft study, volume 2

The potential benefits of a multibody aircraft when compared to a single body aircraft are presented. The analyses consist principally of a detailed point design analysis of three multibody and one single body aircraft, based on a selected payload of 350,000 kg (771,618 lb), for final aircraft definitions; sensitivity studies to evaluate the effects of variations in payload, wing semispan body locations, and fuel price; recommendations as to the research and technology requirements needed to validate the multibody concept. Two, two body, one, three body, and one single body aircraft were finalized for the selected payload, with DOC being the prime figure of merit. When compared to the single body, the multibody aircraft showed a reduction in DOC by as much as 11.3 percent. Operating weight was reduced up to 14 percent, and fly away cost reductions ranged from 8.6 to 13.4 percent. Weight reduction, hence cost, of the multibody aircraft resulted primarily from the wing bending relief afforded by the bodies being located outboard on the wing

Late summer changes in burning conditions in the boreal regions and their implications for NO x and CO emissions from boreal fires

Copyright © 2008 American Geophysical Union. All Rights Reserved.Building emission inventories for the fires in boreal regions remains a challenging task with significant uncertainties in the methods used. In this work, we assess the impact of seasonal trends in fuel consumption and flaming/smoldering ratios on emissions of species dominated by flaming combustion (e.g., NO x ) and species dominated by smoldering combustion (e.g., CO). This is accomplished using measurements of CO and NO y at the free tropospheric Pico Mountain observatory in the central North Atlantic during the active boreal fire seasons of 2004 and 2005. ΔNO y /ΔCO enhancement ratios in aged fire plumes had higher values in June-July (7.3 × 10−3 mol mol−1) relative to the values in August-September (2.8 × 10−3 mol mol−1), indicating that NO x /CO emission ratios declined significantly as the fire season progressed. This is consistent with our understanding that an increased amount of fuel is consumed via smoldering combustion during late summer, as deeper burning of the drying organic soil layer occurs. A major growth in fuel consumption per unit area is also expected, due to deeper burning. Emissions of CO and NO x from North American boreal fires were estimated using the Boreal Wildland Fire Emissions Model, and their long-range transport to the sampling site was modeled using FLEXPART. These simulations were generally consistent with the observations, but the modeled seasonal decline in the ΔNO y /ΔCO enhancement ratio was less than observed. Comparisons using alternative fire emission injection height scenarios suggest that plumes with the highest CO levels at the observatory were lofted well above the boundary layer, likely as a result of intense crown fires

A semi-Lagrangian view of ozone production tendency in North American outflow in the summers of 2009 and 2010

The Pico Mountain Observatory, located at 2225 m a.s.l. in the Azores Islands, was established in 2001 to observe long-range transport from North America to the central North Atlantic. In previous research conducted at the observatory, ozone enhancement (\u3e 55 ppbv) in North American outflows was observed, and efficient ozone production in these outflows was postulated. This study is focused on determining the causes for high d[O3] / d[CO] values (~1 ppbv ppbv−1) observed in the summers of 2009 and 2010. The folded retroplume technique, developed by Owen and Honrath (2009), was applied to combine upwind FLEXPART transport pathways with GEOS-Chem chemical fields. The folded result provides a semi-Lagrangian view of polluted North American outflow in terms of physical properties and chemical processes, including production/loss rate of ozone and NOx produced by lightning and thermal decomposition of peroxy acetyl nitrate (PAN). Two transport events from North America were identified for detailed analysis. High d[O3] / d[CO] was observed in both events, but due to differing transport mechanisms, ozone production tendency differed between the two. A layer of net ozone production was found at 2 km a.s.l. over the Azores in the first event plume, apparently driven by PAN decomposition during subsidence of air mass in the Azores–Bermuda High. In the second event, net ozone loss occurred during transport in the lower free troposphere, yet observed d[O3] / d[CO] was high. We estimate that in both events, CO loss through oxidation contributed significantly to d[O3] / d[CO] enhancement. Thus, it is not appropriate to use CO as a passive tracer of pollution in these events. In general, use of d[O3] / d[CO] as an indicator of net ozone production/loss may be invalid for any situation in which oxidants are elevated. Based on our analysis, use of d[O3] / d[CO] to diagnose ozone enhancement without verifying the assumption of negligible CO loss is not advisable

Kinetics of isothermal and non-isothermal precipitation in an Al-6at%Si alloy

A novel theory which describes the progress of a thermally activated reaction under isothermal and linear heating conditions is presented. It incorporates nucleation, growth and impingement and takes account of temperaturedependent solubility. The model generally fits very well to isothermal calorimetry and differential scanning calorimetry data on precipitation in an Al-6 at.% Si alloy. Analysis of the data shows that two processes occur in this precipitation reaction: growth of large Si particles and growth of pre-existing small nuclei. Determination of the sizes of Si precipitates by transmission electron microscopy indicates that interfacial energy contributions are small and have a negligible influence on solubilit

An overview of snow photochemistry: Evidence, mechanisms and impacts

It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3-4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively shallow boundary layer. Field and laboratory experiments have determined that the origin of the observed NO x flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future

Nitrate stable isotopes and major ions in snow and ice samples from four Svalbard sites

Increasing reactive nitrogen (N-r) deposition in the Arctic may adversely impact N-limited ecosystems. To investigate atmospheric transport of N-r to Svalbard, Norwegian Arctic, snow and firn samples were collected from glaciers and analysed to define spatial and temporal variations (1 10 years) in major ion concentrations and the stable isotope composition (delta N-15 and delta O-18) of nitrate (NO3-) across the archipelago. The delta N-15(NO3-) and delta O-18(NO3-) averaged -4 parts per thousand and 67 parts per thousand in seasonal snow (2010-11) and -9 parts per thousand and 74 parts per thousand in firn accumulated over the decade 2001-2011. East-west zonal gradients were observed across the archipelago for some major ions (non-sea salt sulphate and magnesium) and also for delta N-15(NO3-) and delta O-18(NO3-) in snow, which suggests a different origin for air masses arriving in different sectors of Svalbard. We propose that snowfall associated with long-distance air mass transport over the Arctic Ocean inherits relatively low delta N-15(NO3-) due to in-transport N isotope fractionation. In contrast, faster air mass transport from the north-west Atlantic or northern Europe results in snowfall with higher delta N-15(NO3-) because in-transport fractionation of N is then time-limited

A semi-Lagrangian view of ozone production tendency in North American outflow in the summers of 2009 and 2010

The Pico Mountain Observatory, located at 2225 m a.s.l. in the Azores Islands, was established in 2001 to observe long-range transport from North America to the central North Atlantic. In previous research conducted at the observatory, ozone enhancement (> 55 ppbv) in North American outflows was observed, and efficient ozone production in these outflows was postulated. This study is focused on determining the causes for high d[O3] / d[CO] values (~1 ppbv ppbv−1) observed in the summers of 2009 and 2010. The folded retroplume technique, developed by Owen and Honrath (2009), was applied to combine upwind FLEXPART transport pathways with GEOS-Chem chemical fields. The folded result provides a semi-Lagrangian view of polluted North American outflow in terms of physical properties and chemical processes, including production/loss rate of ozone and NOx produced by lightning and thermal decomposition of peroxy acetyl nitrate (PAN). Two transport events from North America were identified for detailed analysis. High d[O3] / d[CO] was observed in both events, but due to differing transport mechanisms, ozone production tendency differed between the two. A layer of net ozone production was found at 2 km a.s.l. over the Azores in the first event plume, apparently driven by PAN decomposition during subsidence of air mass in the Azores–Bermuda High. In the second event, net ozone loss occurred during transport in the lower free troposphere, yet observed d[O3] / d[CO] was high. We estimate that in both events, CO loss through oxidation contributed significantly to d[O3] / d[CO] enhancement. Thus, it is not appropriate to use CO as a passive tracer of pollution in these events. In general, use of d[O3] / d[CO] as an indicator of net ozone production/loss may be invalid for any situation in which oxidants are elevated. Based on our analysis, use of d[O3] / d[CO] to diagnose ozone enhancement without verifying the assumption of negligible CO loss is not advisable

Surface-Enhanced Nitrate Photolysis on Ice

Heterogeneous nitrates photolysis is the trigger for many chemical processes occurring in the polar boundary layer and is widely believed to occur in a quasi-liquid layer (QLL) at the surface of ice. The dipole forbidden character of the electronic transition relevant to boundary layer atmospheric chemistry and the small photolysis/photoproducts quantum yields in ice (and in water) may confer a significant enhancement and interfacial specificity to this important photochemical reaction at the surface of ice. Using amorphous solid water films at cryogenic temperatures as models for the disordered interstitial air/ice interface within the snowpack suppresses the diffusive uptake kinetics thereby prolonging the residence time of nitrate anions at the surface of ice. This approach allows their slow heterogeneous photolysis kinetics to be studied providing the first direct evidence that nitrates adsorbed onto the first molecular layer at the surface of ice are photolyzed more effectively than those dissolved within the bulk. Vibrational spectroscopy allows the ~3-fold enhancement in photolysis rates to be correlated with the nitrates’ distorted intramolecular geometry thereby hinting at the role played by the greater chemical heterogeneity in their solvation environment at the surface of ice than in the bulk. A simple 1D kinetic model suggests 1-that a 3(6)-fold enhancement in photolysis rate for nitrates adsorbed onto the ice surface could increase the photochemical NO[subscript 2] emissions from a 5(8) nm thick photochemically active interfacial layer by 30%(60)%, and 2-that 25%(40%) of the NO[subscript 2] photochemical emissions to the snowpack interstitial air are released from the top-most molecularly thin surface layer on ice. These findings may provide a new paradigm for heterogeneous (photo)chemistry at temperatures below those required for a QLL to form at the ice surface