Ozone depletion in the plume of a solid-fueled rocket

The local effects of the emission of a solid-fueled rocket on the stratospheric ozone concentration have been investigated by photochemical model calculations. A one-dimensional horizontal model has been applied which calculates the trace gas composition at a single atmospheric altitude spatially resolved around the exhaust plume. Different cases were tested for the emissions of the Space Shuttle concerning the composition of the exhaust and the effects of heterogeneous reactions on atmospheric background aerosol.The strongest depletion of ozone is achieved when a high amount of the emitted chlorine is Cl₂. If it is purely HCl, the effect is smallest, though in this case the heterogeneous reactions show their largest influence. From the results it may be estimated whether ozone depletion caused by rocket launches can be detected by satellite instruments. It appears that the chance of coincidental detection of such an event is rather small.     

Modeling of aircraft exhaust emissions and infrared spectra for remote measurement of nitrogen oxides

Infrared (IR) molecular spectroscopy is proposed to perform remote measurements of NO_x concentrations in the exhaust plume and wake of aircraft. The computer model NIRATAM is applied to simulate the physical and chemical properties of the exhaust plume and to generate low resolution IR spectra and synthetical thermal images of the aircraft in its natural surroundings. High-resolution IR spectra of the plume, including atmospheric absorption and emission, are simulated using the molecular line-by-line radiation model FASCODE2. Simulated IR spectra of a Boeing 747–400 at cruising altitude for different axial and radial positions in the jet region of the exhaust plume are presented. A number of spectral lines of NO can be identified that can be discriminated from lines of other exhaust gases and the natural atmospheric background in the region around 5.2 µm. These lines can be used to determine NO concentration profiles in the plume. The possibility of measuring nitrogen dioxide NO₂ is also discussed briefly, although measurements turn out to be substantially less likely than those of NO. This feasibility study compiles fundamental data for the optical and radiometric design of an airborne Fourier transform spectrometer and the preparation of in-flight measurements for monitoring of aircraft pollutants.     

Chemistry in plumes of high-flying aircraft with H2 combustion engines: a modelling study

Recent discussions on high-speed civil transport (HSCT) systems have renewed the interest in the chemistry of supersonic-aircraft plumes. The engines of these aircraft emit large concentrations of radicals like O, H, OH, and NO. In order to study the effect of these species on the composition of the atmosphere, the detailed chemistry of an expanding and cooling plume is examined for different expansion models.For a representative flight at 26 km the computed trace gas concentrations do not differ significantly for different models of the expansion behaviour. However, it is shown that the distributions predicted by all these models differ significantly from those adopted in conventional meso-scale and global models in which the plume chemistry is not treated in detail. This applies in particular to the reservoir species HONO and H₂O₂.     

Investigation of exhaust gas dispersion in the near-wake region of a light-duty vehicle

The air pollution induced by urban traffic has addressed much attention in recent years as the rapid urbanization and the fast increase of vehicle number in urban area. In this study, we attempted to investigate the dispersion behavior of exhaust gas from exhaust pipe using computational fluid dynamics approach. The time-averaged CO₂ concentration, velocity and temperature profiles along the centerline of the vehicular exhaust plume were simulated in varied situations. The computational results showed good agreement with the experimental data and the numerical model was validated to be an effective method to investigate the pollutant dispersion in the near-wake region of a vehicle. Based on it, the numerical simulations were extended to explore the impacts of the emit concentration, the emit direction and the incoming velocity on the flow dynamics and CO₂ dispersion. The outputs indicated that the emit concentration could change the pollution level in the near-wake region of a vehicle and the emit direction may alter the spreading direction of the vehicular exhaust plume. The incoming velocity was found to have dominant influence on the dispersion of pollutant due to induced vortices and turbulence behind the vehicle. These findings are expected to provide important insight into evaluating the design and control strategies for alleviating mobile source emissions.     

Box and Gaussian plume models of the exhaust composition evolution of subsonic transport aircraft in- and out of the flight corridor

A box and a Gaussian plume model including gas-phase photochemistry and with plume dispersion parameters estimated from the few available plume observations are proposed and used for evaluation of photochemical transformations of exhausts from a single subsonic transport aircraft. The effects of concentration inhomogeneities in the plume cross section on the photochemical sources and sinks in the plume are analyzed for various groups of compounds. The influence of these inhomogeneities on the rate and on the mass of ambient air entrainment into the plume are studied also by comparing the box and the Gaussian plume model simulations during the first hours of their life. Due to the enterance of HO_X and NO_X from ambient air into the plume with rates varying from the wind shear and turbulence conditions, the rate of emitted NOX oxidation in the plume is dependent on these and also on the background concentration levels of HO_X and NO_X.     

Gasdynamic propagation of rocket exhaust products in the upper atmosphere

The dispersion of exhaust products of rocket fuel in the direction perpendicular to the motion of a rocket is investigated in this work. A comparison of the results of numerical calculations with a self-similar approximation of a strong cylindrically symmetric explosion is fulfilled. It is shown that at sufficiently high rocket velocity V _∞, which exceeds the sum of gas exhaust velocity V _e from the nozzle and sound speed V _s (V _∞ > V _e +V _s ), a gasdynamic hole can arise around the rocket trajectory in the upper atmosphere, inside which the total concentration of gas becomes less than the equilibrium concentration of gas at a given altitude. The dynamics of the profiles of density and temperature of the exhaust products inside a rocket plume is calculated.     

An On Line Atmospheric Dispersion Model (OLADMO) for the World Wide Web

This paper presents an overview of earlier and current methods of modelling atmospheric dispersion, and proposes and evaluates a screening model for operation over the World Wide Web. The On Line Atmospheric Dispersion Model (OLADMO) is a quasi boundary layer parameterised Gaussian plume model with additional algorithms to account for plume rise, building wake effects and deposition processes. The Monin–Obukhov length boundary layer parameter is utilised to define six stability classes in order to determine atmospheric turbulence and stability, whilst new equations, derived from an intercomparison study of old and next generation dispersion models, are used to calculate the horizontal and vertical dispersion coefficients σ _y and σ _z . Using data from two field experiments in Copenhagen, Denmark and Lillestrøm, Norway, the model results from OLADMO are found to compare favourably with the results from several old and next generation dispersion models. As a consequence of the unique nature of the meteorological and location factors of the Lillestrøm experiment, all models struggled to represent the concentrations observed during the field study adequately. However, OLADMO was the best performing model in this case, with a mean normalised crosswind integrated concentration 13% closer to the mean observed concentration than its nearest competitor. Because the evaluation of the model was conducted with a limited dataset, several limitations and improvements to both the model and experimental procedure are suggested.     

A SF6 tracer study of horizontal mixing in Lake Constance

Horizontal mixing processes in the hypolimnion of the western part of Lake Constance are studied by measuring the dispersion of a sulfur hexafluoride (SF₆) tracer plume. Only 1 liter gaseous SF₆ (STP) was released at a central hypolimnic depth of 60 m in August 1990. Over a period of 3 months the horizontal dispersion of the tracer plume was measured by 19 surveys using a new, vertically integrating sampling device. The observed horizontal dispersion is marked by strong storm-induced stirring events. Nevertheless mean turbulent diffusion coefficients for the whole period can be computed. They rise about linear from 0.7 10⁵ cm²/s to 3.0 10⁵ cm²/s with the distance from the western end of the lake. For the hypolimnion of Überlingersee, a sill-separated basin in the western part of Lake Constance, a simple budget model gives an exchange time of 67 ± 6 days with the main basin (Obersee).     

Estimation of SO<Subscript>2</Subscript> abundance in the eruption plume of Mt. Etna using two MIVIS thermal infrared channels: a case study from the Sicily-1997 Campaign

In this paper, an algorithm is developed based on the split-window technique, to estimate the SO₂ abundance in the plume of Mt. Etna volcano using the multispectral infrared and visible imaging spectrometer (MIVIS). The MIVIS data were remotely sensed in the thermal infrared (TIR) during the Sicily-1997 Campaign. In this study, the MODTRAN 3.5 code has been used to simulate the radiance at the sensor; the radiative transfer model was input along with the data of radio-sounding performed simultaneously with the MIVIS flight using a mobile radio-theodolite. From the SO₂ map, derived from the MIVIS image, the SO₂ flux along the axis of the plume was computed knowing the wind speed at the plume altitude. The SO₂ flux is variable along the plume axis. The average SO₂ flux (about 45 kg s^-1 on 12 June and about 30 kg s^-1 on 16 June) emitted from the vents is compared with the correlation spectrometer (COSPEC) measurements carried out by other teams (from the ground and from a light aircraft flying under the plume) during the MIVIS flight. Finally, by means of this algorithm it should be easier, with respect to the previously described procedure to monitor the SO₂ flux of a specific volcano such as Mt. Etna.     

The present-day and future impact of NOx emissions from subsonic aircraft on the atmosphere in relation to the impact of NOx surface sources

The effect of present-day and future NO_x emissions from aircraft on the NO_x and ozone concentrations in the atmosphere and the corresponding radiative forcing were studied using a three-dimensional chemistry transport model (CTM) and a radiative model. The effects of the aircraft emissions were compared with the effects of the three most important anthropogenic NO_x surface sources: road traffic, electricity generation and industrial combustion. From the model results, NO_x emissions from aircraft are seen to cause an increase in the NO_x and ozone concentrations in the upper troposphere and lower stratosphere, and a positive radiative forcing. For the reference year 1990, the aircraft emissions result in an increase in the NO_x concentration at 250 hPa of about 20 ppt in January and 50 ppt in July over the eastern USA, the North Atlantic Flight Corridor and Western Europe, corresponding to a relative increase of about 50%. The maximum increase in the ozone concentrations due to the aircraft emissions is about 3-4 ppb in July over the northern mid-latitudes, corresponding to a relative increase of about 3-4%. The aircraft-induced ozone changes cause a global average radiative forcing of 0.025 W/m² in July. According to the ANCAT projection for the year 2015, the aircraft NO_x emissions in that year will be 90% higher than in the year 1990. As a consequence of this, the calculated NO_x perturbation by aircraft emissions increases by about 90% between 1990 and 2015, and the ozone perturbation by about 50-70%. The global average radiative forcing due to the aircraft-induced ozone changes increases by about 50% between 1990 and 2015. In the year 2015, the effects of the aircraft emissions on the ozone burden and radiative forcing are clearly larger than the individual effects of the NO_x surface sources. Taking chemical conversion in the aircraft plume into account in the CTM explicitly, by means of modified aircraft NO_x emissions, a significant reduction of the aircraft-induced NO_x and ozone perturbations is realised. The NO_x perturbation decreases by about 40% and the ozone perturbation by about 30% in July over Western Europe, the eastern USA and the North Atlantic Flight Corridor.     

Simultaneous identification of a single pollution point-source location and contamination time under known flow field conditions

A theoretical framework is presented that allows direct identification of a single point-source pollution location and time in heterogeneous multidimensional systems under known flow field conditions. Based on the concept of the transfer function theory, it is shown that an observed pollution plume contains all the necessary information to predict the concentration at the unknown pollution source when a reversed flow field transport simulation is performed. This target concentration C₀ is obtained from a quadratic integral of the observed pollution plume itself. Backwards simulation of the pollution plume leads to shrinkage of the C₀-contour due to dispersion. When the C₀-contour reduces to a singular point, i.e. becomes a concentration maximum, the position of the pollution source is identified and the backward simulation time indicates the time elapsed since the contaminant release. The theoretical basis of the method is first developed for the ideal case that the pollution plume is entirely known and is illustrated using a synthetic heterogeneous 2D example where all the hydro-dispersive parameters are known. The same example is then used to illustrate the procedure for a more realistic case, i.e. where only few observation points exist.     

Simulating the global transport of nitrogen oxides emissions from aircraft

With the atmosphere general circulation model ECHAM the passive transport of NO_x emitted from global subsonic air traffic and the NO_x concentration change due to these emissions are investigated. The source of NO_x is prescribed according to an aircraft emission data base. The sink of NO_x is parameterized as an exponential decay process with globally constant lifetime. Simulations in perpetual January and July modes are performed. Both the resulting mean and the standard deviation of the NO_x mass mixing ratio are analysed. In January horizontal dispersion is more pronounced and vertical mixing is smaller than in July. In both cases the resulting quasi-stationary fields of the mass mixing ratio display a pronounced zonal asymmetry. The variability accounts up to 30% of the mean field.     

Radiative transfer corrections for accurate spectroscopic measurements of volcanic gas emissions

There is widespread use of passive remote sensing techniques to quantify trace gas column densities in volcanic plumes utilizing scattered sunlight as a light source. Examples include passive DOAS, COSPEC, and the SO₂ camera. In order to calculate trace gas concentrations or volcanic emission fluxes, knowledge about the optical path through the plume is necessary. In the past, a straight photon path through the plume has always been assumed although it was known that this is not always true. Here we present the results of model studies conducted specifically to quantify the effects of realistic radiative transfer in and around volcanic plumes on ground-based remote sensing measurements of SO₂. The results show that measurements conducted without additional information on average photon paths can be inaccurate under certain conditions, with possible errors spanning more than an order of magnitude. Both over and underestimation of the true column density can occur. Actual errors depend on parameters such as distance between instrument and plume, plume SO₂ concentration, plume aerosol load, as well as aerosol conditions in the ambient atmosphere. As an example, a measurement conducted with an SO₂ camera is discussed, the results of which can only be correctly interpreted if realistic radiative transfer is considered. Finally, a method is presented which for the first time allows the retrieval of actual average photon paths in spectroscopic (i.e. DOAS) measurements of adequate resolution. By allowing for a wavelength dependent column density during the evaluation of DOAS measurements, we show how radiative transfer effects can be corrected using information inherently available in the measured spectra, thus greatly enhancing the accuracy of DOAS measurements of volcanic emissions.     

Dynamics of aircraft exhaust plumes in the jet-regime

A computational model describing the two-dimensional, turbulent mixing of a single jet of exhaust gas from aircraft engines with the ambient atmosphere is presented. The underlying assumptions and governing equations are examined and supplemented by a discussion of analytical solutions. As an application, the jet dynamics of a B747-400 aircraft engine in cruise and its dependence on key parameters is investigated in detail. The computer code for this dynamical model is computationally fast and can easily be coupled to complex chemical and microphysical models in order to perform comprehensive studies of atmospheric effects from aircraft exhaust emissions in the jet regime.     

Continuum-scale convective mixing in geological CO2 sequestration in anisotropic and heterogeneous saline aquifers

Deep saline aquifers are important geological formations for CO₂ sequestration. It has been known that dissolution of CO₂ increases brine density, which results in downward density-driven convection and consequently greatly enhances CO₂ sequestration. In this study, a continuum-scale lattice Boltzmann model is used to investigate convective mixing of CO₂ in saline aquifers. It is found that increasing permeability in either the vertical or horizontal direction accelerates the development of convective mixing. In a heterogeneous aquifer, increasing heterogeneity hampers the onset of convective mixing, because the heterogeneous permeability field results in a large portion of low-velocity region which reduces the instability of the system. The critical time for the onset of instability depends mainly on the coefficient of variation (COV) of the permeability field, and is insensitive to the correlation length. This implies that within the scale of critical time, mass transport is dominated by diffusion, and thus depends mainly on fine-scale heterogeneity controlled by COV. We derived an empirical formula for estimating the critical time, which leads to good estimates for all combinations of COV and correlation length. Fingering, channeling, and dispersion are the three mechanisms for mass transport. In dispersion, dissolved mass is approximately proportional to the square root of time, while in fingering and channeling it is approximately proportional to time. Mass transport by channeling depends significantly on permeability structure, while by fingering it is controlled by gravitational instability. It is also found that larger volumes of CO₂ can be stored in heterogeneous aquifers because of higher mass dissolution rates.     

A new technique to estimate volcanic gas composition: plume measurements with a portable multi-sensor system

A portable multi-sensor system was developed to measure volcanic plumes in order to estimate the chemical composition and temperature of volcanic gases. The multi-sensor system consists of a humidity–temperature sensor, SO₂ electrochemical sensor, CO₂ IR analyzer, pump and flow control units, pressure sensor, data logger, and batteries; the whole system is light (∼5 kg) and small enough to carry in a medium-size backpack. Volcanic plume is a mixture of atmosphere and volcanic gas; therefore volcanic gas composition and temperature can be estimated by subtracting the atmospheric gas background from the plume data. In order to obtain the contrasting data of the plume and the atmosphere, measurements were repeated in and out of the plume. The multi-sensor technique was applied to measure the plume of Tarumae, Tokachi, and Meakan volcanoes, Hokkaido, Japan. Repeated measurements at each volcano gave a consistent composition with ±10–30% errors, depending on the stability of the background atmospheric conditions. Fumarolic gas samples were also collected at the Tokachi volcano by a conventional method, and we found a good agreement (the difference <10%) between the composition estimated by the multi-sensor technique and conventional method. Those results demonstrated that concentration ratios of major volcanic gas species (i.e., H₂O, CO₂, and SO₂) and temperature can be estimated by the new technique without any complicated chemical analyses even for gases emitted from an inaccessible open vent. Estimation of a more detailed gas composition can be also achieved by the combination of alkaline filter techniques to measure Cl/F/S ratios in the plume and other sensors for H₂S and H₂.     

CO2 and H2S concentrations in the atmosphere at the Solfatara of Pozzuoli

The CO₂ and H₂S concentration in the Solfatara atmosphere has been measured. The concentrations of both gases are higher neraby the more active areas and decrease away from them. A sharp horizontal and vertical gradient of the CO₂ content has been recognized.Such gradient is assumed to result from a diffusion of gas from the ground to the atmosphere.The total output of CO₂ has been computed based on a turbulent diffusion model. The obtained value is in good agreement with previously abserved values (Italiano et al., 1984).The feasibility of monitoring the atmosphere of Solfatara for either gas hazard and surveillance of volcanic activity has also been evaluated.     

Metropolitan-scale Transport and Dispersion from the New York World Trade Center Following September 11, 2001. Part II: An Application of the CALPUFF Plume Model

Following the collapse of the New York World Trade Center (WTC) towers on September 11, 2001, Local, State, and Federal agencies initiated numerous air monitoring activities to better understand the ongoing impacts of emissions from the disaster. The collapse of the World Trade Center towers and associated fires that lasted for several weeks resulted at times in a noticeable plume of material that was dispersed around the Metropolitan New York City (NYC) area. In general, the plume was only noticeable for a short period of time following September 11, and only apparent close to the World Trade Center site. A study of the estimated pathway which the plume of WTC material would likely follow was completed to support the United States Environmental Protection Agency’s 2002 initial exposure assessments. In this study, the WTC emissions were simulated using the CALMET-CALPUFF model in order to examine the general spatial and temporal dispersion patterns over NYC. This paper presents the results of the CALPUFF plume model in terms of plume dilution and location, since the exact source strength remains unknown. Independent observations of PM_2.5 are used to support the general dispersion features calculated by the model. Results indicate that the simulated plume matched well with an abnormal increase (600–1000% of normal) in PM_2.5 two nights after the WTC collapse as the plume rotated north to southeast, towards parts of NYC. Very little if any evidence of the plume signature was noted during a similar flow scenario a week after September 11. This leads to the conclusion that other than areas within a few kilometers from the WTC site, the PM_2.5 plume was not observable over NYC’s background concentration after the first few days.     

Pyrite Oxidation Halts Migration of a Phosphorus Plume

We have established a monitoring record of phosphate (PO₄³⁻) migration in the Long Point, ON campground septic system plume that now spans 26 years. Previously, at year 16 (2006), a P plume 16 m in length was documented and provided a good fit with an analytical advection dispersion model when a P migration velocity of 0.8 m/yr was used (retardation factor of 37) and when P behaved in an otherwise conservative manner (sorption only). However, between years 16 and 26 (2016), the P plume length expanded by only 2 m (0.2 m/yr) and increased in depth by only 0.5 m. The zone of abrupt P depletion at depth occurs close to the zone where SO₄²⁻ concentrations increase in response to NO₃⁻ oxidation of pyrite. Scanning electron microscope images of sand grains from the nose of the P plume reveal abundant authigenic mineral coatings of considerable thickness (∼5 to 20 μm), with Fe as the dominant cation and containing 1 to 3 wt % P. This evidence suggests that P is now being attenuated along a reaction front that coincides with the zone where pyrite oxidation is occurring. P migration may now be controlled by the rate of migration of the pyrite oxidation front and this is several times slower than the previously indicated rate in the shallower, sorption-controlled portion of the plume. Monitoring at Long Point has demonstrated the danger of embracing an overly simplistic conceptual model when attempting to predict wastewater P migration in groundwater and also highlights the unique insight provided by a long-term monitoring record.