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A study of dispersion in complex terrain under winter conditions using high-resolution mesoscale and Lagrangian particle models

A mesoscale model (MM5), a dispersive Langrangian particle model (FLEXPART), and intensive meteorological and COrrelation SPECtrometer (COSPEC) measurements from a field campaign are used to examine the advection and turbulent diffusion patterns associated with interactions and forcings between topography, synoptic atmospheric flows and thermally-driven circulations. This study describes the atmospheric dispersion of emissions from a power plant with a 343-m tall chimney, situated on very complex terrain in the North-East of Spain, under winter conditions. During the field campaign, the plume was transported with low transversal dispersion and deformed essentially due to the effect of mechanical turbulence. The main surface impacts appeared at long distances from the emission source (more than 30 km). The results show that the coupled models (MM5 and FLEXPART) are able to predict the plume integral advection from the power plant on very complex terrain. Integral advection and turbulent dispersion are derived from the dispersive Lagrangian model output for three consecutive days so that a direct quantitative comparison has been made between the temporal evolution of the predicted three-dimensional dispersive conditions and the COSPEC measurements. Comparison between experimental and simulated transversal dispersion shows an index of agreement between 80% and 90%, within distance ranges from 6 to 33 km from the stack. Linked to the orographic features, the simulated plume impacts on the ground more than 30 km away from the stack, because of the lee waves simulated by MM5.
OH and HO2 chemistry during NAMBLEX: roles of oxygenates, halogen oxides and heterogeneous uptake

Several zero-dimensional box-models with different levels of chemical complexity, based on the Master Chemical Mechanism (MCM), have been used to study the chemistry of OH and HO2 in a coastal environment in the Northern Hemisphere. The models were constrained to and compared with measurements made during the NAMBLEX campaign (Mace Head, Ireland) in summer 2002. The base models, which were constrained to measured CO, CH4 and NMHCs, were able to reproduce [OH] within 25%, but overestimated [HO2] by about a factor of 2. Agreement was improved when the models were constrained to oxygenated compounds (acetaldehyde, methanol and acetone), highlighting their importance for the radical budget. When the models were constrained to measured halogen monoxides (IO, BrO) and used a more detailed, measurements-based, treatment to describe the heterogeneous uptake, modelled [OH] increased by up to 15% and [HO2] decreased by up to 30%. The actual impact of halogen monoxides on the modelled concentrations of HOx was dependant on the uptake coefficients used for HOI, HOBr and HO2. Better agreement, within the combined uncertainties of the measurements and of the model, was achieved when using high uptake coefficients for HO2 and HOI (γHO2=1, γHOI=0.6). A rate of production and destruction analysis of the models allowed a detailed study of OH and HO2 chemistry under the conditions encountered during NAMBLEX, showing the importance of oxygenates and of XO (where X=I, Br) as co-reactants for OH and HO2 and of HOX photolysis as a source for OH.
Measurements of optical properties of atmospheric aerosols in Northern Finland

Three years of continuous measurements of aerosol optical properties and simultaneous aerosol number size distribution measurements at Pallas GAW station, a remote subarctic site in the northern border of the boreal forest zone, have been analysed. The scattering coefficient at 550 nm varied from 0.2 to 94.4 Mm−1 with an average of 7.1±8.6 Mm−1. Both the scattering and backscattering coefficients had a clear seasonal cycle with an autumn minimum and a 4–5 times higher summer maximum. The scattering was dominated by submicron aerosols and especially so during late summer and autumn. The Ångström exponent had a clear seasonal pattern with maximum values in late summer and minimum values during wintertime. The highest hemispheric backscattering fraction values were observed in autumn. To analyse the influence of air mass origin on the aerosol optical properties a trajectory climatology was applied to the Pallas aerosol data. The most polluted trajectory patterns represented air masses from the Kola Peninsula, Scandinavia and Russia as well as long-range transport from Britain and Eastern Europe. These air masses had the largest average scattering and backscattering coefficients for all seasons. Higher than average values of the Ångström exponent were also observed in connection with transport from these areas.
Methane production from mixed tropical savanna and forest vegetation in Venezuela

Measurements of methane concentrations in the boundary layer in the northern part of the Guayana shield, Venezuela, during the wet season (October 1988), showed the presence of substantial methane surface emissions. The measuring site is within the savanna climate region, but is affected by emissions from savanna and forest vegetation. From day versus night concentration measurements, with higher concentrations during night, a methane source strength near the site of 3–7×1011 molecules/cm2/s can be estimated, which includes emissions from small tracts of flooded soils, termites and especially tropical vegetation. Extrapolated to the entire savanna, this may imply a methane source of ~30–60 Tg yr−1 similar to the one calculated for tropical vegetation on the basis of recently published in vitro plant emission experiments by Keppler et al. (2006), which indicate emissions of ~30 Tg yr−1 for tropical savannas and grasslands and ~78 Tg yr−1 for tropical forests.
On the possible causes of recent increases in northern hemispheric total ozone from a statistical analysis of satellite data from 1979 to 2003

Global total ozone measurements from various satellite instruments such as SBUV, TOMS, and GOME show an increase in zonal mean total ozone at northern hemispheric (NH) mid to high latitudes since the mid-nineties. This increase could be expected from the peaking and start of decline in the effective stratospheric halogen loading, but the rather rapid increase observed in NH zonal mean total ozone suggests that another physical mechanism such as winter planetary wave activity has increased which has led to higher stratospheric Arctic temperatures. This has enhanced ozone transport into higher latitudes in recent years as part of the residual circulation and at the same time reduced the frequency of cold Arctic winters with enhanced polar ozone loss. Results from various multi-variate linear regression analyses using SBUV V8 total ozone with explanatory variables such as a linear trend or, alternatively, EESC (equivalent effective stratospheric chlorine) and on the other hand planetary wave driving (eddy heat flux) or, alternatively, polar ozone loss (PSC volume) in addition to proxies for stratospheric aerosol loading, QBO, and solar cycle, all considered to be main drivers for ozone variability, are presented. It is shown that the main contribution to the recent increase in NH total ozone is from the combined effect of rising tropospheric driven planetary wave activity associated with reduced polar ozone loss at high latitudes as well as increasing solar activity. This conclusion can be drawn regardless of the use of linear trend or EESC terms in our statistical model. It is also clear that more years of data will be needed to further improve our estimates of the relative contributions of the individual processes to decadal ozone variability. The question remains if the observed increase in planetary wave driving is part of natural decadal atmospheric variability or will persist. If the latter is the case, it could be interpreted as a possible signature of climate change.
An improved inlet for precisely measuring the atmospheric Ar/N2 ratio

The atmospheric Ar/N2 ratio is expected to be useful as a tracer of air-sea heat exchange, but this application has been hindered in part due to sampling artifacts. Here we show that the variability in δ(Ar/N2) due to thermal fractionation at the inlet can be on the order of 40-80 per meg, and we introduce the use of an aspirated solar shield that successfully minimizes such fractionation. The data collected using this new inlet have a mean diurnal cycle of 1.0 per meg or less, suggesting that any residual thermal fractionation effect is reduced to this level.
Modeling of trace gases from the 1998 North Central Mexico forest fire smoke plume, as measured over Phoenix

Forest fires in North and Central America have been frequent and extensive over the past few years. Though much research has addressed the effects of forest fires in tropical South America and Africa on regional and global-scale oxidants, the same is not true for North America. Here we show that one of the days during an intensive field campaign conducted over Phoenix, Arizona, in 1998 was substantially influenced by transport from forest fires in central and southern Mexico. We combined data collected from aircraft platforms, surface stations, and satellite with model results to establish that the origin of the air sampled over Phoenix on 20 May 1998, was from forest fires in Mexico. We also investigated the effect of the smoke layer on photolysis rates and hence photochemistry over a five-day travel period from the source region to Phoenix. The results show that a smoke layer could reduce photolysis rates of key tropospheric constituents significantly and decrease the oxidant formation rates during the first few days of the plume history. The ultimate effect of the smoke layer on the evolution of oxidants in the plume was, however, shown to be minimal.
Convective formation of pileus cloud near the tropopause

Pileus clouds form where humid, vertically stratified air is mechanically displaced ahead of rising convection. This paper describes convective formation of pileus cloud in the tropopause transition layer (TTL), and explores a possible link to the formation of long-lasting cirrus at cold temperatures. The study examines in detail in-situ measurements from off the coast of Honduras during the July 2002 CRYSTAL-FACE experiment that showed an example of TTL cirrus associated with, and penetrated by, deep convection. The TTL cirrus was enriched with total water compared to its surroundings, but was composed of extremely small ice crystals with effective radii between 2 and 4 μm. Through gravity wave analysis, and intercomparison of measured and simulated cloud microphysics, it is argued that the TTL cirrus originated neither from convectively-forced gravity wave motions nor environmental mixing alone. Rather, it is hypothesized that a combination of these two processes was involved in which, first, a pulse of convection forced pileus cloud to form from TTL air; second, the pileus layer was punctured by the convective pulse and received larger ice crystals through interfacial mixing; third, the addition of this condensate inhibited evaporation of the original pileus ice crystals where a convectively forced gravity wave entered its warm phase; fourth, through successive pulses of convection, a sheet of TTL cirrus formed. While the general incidence and longevity of pileus cloud remains unknown, in-situ measurements, and satellite-based Microwave Limb Sounder retrievals, suggest that much of the tropical TTL is sufficiently humid to be susceptible to its formation. Where these clouds form and persist, there is potential for an irreversible repartition from water vapor to ice at cold temperatures.
Spectroscopic evidence for NAT, STS, and ice in MIPAS infrared limb emission measurements of polar stratospheric clouds

We have analyzed mid-infrared limb-emission measurements of polar stratospheric clouds (PSCs) by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) during the Antarctic winter 2003 with respect to PSC composition. Coincident Lidar observations from McMurdo were used for comparison with PSC types 1a, 1b and 2. Application of new refractive index data of β-NAT have allowed to accurately simulate the prominent spectral band at 820 cm-1 observed by MIPAS at the location where the Lidar instrument observed type 1a PSCs. Broadband spectral fits covering the range from 780 to 960 cm-1 and from 1220 to 1490 cm-1 showed best agreement with the MIPAS measurements when spectroscopic data of NAT were used to simulate the MIPAS spectra. MIPAS measurements collocated with Lidar observations of Type 1b and Type 2 PSCs could only be reproduced by assuming a composition of supercooled ternary H2SO4/HNO3/H2O solution (STS) and of ice, respectively. Particle radius and number density profiles derived from MIPAS were generally consistent with the Lidar observations. Only in the case of ice clouds, PSC volumes are partly underestimated by MIPAS due to large cloud optical thickness in the limb-direction. A comparison of MIPAS cloud composition and Lidar PSC-type determination based on all available MIPAS-Lidar coincident measurements revealed good agreement between PSC-types 1a, 1b and 2, and NAT, STS and ice, respectively. We could not find spectroscopic evidence for the presence of nitric acid dihydrate (NAD) from MIPAS observations of PSCs over Antarctica in 2003.
MIPAS detects Antarctic stratospheric belt of NAT PSCs caused by mountain waves

Space borne infrared limb emission measurements by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) reveal the formation of a belt of polar stratospheric clouds (PSCs) of nitric acid trihydrate (NAT) particles over Antarctica in mid-June 2003. By mesoscale microphysical simulations we show that this sudden onset of NAT PSCs was caused by heterogeneous nucleation on ice in the cooling phases of large-amplitude stratospheric mountain waves over the Antarctic Peninsula and the Ellsworth Mountains. MIPAS observations of PSCs before this event show no indication for the presence of NAT clouds with volume densities larger than about 0.3 µm3/cm3 and radii smaller than 3 µm, but are consistent with supercooled droplets of ternary H2SO4/HNO3/H2O solution (STS). Simulations indicate that homogeneous surface nucleation rates have to be reduced by three orders of magnitude to comply with the observations.