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A size-segregated aerosol dynamics model UHMA (University of Helsinki Multicomponent Aerosol model) was developed for studies of multicomponent tropospheric aerosol particles. The model includes major aerosol microphysical processes in the atmosphere with a focus on new particle formation and growth; thus it incorporates particle coagulation and multicomponent condensation, applying a revised treatment of condensation flux onto free molecular regime particles and the activation of nanosized clusters by organic vapours (Nano-Köhler theory), as well as recent parameterizations for binary H<sub>2</sub>SO<sub>4</sub>-H<sub>2</sub>O and ternary H<sub>2</sub>SO<sub>4</sub>-NH<sub>3</sub>-H<sub>2</sub>O homogeneous nucleation and dry deposition. The representation of particle size distribution can be chosen from three sectional methods: the hybrid method, the moving center method, and the retracking method in which moving sections are retracked to a fixed grid after a certain time interval. All these methods can treat particle emissions and atmospheric transport consistently, and are therefore suitable for use in large scale atmospheric models. In a test simulation against an accurate high resolution solution, all the methods showed reasonable treatment of new particle formation with 20 size sections although the hybrid and the retracking methods suffered from artificial widening of the distribution. The moving center approach, on the other hand, showed extra dents in the particle size distribution and failed to predict the onset of detectable particle formation. In a separate test simulation of an observed nucleation event, the model captured the key qualitative behaviour of the system well. Furthermore, its prediction of the organic volume fraction in newly formed particles, suggesting values as high as 0.5 for 3–4 nm particles and approximately 0.8 for 10 nm particles, agrees with recent indirect composition measurements.
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The urban boundary layer (UBL), in comparison with "rural" homogeneous atmospheric boundary layers, is characterised by greatly enhanced mixing, resulting from both the large surface roughness and increased surface heating, and by horizontal heterogeneity of the mixing height (MH) and other meteorological fields due to variations in surface roughness and heating from rural to central city areas. So, the UBL is considered as a specific case of the atmospheric boundary layer (ABL) over a non-homogeneous terrain. Therefore it is important to study how much the MH characteristics differ in urban and rural, marine or other more homogeneous areas. Most of the parameterisations of MH were developed for the conditions of a homogeneous terrain, so their applicability for urban conditions should be verified. Just a few authors suggested specific methods for MH determination in urban areas. In this paper the MH over urban, semi-urban, rural and marine areas of the Copenhagen metropolitan area is considered. Proceeding from the data from the Jægersborg radiosounding station measurement and analysis of different methods of the MH estimation, the peculiarities of the UBL and intercomparison of different MH estimation methods for urban and rural conditions are discussed. It is shown that the urban MH is considerably bigger for stably stratified (nocturnal) boundary layer cases in comparison with the "non-urban" MH. Daytime (usually the convective boundary layer) MH does not differ significatly in urban and "non-urban" sectors.
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For the first time, three different temperature lidar methods are combined to obtain time-resolved complete temperature profiles with high altitude resolution over an altitude range from the planetary boundary layer up to the lower thermosphere (about 1–105 km). The Leibniz-Institute of Atmospheric Physics (IAP) at Kühlungsborn, Germany (54° N, 12° E) operates two lidar instruments, using three different temperature measurement methods, optimized for three altitude ranges: (1) Probing the spectral Doppler broadening of the potassium D<sub>1</sub> resonance lines with a tunable narrow-band laser allows atmospheric temperature profiles to be determined at metal layer altitudes (80–105 km). (2) Between about 20 and 90 km, temperatures were calculated from Rayleigh backscattering by air molecules, where the upper start values for the calculation algorithm were taken from the potassium lidar results. Correction methods have been applied to account for, e.g. Rayleigh extinction or Mie scattering of aerosols below about 32 km. (3) At altitudes below about 25 km, backscattering in the Rotational Raman lines is strong enough to obtain temperatures by measuring the temperature dependent spectral shape of the Rotational Raman spectrum. This method works well down to about 1 km. The instrumental configurations of the IAP lidars were optimized for a 3–6 km overlap of the temperature profiles at the method transition altitudes. We present two night-long measurements with clear wave structures propagating from the lower stratosphere up to the lower thermosphere.
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In the past, many studies have been carried out to demonstrate the influence of meteoroids on the atmospheric metal layer, observed roughly in the altitude range 80–105 km. Even with the capability of present day resonance lidars to measure metal densities within single meteor trails, it has been difficult to prove any influence of meteors on the average metal layer. In contrast to approaches taken earlier, we discuss here the seasonal characteristics of potassium, calcium, calcium ion, iron and sodium above 110 km altitude where the average nocturnal densities are so low that the existence of a baseline level of metal atoms and ions is often overlooked. By comparing simultaneous and common-volume observations of different metal layers at one location, we demonstrate that despite their different seasonal characteristics at lower altitudes remarkably similar seasonal characteristics are observed at higher altitudes. In addition, a qualitative agreement is also found for potassium at different latitudes. A comparison of metal densities at 113 km altitude with known meteor showers indicates a strong influence of shower meteoroids on the topside of the metal layers. Simultaneous observations of K along with Ca, Fe and/or Na permit the calculation of abundance ratios, which at 113 km altitude are quite similar to values measured in single meteor trails by ground based lidars. Furthermore, the increase in densities throughout summer is strong evidence for the influence of sporadic meteoroids on the high metal layers. This increase correlates well with the seasonal variation of sporadic micrometeor input independent of meteor showers. Given these evidences, we contend that there is a direct influence of ablating meteoroids on the topside of the mesospheric metal layer.
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Understanding the global meteor flux at Earth requires the measurement of meteor velocities. While several radar methods exist for measuring meteor velocity, they may be biased by plasma reflection mechanisms. This paper presents a new method for deriving meteoroid velocity from the altitudinal extent of non-specular trails. This method employs our recent discoveries on meteor trail plasma instability. Dyrud et al. (2002) demonstrated that meteor trails are unstable over a limited altitude range, and that the precise altitudes of instability are dependent on the meteoroid that generated the trail. Since meteor trail instability results in field aligned irregularities (FAI) that allow for radar reflection, non-specular trail observations may be used to derive velocity. We use ALTAIR radar data of combined head echos and non-specular trails to test non-specular trail derived velocity against head echo velocities. Meteor velocities derived from non-specular trail altitudinal width match to within 5 km/s when compared with head echo range rates from the same meteor. We apply this technique to Piura radar observations of hundreds of non-specular trails to produce histograms of occurrence of meteor velocity based solely on this non-specular trails width criterion. The results from this study show that the most probable velocity of meteors seen by the Piura radar is near 50 km/s, which is comparable with modern head echo studies.
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Atmospheric gravity waves have been the subject of intense research for several decades because of their extensive effects on the atmospheric circulation and the temperature structure. The U. Bonn lidar at the Esrange and the ALOMAR RMR lidar at the Andøya Rocket Range are located in northern Scandinavia 250 km apart on the east and west side of the Scandinavian mountain ridge. During January and February 2003 both lidar systems conducted measurements and retrieved atmospheric temperatures. On 19/20 January 2003 simultaneous measurements for more than 7 h were possible. Although during most of the campaign time the atmosphere was not transparent for the propagation of orographically induced gravity waves, they were nevertheless observed at both lidar stations with considerable amplitudes during these simultaneous measurements. And while the source of the observed waves cannot be determined unambiguously, the observations show many characteristics of orographically excited gravity waves. The wave patterns at ALOMAR show a random distribution with time whereas at the Esrange a persistency in the wave patterns is observable. This persistency can also be found in the distribution of the most powerful vertical wavelengths. The mode values are both at about 5 km vertical wavelength, however the distributions are quite different, narrow at the Esrange with values from λ<i><sub>z</sub></i>=2–6 km and broad at ALOMAR, covering λ<i><sub>z</sub></i>=1–12 km vertical wavelength. In particular the difference between the observations at ALOMAR and at the Esrange can be understood by different orographic conditions while the propagation conditions were quite similar. At both stations the waves deposit energy in the atmosphere with increasing altitude, which leads to a decrease of the observed gravity wave potential energy density with altitude. The meteorological situation during these measurements was different from common winter situations. The ground winds were mostly northerlies, changed in the upper troposphere and lower stratosphere to westerlies and returned to northerlies in the middle stratosphere.
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During the ESCOMPTE precampaign (summer 2000, over Southern France), a 3-day period of intensive observation (IOP0), associated with ozone peaks, has been simulated. The comprehensive RAMS model, version 4.3, coupled on-line with a chemical module including 29 species, is used to follow the chemistry of the polluted zone. This efficient but time consuming method can be used because the code is installed on a parallel computer, the SGI 3800. Two runs are performed: run 1 with a single grid and run 2 with two nested grids. The simulated fields of ozone, carbon monoxide, nitrogen oxides and sulfur dioxide are compared with aircraft and surface station measurements. The 2-grid run looks substantially better than the run with one grid because the former takes the outer pollutants into account. This on-line method helps to satisfactorily retrieve the chemical species redistribution and to explain the impact of dynamics on this redistribution.
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Model-measurement comparisons of HO<sub>x</sub> in extremely clean air ([NO]<3 ppt) are reported. Measurements were made during the second Southern Ocean Photochemistry Experiment (SOAPEX-2), held in austral summer 1999 at the Cape Grim Baseline Air Pollution Station in north-western Tasmania, Australia. <P style="line-height: 20px;"> The free-radical chemistry was studied using a zero-dimensional box-model based upon the Master Chemical Mechanism (MCM). Two versions of the model were used, with different levels of chemical complexity, to explore the role of hydrocarbons upon free-radical budgets under very clean conditions. The "detailed" model was constrained to measurements of CO, CH<sub>4</sub> and 17 NMHCs, while the "simple" model contained only the CO and CH<sub>4</sub> oxidation mechanisms, together with inorganic chemistry. The OH and HO<sub>2</sub> (HO<sub>x</sub>) concentrations predicted by the two models agreed to within 5–10%. <P style="line-height: 20px;"> The model results were compared with the HO<sub>x</sub> concentrations measured by the FAGE (Fluorescence Assay by Gas Expansion) technique during four days of clean Southern Ocean marine boundary layer (MBL) air. The models overestimated OH concentrations by about 10% on two days and about 20% on the other two days. HO<sub>2</sub> concentrations were measured during two of these days and the models overestimated the measured concentrations by about 40%. Better agreement with measured HO<sub>2</sub> was observed by using data from several MBL aerosol measurements to estimate the aerosol surface area and by increasing the HO<sub>2</sub> uptake coefficient to unity. This reduced the modelled HO<sub>2</sub> overestimate by ~40%, with little effect on OH, because of the poor HO<sub>2</sub> to OH conversion at the low ambient NO<sub>x</sub> concentrations. <P style="line-height: 20px;"> Local sensitivity analysis and Morris One-At-A-Time analysis were performed on the "simple" model, and showed the importance of reliable measurements of j(O<sup>1</sup>D) and [HCHO] and of the kinetic parameters that determine the efficiency of O(<sup>1</sup>D) to OH and HCHO to HO<sub>2</sub> conversion. A 2σ standard deviation of 30–40% for OH and 25–30% for HO<sub>2</sub> was estimated for the model calculations using a Monte Carlo technique coupled with Latin Hypercube Sampling (LHS).
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Nitrate is an important component of (secondary inorganic) fine aerosols in Europe. We present a model simulation for the year 1995 in which we account for the formation of secondary inorganic aerosols including ammonium sulphate and ammonium nitrate, a semi volatile component. For this purpose, the chemistry-transport model LOTOS was extended with a thermodynamic equilibrium module and additional relevant processes to account for secondary aerosol formation and deposition. During winter, fall and especially spring high nitrate levels are projected over north western, central and eastern Europe. During winter nitrate concentrations are highest in Italy, in accordance with observed data. In winter nitric acid, the precursor for aerosol nitrate is formed through heterogeneous reactions on the surface of aerosols. Modelled and observed sulphate concentrations show little seasonal variation. Compared to sulphate levels, appreciable ammonium nitrate concentrations in summer are limited to those areas with high ammonia emissions, e.g. the Netherlands, since high ammonia concentrations are necessary to stabilise this aerosol component at high temperatures. As a consequence of the strong seasonal variation in nitrate levels the AOD depth of nitrate over Europe is especially significant compared to that of sulphate in winter and spring when equal AOD values are calculated over large parts of Europe. Averaged over all stations the model reproduces the measured concentrations for NO<sub>3</sub>, SO<sub>4</sub>, NH<sub>4</sub>, TNO<sub>3</sub> (HNO<sub>3</sub>+NO<sub>3</sub>), TNH<sub>4</sub> (NH<sub>3</sub>+NH<sub>4</sub>) and SO<sub>2</sub> within 20%. The daily variation is captured well, albeit that the model does not always represent the amplitude of single events. The model underestimates wet deposition which was attributed to the crude representation of cloud processes. Comparison of retrieved and computed aerosol optical depth (AOD) showed that the model underestimates AOD significantly, which was expected due to the lack of carbonaceous aerosols, sea salt and dust in the model. The treatment of ammonia was found to be a major source for uncertainties in the model representation of secondary aerosols. Also, inclusion of sea salt is necessary to properly assess the nitrate and nitric acid levels in marine areas.
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The importance of emission inventory uncertainty on the simulation of summertime tropospheric ozone over China has been analyzed using a regional chemical transport model. Three independent emissions inventories, that are (i) emission estimates from the Emission Database for Global Atmospheric Research (EDGAR) for the year 1995, (ii) a regional emission inventory used in the Transport and Chemical Evolution over the Pacific (TRACE-P) program with emissions for the year 2000 and (iii) a national emission inventory used in the China Ozone Research Program (CORP) with emission estimates for the year 1995, are used for model simulation over a summer period. Methods used for the development of the inventories are discussed and differences in simulated ozone and its precursors with these emission inventories are analyzed. Comparison of the emission inventories revealed large differences in the emission estimates (up to 50% for NO<sub>x</sub>, ~100% for NMVOC and ~1000% for CO). Application of the different emission inventories in three model simulations showed minor differences in both surface O<sub>3</sub> in rather unpolluted areas in China and at higher altitudes (500mbar). In polluted areas, differences in surface O<sub>3</sub> are 30-50% between the different model simulations which seem rather small taking into account the large differences in the emission inventories. Additional sensitivity runs showed that the difference in NO<sub>x</sub> emissions as well NMVOC emissions is a dominant factor which controls the differences in simulated O<sub>3</sub> concentrations while the impact of differences in CO emissions is relatively small. Although the CO emission estimate by CORP seems to be underestimated, there is no confidence to highlight one emission inventory better than the others.
