Atmospheric particle formation in spatially and temporally varying conditions

Atmospheric particles affect the radiation balance of the Earth and thus the climate. New particle formation from nucleation has been observed in diverse atmospheric conditions but the actual formation path is still unknown. The prevailing conditions can be exploited to evaluate proposed formation mechanisms. This study aims to improve our understanding of new particle formation from the view of atmospheric conditions. The role of atmospheric conditions on particle formation was studied by atmospheric measurements, theoretical model simulations and simulations based on observations. Two separate column models were further developed for aerosol and chemical simulations. Model simulations allowed us to expand the study from local conditions to varying conditions in the atmospheric boundary layer, while the long-term measurements described especially characteristic mean conditions associated with new particle formation. The observations show statistically significant difference in meteorological and back-ground aerosol conditions between observed event and non-event days. New particle formation above boreal forest is associated with strong convective activity, low humidity and low condensation sink. The probability of a particle formation event is predicted by an equation formulated for upper boundary layer conditions. The model simulations call into question if kinetic sulphuric acid induced nucleation is the primary particle formation mechanism in the presence of organic vapours. Simultaneously the simulations show that ignoring spatial and temporal variation in new particle formation studies may lead to faulty conclusions. On the other hand, the theoretical simulations indicate that short-scale variations in temperature and humidity unlikely have a significant effect on mean binary water sulphuric acid nucleation rate. The study emphasizes the significance of mixing and fluxes in particle formation studies, especially in the atmospheric boundary layer. The further developed models allow extensive aerosol physical and chemical studies in the future.

How the development of condensation particle counters is reforming our view on atmospheric nucleation

Aerosol particles deteriorate air quality, atmospheric visibility and our health. They affect the Earth s climate by absorbing and scattering sunlight, forming clouds, and also via several feed-back mechanisms. The net effect on the radiative balance is negative, i.e. cooling, which means that particles counteract the effect of greenhouse gases. However, particles are one of the poorly known pieces in the climate puzzle. Some of the airborne particles are natural, some anthropogenic; some enter the atmosphere in particle form, while others form by gas-to-particle conversion. Unless the sources and dynamical processes shaping the particle population are quantified, they cannot be incorporated into climate models. The molecular level understanding of new particle formation is still inadequate, mainly due to the lack of suitable measurement techniques to detect the smallest particles and their precursors. This thesis has contributed to our ability to measure newly formed particles. Three new condensation particle counter applications for measuring the concentration of nano-particles were developed. The suitability of the methods for detecting both charged and electrically neutral particles and molecular clusters as small as 1 nm in diameter was thoroughly tested both in laboratory and field conditions. It was shown that condensation particle counting has reached the size scale of individual molecules, and besides measuring the concentration they can be used for getting size information. In addition to atmospheric research, the particle counters could have various applications in other fields, especially in nanotechnology. Using the new instruments, the first continuous time series of neutral sub-3 nm particle concentrations were measured at two field sites, which represent two different kinds of environments: the boreal forest and the Atlantic coastline, both of which are known to be hot-spots for new particle formation. The contribution of ions to the total concentrations in this size range was estimated, and it could be concluded that the fraction of ions was usually minor, especially in boreal forest conditions. Since the ionization rate is connected to the amount of cosmic rays entering the atmosphere, the relative contribution of neutral to charged nucleation mechanisms extends beyond academic interest, and links the research directly to current climate debate.

Novel Approaches to the Sampling of Atmospheric Aerosols and Determination of Chemical Composition

The Earth s climate is a highly dynamic and complex system in which atmospheric aerosols have been increasingly recognized to play a key role. Aerosol particles affect the climate through a multitude of processes, directly by absorbing and reflecting radiation and indirectly by changing the properties of clouds. Because of the complexity, quantification of the effects of aerosols continues to be a highly uncertain science. Better understanding of the effects of aerosols requires more information on aerosol chemistry. Before the determination of aerosol chemical composition by the various available analytical techniques, aerosol particles must be reliably sampled and prepared. Indeed, sampling is one of the most challenging steps in aerosol studies, since all available sampling techniques harbor drawbacks. In this study, novel methodologies were developed for sampling and determination of the chemical composition of atmospheric aerosols. In the particle-into-liquid sampler (PILS), aerosol particles grow in saturated water vapor with further impaction and dissolution in liquid water. Once in water, the aerosol sample can then be transported and analyzed by various off-line or on-line techniques. In this study, PILS was modified and the sampling procedure was optimized to obtain less altered aerosol samples with good time resolution. A combination of denuders with different coatings was tested to adsorb gas phase compounds before PILS. Mixtures of water with alcohols were introduced to increase the solubility of aerosols. Minimum sampling time required was determined by collecting samples off-line every hour and proceeding with liquid-liquid extraction (LLE) and analysis by gas chromatography-mass spectrometry (GC-MS). The laboriousness of LLE followed by GC-MS analysis next prompted an evaluation of solid-phase extraction (SPE) for the extraction of aldehydes and acids in aerosol samples. These two compound groups are thought to be key for aerosol growth. Octadecylsilica, hydrophilic-lipophilic balance (HLB), and mixed phase anion exchange (MAX) were tested as extraction materials. MAX proved to be efficient for acids, but no tested material offered sufficient adsorption for aldehydes. Thus, PILS samples were extracted only with MAX to guarantee good results for organic acids determined by liquid chromatography-mass spectrometry (HPLC-MS). On-line coupling of SPE with HPLC-MS is relatively easy, and here on-line coupling of PILS with HPLC-MS through the SPE trap produced some interesting data on relevant acids in atmospheric aerosol samples. A completely different approach to aerosol sampling, namely, differential mobility analyzer (DMA)-assisted filter sampling, was employed in this study to provide information about the size dependent chemical composition of aerosols and understanding of the processes driving aerosol growth from nano-size clusters to climatically relevant particles (>40 nm). The DMA was set to sample particles with diameters of 50, 40, and 30 nm and aerosols were collected on teflon or quartz fiber filters. To clarify the gas-phase contribution, zero gas-phase samples were collected by switching off the DMA every other 15 minutes. Gas-phase compounds were adsorbed equally well on both types of filter, and were found to contribute significantly to the total compound mass. Gas-phase adsorption is especially significant during the collection of nanometer-size aerosols and needs always to be taken into account. Other aims of this study were to determine the oxidation products of β-caryophyllene (the major sesquiterpene in boreal forest) in aerosol particles. Since reference compounds are needed for verification of the accuracy of analytical measurements, three oxidation products of β-caryophyllene were synthesized: β-caryophyllene aldehyde, β-nocaryophyllene aldehyde, and β-caryophyllinic acid. All three were identified for the first time in ambient aerosol samples, at relatively high concentrations, and their contribution to the aerosol mass (and probably growth) was concluded to be significant. Methodological and instrumental developments presented in this work enable fuller understanding of the processes behind biogenic aerosol formation and provide new tools for more precise determination of biosphere-atmosphere interactions.

Tibetan Written Images : A Study of Imagery in the Writings of Dhondup Gyal

Dhondup Gyal (Don grub rgyal, 1953 - 1985) was a Tibetan writer from Amdo (Qinghai, People's Republic of China). He wrote several prose works, poems, scholarly writings and other works which have been later on collected together into The Collected Works of Dhondup Gyal, in six volumes. He had a remarkable influence on the development of modern Tibetan literature in the 1980s. Examining his works, which are characterized by rich imagery, it is possible to notice a transition from traditional to modern ways of literary expression. Imagery is found in both the poems and prose works of Dhondup Gyal. Nature imagery is especially prominent and his writings contain images of flowers and plants, animals, water, wind and clouds, the heavenly bodies and other environmental elements. Also there are images of parts of the body and material and cultural images. To analyse the images, most of which are metaphors and similes, the use of the cognitive theory of metaphor provides a good framework for making comparisons with images in traditional Tibetan literature and also some images in Chinese, Indian and Western literary works. The analysis shows that the images have both traditional and innovative features. The source domains of images often appear similar to those found in traditional Tibetan literature and are slow to change. However, innovative shifts occur in the way they are mapped on their target domains, which may express new meanings and are usually secular in nature if compared to the religiosity which often characterizes traditional Tibetan literature. Dhondup Gyal's poems are written in a variety of styles, ranging from traditional types of verse compositions and poems in the ornate kāvya-style to modern free verse poetry. The powerful central images of his free verse poems and some other works can be viewed as structurally innovative and have been analysed with the help of the theory of conceptual blending. They are often ambiguous in their meaning, but can be interpreted to express ideas related to creativity, freedom and the need for change and development.

Categorical Meteorological Products: Evaluation and Analysis

In meteorology, observations and forecasts of a wide range of phenomena for example, snow, clouds, hail, fog, and tornados can be categorical, that is, they can only have discrete values (e.g., "snow" and "no snow"). Concentrating on satellite-based snow and cloud analyses, this thesis explores methods that have been developed for evaluation of categorical products and analyses. Different algorithms for satellite products generate different results; sometimes the differences are subtle, sometimes all too visible. In addition to differences between algorithms, the satellite products are influenced by physical processes and conditions, such as diurnal and seasonal variation in solar radiation, topography, and land use. The analysis of satellite-based snow cover analyses from NOAA, NASA, and EUMETSAT, and snow analyses for numerical weather prediction models from FMI and ECMWF was complicated by the fact that we did not have the true knowledge of snow extent, and we were forced simply to measure the agreement between different products. The Sammon mapping, a multidimensional scaling method, was then used to visualize the differences between different products. The trustworthiness of the results for cloud analyses [EUMETSAT Meteorological Products Extraction Facility cloud mask (MPEF), together with the Nowcasting Satellite Application Facility (SAFNWC) cloud masks provided by Météo-France (SAFNWC/MSG) and the Swedish Meteorological and Hydrological Institute (SAFNWC/PPS)] compared with ceilometers of the Helsinki Testbed was estimated by constructing confidence intervals (CIs). Bootstrapping, a statistical resampling method, was used to construct CIs, especially in the presence of spatial and temporal correlation. The reference data for validation are constantly in short supply. In general, the needs of a particular project drive the requirements for evaluation, for example, for the accuracy and the timeliness of the particular data and methods. In this vein, we discuss tentatively how data provided by general public, e.g., photos shared on the Internet photo-sharing service Flickr, can be used as a new source for validation. Results show that they are of reasonable quality and their use for case studies can be warmly recommended. Last, the use of cluster analysis on meteorological in-situ measurements was explored. The Autoclass algorithm was used to construct compact representations of synoptic conditions of fog at Finnish airports.

Thunderstorm climatology and lightning location applications in northern Europe

Thunderstorm is a dangerous electrical phenomena in the atmosphere. Thundercloud is formed when thermal energy is transported rapidly upwards in convective updraughts. Electrification occurs in the collisions of cloud particles in the strong updraught. When the amount of charge in the cloud is large enough, electrical breakdown, better known as a flash, occurs. Lightning location is nowadays an essential tool for the detection of severe weather. Located flashes indicate in real time the movement of hazardous areas and the intensity of lightning activity. Also, an estimate for the flash peak current can be determined. The observations can be used in damage surveys. The most simple way to represent lightning data is to plot the locations on a map, but the data can be processed in more complex end-products and exploited in data fusion. Lightning data serves as an important tool also in the research of lightning-related phenomena, such as Transient Luminous Events. Most of the global thunderstorms occur in areas with plenty of heat, moisture and tropospheric instability, for example in the tropical land areas. In higher latitudes like in Finland, the thunderstorm season is practically restricted to the summer season. Particular feature of the high-latitude climatology is the large annual variation, which regards also thunderstorms. Knowing the performance of any measuring device is important because it affects the accuracy of the end-products. In lightning location systems, the detection efficiency means the ratio between located and actually occurred flashes. Because in practice it is impossible to know the true number of actually occurred flashes, the detection efficiency has to be esimated with theoretical methods.

3D MHD simulations of subsurface convection in OB stars

During their main sequence evolution, massive stars can develop convective regions very close to their surface. These regions are caused by an opacity peak associated with iron ionization. Cantiello et al. (2009) found a possible connection between the presence of sub-photospheric convective motions and small scale stochastic velocities in the photosphere of early-type stars. This supports a physical mechanism where microturbulence is caused by waves that are triggered by subsurface convection zones. They further suggest that clumping in the inner parts of the winds of OB stars could be related to subsurface convection, and that the convective layers may also be responsible for stochastic excitation of non-radial pulsations. Furthermore, magnetic fields produced in the iron convection zone could appear at the surface of such massive stars. Therefore subsurface convection could be responsible for the occurrence of observable phenomena such as line profile variability and discrete absorption components. These phenomena have been observed for decades, but still evade a clear theoretical explanation. Here we present preliminary results from 3D MHD simulations of such subsurface convection.

Mapping Road Infrastructure in Developing Countries Applying Remote Sensing and GIS - The Case of the Taita Hills, Kenya

Road transport and infrastructure has a fundamental meaning for the developing world. Poor quality and inadequate coverage of roads, lack of maintenance operations and outdated road maps continue to hinder economic and social development in the developing countries. This thesis focuses on studying the present state of road infrastructure and its mapping in the Taita Hills, south-east Kenya. The study is included as a part of the TAITA-project by the Department of Geography, University of Helsinki. The road infrastructure of the study area is studied by remote sensing and GIS based methodology. As the principal dataset, true colour airborne digital camera data from 2004, was used to generate an aerial image mosaic of the study area. Auxiliary data includes SPOT satellite imagery from 2003, field spectrometry data of road surfaces and relevant literature. Road infrastructure characteristics are interpreted from three test sites using pixel-based supervised classification, object-oriented supervised classifications and visual interpretation. Road infrastructure of the test sites is interpreted visually from a SPOT image. Road centrelines are then extracted from the object-oriented classification results with an automatic vectorisation process. The road infrastructure of the entire image mosaic is mapped by applying the most appropriate assessed data and techniques. The spectral characteristics and reflectance of various road surfaces are considered with the acquired field spectra and relevant literature. The results are compared with the experimented road mapping methods. This study concludes that classification and extraction of roads remains a difficult task, and that the accuracy of the results is inadequate regardless of the high spatial resolution of the image mosaic used in this thesis. Visual interpretation, out of all the experimented methods in this thesis is the most straightforward, accurate and valid technique for road mapping. Certain road surfaces have similar spectral characteristics and reflectance values with other land cover and land use. This has a great influence for digital analysis techniques in particular. Road mapping is made even more complicated by rich vegetation and tree canopy, clouds, shadows, low contrast between roads and surroundings and the width of narrow roads in relation to the spatial resolution of the imagery used. The results of this thesis may be applied to road infrastructure mapping in developing countries on a more general context, although with certain limits. In particular, unclassified rural roads require updated road mapping schemas to intensify road transport possibilities and to assist in the development of the developing world.

Dependence of the large-scale vortex instability on latitude, stratification and domain size

In an earlier study, we reported on the excitation of large-scale vortices in Cartesian hydrodynamical convection models subject to rapid enough rotation. In that study, the conditions for the onset of the instability were investigated in terms of the Reynolds (Re) and Coriolis (Co) numbers in models located at the stellar North pole. In this study, we extend our investigation to varying domain sizes, increasing stratification, and place the box at different latitudes. The effect of the increasing box size is to increase the sizes of the generated structures, so that the principal vortex always fills roughly half of the computational domain. The instability becomes stronger in the sense that the temperature anomaly and change in the radial velocity are observed to be enhanced. The model with the smallest box size is found to be stable against the instability, suggesting that a sufficient scale separation between the convective eddies and the scale of the domain is required for the instability to work. The instability can be seen upto the colatitude of 30 degrees, above which value the flow becomes dominated by other types of mean flows. The instability can also be seen in a model with larger stratification. Unlike the weakly stratified cases, the temperature anomaly caused by the vortex structures is seen to depend on depth.