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University of Zimbabwe Faculty of Science University of Zimbabwe Faculty of Science Atmospheric aerosol particles and transport: a climatological perspective for Zimbabwe by Daniel NYANGANYURA The thesis is submitted in partial fulfilment of the requirements for the Doctor of Philosophy Degree 2006 To my wife Maybe and to our two boys Pedro and Danilo who always give me the will to go on, and to my parents who although they lived in a different epoch, have contributed to what I became. Abstract Atmospheric aerosol particles were collected in the coarse (2-10 µm diameter) and fine (< 2 µm diameter) size fractions at Rukomechi research station, (16.1 °S, 29.4 °E, 500 m a.s.l.), northern Zimbabwe from September 1994 to January 2000. The collected samples were analysed for particulate mass (PM), black carbon and 47 elements at the Gent Institute for Nuclear Sciences. The main sources of coarse and fine aerosols were found to be crustal matter, sea salt and biomass burning for both wet and dry seasons. However, additional sources for copper and biogenic aerosols were detected during the wet and dry seasons, respectively, while anthropogenic influences were only found in the fine aerosols. The Absolute Principal Component Analysis (APCA) attributed 29% of the total wet season coarse particulate mass to the mixed biogenic/biomass burning component, while the major contribution (32%) was attributed to biomass burning during the dry season. The biomass burning component also provided the major contribution to the total fine particulate mass, accounting for 44% and 79% in the wet and dry seasons, respectively. The climatology of air mass transport to northern Zimbabwe was examined through an analysis of 5-day kinematic back trajectories arriving daily at Rukomechi at ~ 850 hPa for the period of 1994 to 1999. Classification of trajectories into different flow regimes was done using a non-hierarchical cluster algorithm. The dominant transport features include the eastern corridor, the south-east corridor, southern and north north-westerly flows, as well as regionally re-circulated air. The eastern corridor is comprised of fast and slow air masses that contribute 35% of the total number of trajectories. The air masses in these corridors bring late dry season to wet season air masses driven by an anticyclone that wraps around the subcontinent and stretches into the Mozambique Channel. The south-east corridor is also composed of fast and slow winds that contribute late wet season to dry season air masses and account for 44% of the total number of trajectories. These winds are associated with the Atlantic Ocean anticyclone and the Indian Ocean tropical depression. The fast dry season southern flow contributes 8% of the total number of trajectories and is driven by a continental anticyclone over South Africa coupled to an Atlantic Ocean anticyclone. The north north-westerly flow contributes least to the total number of trajectories (6%) and is associated with Inter- Tropical Convergence Zone while the regionally re-circulated air, as a result of differential heating at the surface, is the slowest. Of the seven air flows, only four were found carrying air significantly loaded with aerosols to northern Zimbabwe. These are namely: the fast easterly that carries aerosols mainly from biomass burning related sources; the slow south easterly that is associated with aerosols from various sources; the southerly containing mineral dust, sea salt and anthropogenic aerosols; and the regional flows that contain aerosols of anthropogenic origin. The potential sources of biomass burning aerosols were found to be due to fire activities from northern Zimbabwe and central Mozambique. The other pathways carry anthropogenic aerosols, especially copper (from areas around the Copper-belt regions), sulphur (from South African industrial areas), and lead (from the major Southern African road network). i Acknowledgements I am grateful for the contributions of several institutions and individuals who made this PhD thesis possible. I am grateful to the University of Zimbabwe, Department of Physics, for giving me the opportunity to do my PhD study. I am gratefully indebted to the German Academic Exchange Service (DAAD) and the Max Planck Society (partially through the Max Planck International Research School of Atmospheric Chemistry and Physics) for the financial support provided during the course of this research and to the Belgian Federal Science Policy Office for the financial support for the aerosol chemical analysis. I regard myself very privileged to have the opportunity to carry out this research under the guidance of my supervisors Dr A. Makarau, Dr M. Mathuthu and Prof F. X. Meixner. I’m particularly indebted to Prof F. X. Meixner whose commitment to my work is unmatched, and I appreciate his guidance, wisdom, and attention to detail. Big thanks also go to the Max Planck Institute for Chemistry, Biogeochemistry department group members, my office colleague Dr Ivonne Trebs and particularly to Dr. Günter Helas, for their unwavering support and for providing me with an excellent research environment. I am also indebted to Prof Meinrat O. Andreae who supported my studies and also provided logistical support. My gratitude also goes to Prof. W. Maenhaut (Institute of Nuclear Sciences, University of Gent, Belgium) for his assistance with data analysis, his valuable advice and support. I am also grateful to Prof. H. Wernli (Institute of Atmospheric Sciences, University of Mainz, Germany) for his valuable help and advice, and the European Centre for Medium Range Weather Forecasting for providing data for plotting the surface pressure maps and Dr G. Kirkman whose assistance in developing the fire plot procedure was very valuable and Dr A Lupu for developing the potential source contribution function procedure that was used in this study. I also thank M.-T. Fernández-Jiménez, I. Rajta, S. Dubtsov, D.J.A. De Ridder and N. Raes from Ghent University for the chemical analyses of the samples. I am also grateful to P. Chimanga, M. Chiranda and J. Mlambo from the Tsetse Control Branch, Harare, Zimbabwe, for collecting the aerosol samples at the Rukomechi site. I also thank Dr. Steve Torr (Natural Resources Institute, Chatham/U.K.) for providing the 1992-1999 data set of the automated meteorological station at Rukomechi. Finally, I would like to express my heart-felt gratitude to my wife, Maybe and our three boys Pedro, Danilo and Daniel Junior (a family that made a difference) for tolerating years of my absence from the family. ii Table of contents Abstract ......................................................................................................................... i Acknowledgements............................................................................................................... ii List of tables ....................................................................................................................... vi List of figures ...................................................................................................................... vii Chapter 1 Introduction.................................................................................................. 1 1.1 Background .......................................................................................................................... 1 1.2 Motivation for the research................................................................................................. 2 1.3 Objectives of the research ................................................................................................... 3 1.4 Layout of the chapters......................................................................................................... 4 Chapter 2 Theory .......................................................................................................... 5 2.1 Aerosols................................................................................................................................. 5 2.2 Sources of aerosols ............................................................................................................... 7 2.2.1 Mineral dust aerosols .......................................................................................................................8 2.2.2 Biogenic aerosols .............................................................................................................................8 2.2.3 Anthropogenic aerosols....................................................................................................................9 2.2.4 Marine aerosols ................................................................................................................................9 2.2.5 Biomass burning.............................................................................................................................10 2.3 Effects of aerosols............................................................................................................... 11 2.3.1 Direct and indirect effect on climate..............................................................................................11 2.3.2 Aerosol effects on human health and environment .......................................................................13 2.4 Aerosol sampling................................................................................................................13 2.5 Physical and elemental analysis of aerosols..................................................................... 16 2.5.1
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