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- ItemOverview of the international project on biogenic aerosol formation in the boreal forest (BIOFOR)(Milton Park : Taylor & Francis, 2001) Kulmala, M.; Hämeri, K.; Aalto, P.P.; Mäkelä, J.M.; Pirjola, L.; Nilsson, E. Douglas; Buzorius, G.; Rannik, Ü.; Dal Maso, M.; Seidl, W.; Hoffman, T.; Janson, R.; Hansson, H.-C.; Viisanen, Y.; Laaksonen, A.; O’dowd, C.D.Aerosol formation and subsequent particle growth in ambient air have been frequently observed at a boreal forest site (SMEAR II station) in Southern Finland. The EU funded project BIOFOR (Biogenic aerosol formation in the boreal forest) has focused on: (a) determination of formation mechanisms of aerosol particles in the boreal forest site; (b) verification of emissions of secondary organic aerosols from the boreal forest site; and (c) quantification of the amount of condensable vapours produced in photochemical reactions of biogenic volatile organic compounds (BVOC) leading to aerosol formation. The approach of the project was to combine the continuous measurements with a number of intensive field studies. These field studies were organised in three periods, two of which were during the most intense particle production season and one during a non-event season. Although the exact formation route for 3 nm particles remains unclear, the results can be summarised as follows: Nucleation was always connected to Arctic or Polar air advecting over the site, giving conditions for a stable nocturnal boundary layer followed by a rapid formation and growth of a turbulent convective mixed layer closely followed by formation of new particles. The nucleation seems to occur in the mixed layer or entrainment zone. However two more prerequisites seem to be necessary. A certain threshold of high enough sulphuric acid and ammonia concentrations is probably needed as the number of newly formed particles was correlated with the product of the sulphuric acid production and the ammonia concentrations. No such correlation was found with the oxidation products of terpenes. The condensation sink, i.e., effective particle area, is probably of importance as no nucleation was observed at high values of the condensation sink. From measurement of the hygroscopic properties of the nucleation particles it was found that inorganic compounds and hygroscopic organic compounds contributed both to the particle growth during daytime while at night time organic compounds dominated. Emissions rates for several gaseous compounds was determined. Using four independent ways to estimate the amount of the condensable vapour needed for observed growth of aerosol particles we get an estimate of 2–10×107 vapour molecules cm−3. The estimations for source rate give 7.5–11×104 cm−3 s−1. These results lead to the following conclusions: The most probable formation mechanism is ternary nucleation (water-sulphuric acid-ammonia). After nucleation, growth into observable sizes (~3 nm) is required before new particles appear. The major part of this growth is probably due to condensation of organic vapours. However, there is lack of direct proof of this phenomenon because the composition of 1–5 nm size particles is extremely difficult to determine using the present state-of-art instrumentation.
- ItemEmission fluxes and atmospheric degradation of monoterpenes above a boreal forest: Field measurements and modelling(Milton Park : Taylor & Francis, 2001) Spanke, Jörg; Rannik, Üllar; Forkel, Renate; Nigge, Walter; Hoffman, ThorstenThe contribution of monoterpenes to aerosol formation processes within and above forests is not well understood. This is also true for the particle formation events observed during the BIOFOR campaigns in Hyytiälä, Finland. Therefore, the diurnal variation of the concentrations of several biogenic volatile organic compounds (BVOCs) and selected oxidation products in the gas and particle phase were measured on selected days during the campaigns in Hyytiälä, Finland. α-pinene and Δ3-carene were found to represent the most important monoterpenes above the boreal forest. A clear vertical gradient of their concentrations was observed together with a change of the relative monoterpene composition with height. Based on concentration profile measurements of monoterpenes, their fluxes above the forest canopy were calculated using the gradient approach. Most of the time, the BVOC fluxes show a clear diurnal variation with a maximum around noon. The highest fluxes were observed for α-pinene with values up to 20 ng m−2 s−1 in summer time and almost 100 ng m−2 s−1 during the spring campaign. Furthermore, the main oxidation products from α-pinene, pinonaldehyde, and from β-pinene, nopinone, were detected in the atmosphere above the forest. In addition to these more volatile oxidation products, pinic and pinonic acid were identified in the particle phase in a concentration range between 1 and 4 ng m−3. Beside these direct measurement of known oxidation products, the chemical sink term in the flux calculations was used to estimate the amount of product formation of the major terpenes (α-pinene, β-pinene, Δ3-carene). A production rate of very low volatile oxidation products (e.g., multifunctional carboxylic) from ·OH- and O3-reaction of monoterpenes of about 1.3·104 molecules cm−3 s−1 was estimated for daylight conditions during summer time. Additionally, model calculations with the one-dimensional multilayer model CACHE were carried out to investigate the diurnal course of BVOC fluxes and chemical degradation of terpenes.
- ItemThe feedback of midlatitude waves onto the Hadley cell in a simple general circulation model(Milton Park : Taylor & Francis, 1996) Becker, E.; Schmitz, G.; Geprägs, R.We present self-consistent comparisons of axissymmetric and 3-dimensional simulations of the tropospheric circulation under idealized physical conditions. These reveal a feedback of transient eddies onto the Hadley circulation which, first, strongly depends on equatorial heating and, second, is in case of realistic heating quite different from prescribed eddy forcing. A quantitative estimation for the eddy-induced mixing of vorticity into the poleward flow of the Hadley cell is given. The proposed relation is in accordance with observations. It is derived from the computational result that eddy momentum flux convergence is of the same order as the equatorward flux of relative vorticity generated by the Hadley circulation. Evaluation of the local budgets of sensible heat gives rise to a clear picture of how the poleward heat transports due to Hadley circulation and transient eddies interlock. This mechanism is found to be essential for an interpretation of the eddy feedback.
- ItemThe rôle of orographically and thermally forced stationary waves in the causation of the residual circulation(Milton Park : Taylor & Francis, 1999) Becker, E.; Schmitz, G.Several experiments performed with an idealized troposphere–stratosphere GCM are comparedto estimate the impact of orography and prescribed local heat sources on the residual circulationin the northern winter stratosphere. It is found that only the combined action of orographicand thermal wave forcing in northern midlatitudes is capable of inducing a residual circulationreaching continuously from tropical to polar latitudes at stratospheric altitudes. Intensificationsof the residual circulation in response to modified forcing of stationary waves are generallyassociated with, firstly, a reduced polar night jet accompanied by enhanced easterlies inlow and summer hemispheric latitudes and, secondly, substantial warming of the polar nightstratosphere completely compensated by cooling in the tropics and subtropics.
- ItemVery low ozone episodes due to polar vortex displacement(Milton Park : Taylor & Francis, 2000) James, P.M.; Peters, D.; Waugh, D.W.The large-scale ozone distribution over the northern hemisphere undergoes strong fluctuationseach winter on timescales of up to a few weeks. This is closely linked to changes in the stratosphericpolar vortex, whose shape, intensity and location vary with time. Elliptical diagnosticparameters provide an empirical description of the daily character of the polar vortex. Theseparameters are used as an objective measure to define two characteristic wintertime vortexdisplacements, towards northern Europe and Canada, respectively. The large-scale structuresin both the stratosphere and troposphere and the 3D ozone structures are determined for bothvortex displacement scenarios. A linear ozone transport model shows that the contribution ofhorizontal ozone advection dominates locally in the middle stratosphere. Nevertheless, thelargest contribution is due to vertical advection around the ozone layer maximum. The findingsare in agreement with an EOF analysis which reveals significant general modes of ozone variabilitylinked to polar vortex displacement and to phase-shifted large-scale tropospheric waves.When baroclinic waves travel through the regions of vortex-related ozone reduction, the combinedeffect is to produce transient synoptic-scale areas of exceptionally low ozone; namelydynamically induced strong ozone mini-holes.