Aerosol Basics: Definitions, size distributions, structure

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Aerosol Basics: Definitions, size distributions, structure Antti Lauri NetFAM Summer School Zelenogorsk, 9 July 2008 Department of Physics, Division of Atmospheric Sciences and Geophysics, University of Helsinki

Aerosol particles Liquid or solid particles suspended in a carrier gas Described by their Size Concentration - Number - Surface - Mass - Volume Chemical composition Lifetime seconds years (in troposphere typically hours days)

The Earth s energy balance Kiehl and Trenberth, 1997

Climate effects of aerosols Direct effects Scattering and absorbing short- and longwave radiation Examples: sulphate, organic carbon, black carbon, aerosols from biomass burning, mineral dust Indirect effects Cloud formation: effectiveness of the aerosol acting as cloud condensation nuclei (CCN) Depend on: size, chemical composition, ambient environment Big uncertainty in the effects Longest continuous measurement time series 12 years

IPCC, 2007

Aerosols, clouds and climate Direct effect Indirect (cloud) effect Clean cloud less droplets smaller albedo lower lifetime Polluted cloud more droplets larger albedo longer lifetime (mostly) COOLING 1750 1900 Figure by Ari Asmi / EUCAARI

Indirect climate effects of aerosols

Visibility Antarctica: > 100 km New Delhi: < 1.5 km Pictures: Ismo K. Koponen and Petteri Mönkkönen

Atmospheric Brown Cloud (Pollution)

MODIS 3.5.2006 09:29 http://www.sat. dundee.ac.uk/

Effect on air quality (Helsinki, August 2006) Photos: Pia Anttila, FMI

Aerosols and Health Current estimates show that aerosol particles have significant effect on both life expectancy and life quality

Types of Aerosols Based on their formation processes, aerosols are either primary or secondary: Primary aerosols are directly emitted to the atmosphere. Secondary aerosols are formed in the atmosphere by gas-to-particle conversion processes: Based on their sources, aerosols are either natural or anthropogenic: Natural aerosols are emitted as a result of processes in the nature (windblown dust, pollen, plant fragments, seasalt, seaspray, volcanic emissions) Anthropogenic aerosols are somehow related to human activities (fossil fuel burning, industrial processes, traffic, burning of biomass or biofuel, agricultural activities, etc.)

Small particles Big particles Nanoparticles Gas molecules CCN Light Fog Concrete dust Rain Sand Gravel Cigarette smoke Pollen Viruses Bacteria Hair Traffic Road dust Energy production 0.001 0.01 0.1 1 10 100 1000 Particle diameter μm (1mm) 10 000 (1 cm) Figure by Mikko Moisio and Ilona Riipinen

Structures Asbestos Volcanoes In model calculations, the shape of an aerosol particle is assumed spherical In practice, this is not always the case There are several ways of characterizing real particles with a certain diameter so that some of their features correspond to the features of a spherical particle of the given size Electrical mobility Terminal velocity Density Coal Wielding

Variation of Aerosol Concentrations Concentration varies depending on location and time high concentrations are encountered when there are nearby sources. PN [cm -3 ] PM 10 [μg/m 3 ] Lower troposphere: -Urban traffic -Urban background -Rural -Marine -Remote Free troposphere Stratosphere (background) > 100 000 10 000 50 000 500 10 000 200 5000 50 500 100 100 000 1 20 >20 20 100 10 50 5 20 0.02 1

Aerosol size distributions The total concentration of atmospheric aerosol particles can vary over 7 orders of magnitude (~10 1 ~10 8 #/cm 3) The size range spans over 5 orders of magnitude (~1 nm ~100 μm) Size affects both the lifetime and the physical and chemical properties How to describe the aerosol size and number/area/volume in a simple way? Aerosol size distribution

#/cm 3 nucleation Aitken accumulation coarse ~10 1 molec. ~10 9-10 12 molec. Marine Remote continental Urban Free troposphere 10nm 100nm 1000nm Diameter From gases primary combustion Dust, sea salt, cloud droplets Figure by Hanna Vehkamäki and Veli-Matti Kerminen

Lognormal distribution function It has been observed that atmospheric aerosols can be described rather well with a set of log-normal distribution functions (log-normal = normally distributed in logarithmic scale) n N ( log D ) p = n i= 1 ( 2π ) N 1/ 2 i logσ i exp ( log D log D ) pi p 2log 2 σ i 2 n N (log D p ): number of particles of diameter D p N i : number concentration of particles in the mode σ i : geometric standard deviation D pi : median diameter of the mode

Representations of Aerosol Concentrations Aerosol particle concentrations can be expressed by Number, Surface area, Volume, or Mass per unit volume: The number concentration is (in most cases) dominated by the ultrafine aerosols. The mass or volume concentration is dominated by the coarse and accumulation aerosols. Representation of number and volume aerosol size distributions Figure from Seinfeld & Pandis, 2006

Urban aerosol Mixture of primary emissions from industry, transportation, power generation, and natural sources and secondary aerosols through gas-to-particle conversion Number concentration dominated by ultrafine particles Surface area mostly in the 0.1-0.5 μm sizes Mass typically has two dominating modes: accumulation and coarse Huge variation depending on the measurement site and current meteorological conditions Typical urban aerosol size distribution Figure from Seinfeld & Pandis, 2006

Rural aerosol Mainly of natural origin, but with some influence of anthropogenic sources Number concentration typically has two dominating modes in the ultrafine size range Surface area mostly in the 0.1-0.5 μm sizes Mass dominated by coarse mode Typical rural aerosol size distribution Figure from Seinfeld & Pandis, 2006

Remote continental aerosol Mainly natural primary particles including dust, pollen, plant waxes and secondary oxidation products Number concentration typically has two dominating modes (nucleation mode, accumulation mode) Surface area mostly in accumulation mode Mass dominated by accumulation mode Typical remote continental aerosol size distribution. Figure from Seinfeld & Pandis, 2006

Marine aerosol Mostly of marine origin: evaporation of seaspray, seasalt, secondary aerosols formed after oxidation of dimethyl sulfide emitted by phytoplankton Number concentration typically has two dominating modes around 60 nm and 200 nm Mass dominated by coarse mode Marine aerosol size distributions from different measurements and a model distribution. Figures from Seinfeld & Pandis, 2006

Free tropospheric aerosol Mid- and upper troposphere above clouds Modes around 10 nm and 250 nm Number concentration of accumulation mode particles typically higher than in the lower troposphere No precipitation scavenging Nucleation mode often present Suitable conditions for new particle formation Typical free tropospheric aerosol size distribution. Figure from Seinfeld & Pandis, 2006

Polar aerosol Very low total concentrations Accumulation mode dominates Arctic haze during the winter and early spring: anthropogenic sources Composition: aged carbonaceous aerosols originated from midlatitude pollution sources, sulfate, seasalt, mineral dust Typical polar aerosol size distribution. Figure from Seinfeld & Pandis, 2006

Desert aerosol Three overlapping modes at 10 nm, 50 nm, and 10 μm Surface area and volume strongly dominated by windblown sand Individual dust storms can transfer desert aerosol over the ocean Typical desert aerosol size distribution. Figure from Seinfeld & Pandis, 2006

Parameters for model aerosol distributions

Processes Modifying Atmospheric Aerosols Processes affecting the concentration and other properties (size, chemical composition) of atmospheric aerosols include: Emissions (primary particles, emissions of aerosol precursor gases) Atmospheric transportation Deposition from the atmosphere to surfaces (ground, vegetation, water) Aerosol dynamics and chemistry

Cloud/fog formation RH > 100% Due to cooling (isobaric/adiabatic) Isobaric cooling (pressure remains constant) Radiative losses of energy, horizontal movement of an airmass over a colder land surface or colder airmass Adiabatic cooling (no heat exchange) Ascending air parcel pressure decrease, volume expansion, temperature decrease

Cloud/fog formation Droplet formation without existing nuclei would require considerable supersaturations e.g. pure water: RH 300-500% Aerosol particles that can facilitate droplet formation at low supersaturations are called cloud condensation nuclei (CCN)

Köhler theory Two effects A smaller droplet has higher equilibrium vapour pressure due to curvature (Kelvin effect) A solution has lower equilibrium vapour pressure than a pure substance Köhler theory: combination of two expressions Kelvin equation Raoult s law Modified versions of the Köhler theory available for soluble trace gases, slightly soluble substances and surface-active solutes

Köhler curves

Cloud droplet composition Liquids Water (solvent) Dissolved compounds, e.g. O 3 (aq), H 2 O 2 (aq) Ions, e.g. SO 2-4, NH + 4 Solids Soluble compounds, e.g. ammonium sulfate Slightly soluble compounds, e.g. organic acids, calcium sulfate Insoluble compounds, e.g. dust, elemental carbon Condensing gases e.g. H 2 O, HNO 3, NH 3, SO 2, H 2 O 2

Mixing state of the aerosol Important when determining e.g. CCN solubility or aerosol optical properties External mixture: each particle from only one source Internal mixture: all the particles of a certain size contain a uniform mixture of components from each source

nm 100 An example of time evolution 10 of size 1.Apr distribution in 30.Apr Hyytiälä A new particle formation event New particles appearing in the 3-25 nm size range (A) B A Newborn particles growing, sometimes to sizes where they can act as cloud condensation nuclei (B)

Formation dynamics Pre-existing aerosol Vapor sink (condensation) Particle sink (coagulation) 3 nm Growth by condensation Particle source (nucleation) Vapor source (e.g. organics+ hν, sulphuric acid) Activation to CCN Figure by Miikka Dal Maso and Ilona Riipinen

Condensation & Coagulation sinks Condensation sink (CS) describes the aerosol population s ability to remove vapor by condensation CS = 4π D 0 r β M (r) n(r) dr = 4π D i β M r i N i Coagulation sink (CoagS(D p )) describes the aerosol population s ability to remove particles of size D p CoagS(D Sinks sensitive to particle size changes hygroscopic growth must be accounted for p ) = D p K(D p,d p ',T,...) n(d p ) dd p