from bulk-mass towards size resolved aerosols

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Presentation transcript:

from bulk-mass towards size resolved aerosols EMEP-MAFOR: from bulk-mass towards size resolved aerosols (Matthias Karl and Svetlana Tsyro) TFMM 16-th meeting Kraków, Poland, May 5-8, 2015

Motivation Knowing the aerosol number concentrations (NC) and size distribution is highly relevant for studies of: Health implications of air pollution: “epidemiological and toxicological studies show clear correlation between ultrafine particles (UF) and health endpoints “ Daher et al., Environ. Science, 2013 Note: UF particles contribute negligibly to PM mass – described by PNC Aerosol optical properties and radiative effects Estimations of climate relevant effects of aerosols, acting as SLCF AOD and aerosol extinction profile measurements from satellite and ground-based instruments offers new opportunity for models’ evaluation (global coverage, high resolution, 3D) and for adequate modelling of aerosol processes such as aerosol- clouds interaction, formation of new particles and secondary aerosols, dry deposition .. Knowing the aerosol size distribution on high temporal and spatial resolution is of great importance for the assessment of health risks from air pollution. Ultrafine particles, ie the small particles of less than 100 nm size contribute negligible to the particle mass, and are better represented in terms of particle number. UFP penetrate deep into the lung, where they can accumulate in the lymph nodes. Although causal relationships are not proven, there is increasing evidence for a correlation between UFP and health end points.

MAFOR Aerosol Dynamics Solves size distribution of a mixed multicomponent aerosol on a fixed sectional grid (1 nm – 10 µm; 16 – 60 bins tested) Consistent time integration of particle number and mass concentrations Flexible with respect to number of size sections and aerosol components; and computationally efficient Stand-alone module – easily implemented Documentation: Karl et al., Tellus, 2011; http://mafor.nilu.no Evaluated with chamber data, nucleation event observations on central Arctic Ocean (Karl et al., 2012), PNC measurements at motorway (Keuken et al., AE, 2012) EMEP-MAFOR: still on-going work (first report EMEP Status Report 1/2014) evaluated with continuous PNC and size distribution 2008-2010 (EUCAARI/EUSAAR) + campaigns/episodes (from 2003 onwards) Presented at several conferences (EAC-2013, IAMA-2013, IAC-2014, EGU-2014)

Computational structure of EMEP-MAFOR Gas emissions Advection PM emissions SO2 NOx NH3 Gas & aqueous chemistry EC POM PMXX(n) Sea salt Min. Dust H2SO4 LV Org VOC MARS (Equilibrium) Inorg. dust SO4, HNO3/NO3, NH3/NH4 SOA (VBS) MAFOR Aerosol Dynamics Nucleation Condensation Coagulation dPNC(n)/dt dSO4(n)/dt, dSOA(n)/dt PMXX gmd(m)  nucl 0.008 1.45 Ait 0.080 1.7 acc 0.300 1.7 coar 3.0 1.8 AFT: aerosol formation treatment ADM: aerosol dynamic model Output: PM2.5, PM10, PNC, number size distribution (16bins) + chem. composition (4 modes) Dry /wet deposition

Model: particle number and mass concentrations 2008 mean Total PNC PM2.5 Nucleation PNC Aitken PNC Accumulation PNC

EMEP-MAFOR evaluation with measurements: Asmi et al. Year: 2008 (annual/seasonal PNC & size distribution) EUSAAR/ACTRIS/EBAS: Year 2010, dN/dlogDp SPC (San Pietro Capofiume): Year 2010, dN/dlogDp SmartSMEAR (Hyytiälä) : Summer 2010, VOC, H2SO4, OH Ny_Alesund2 Pallas Hyytiala Birkenes Aspvreten Vavihill MaceHead Waldhof Harwell Finokalia Zugspitze Jungfraujoch Hohenpeissenberg Puy_deDome Schauinsland Mt_Cimone Melpitz Kosetice K_Puszta Boesel Cabauw Ispra Modelled vs. observed total PNC (d>10nm) in 2008 Measurements as in Asmi et al., ACP, 2011 Model compared to measured PNCs: Underestimates at polluted sites (C. Europe) Quite close at less polluted sites (N. Europe) Overestimates at mountain sites 1:1 ISP Modelled total PNC for EUSAAR sites correlate quite well with observations presented by Asmi et al. 2011 (available through the link here). It shows very good agreement for many remote sites including the mountain sites – while PNC at more polluted sites are underestimated by roughly a factor of two. KPT MPZ CBW BOS OBK

Seasonal median size distribution (2008) Birkenes Hyytiälä O Modelled PNCs compared to the measurements: bimodal size distribution (observed is closer to unimodal) Discrepancies in seasonality Summer: too many newly formed particles <20nm, whereas too few > 50nm. Indicates slow growth Winter: quite close at cleaner sites, but too low at polluted sites (wood burning for residential heating?? Melpitz Ispra O O Looking at seasonal median size distributions from European sites, modelled size distributions show a distinct bimodal shape while in particulat at the more polluted sites Ispra, K-Puszta and Melpitz the observations resemble an unimodal distribution. At these sites, particles between 50-500 nm are underestimated, which points to missing biomass burning emissions in winter and in summer, not represented in the EMEP model. For the remote sites, EMEP-MAFOR does not capture secondary particle formation in summer. Despite the particles are formed in the model – they just did not grow to the observed sizes.

Nucleation Event Frequency The Frequency of new particle formation events defined as fraction of event days in each month for the selected sites Hyytiala, SP Capofiume, Birkenes in Norway and Pallas in N.-Finland. Blue bars are observed event day fraction, red for Reference simulation, green for BIO and orange for SO4 Tests. On average BIO overestimates the number of events, in particular in summer.

Birkenes, 2010 (EBAS) OBS MODEL Total PNC (>10nm) PN distribution PNC evolution Total PNC (>10nm)

Hyytiälä, 2010 (EBAS) OBS MODEL Total PNC (>10nm) PN distribution PNC evolution Total PNC (>10nm)

AOD & Extinction profiles Bulk-mass aerosol 3D concentrations of fine and coarse aerosols Specific Extinction Efficiencies for aerosol components (Hess et al, 1998) Effective cross-sections; implicit account for the effect of relative humidity (Chin et al, 2002) Size-resolved aerosol (using Mie-theory) Effective complex refractive index- volume weighted for internal mixture: Bruggeman (1935) mixing rule for homogeneous mixtures (Chylek et al., 2000); Maxwell&Garnett (1904) rule for EC and min. dust inclusions Extinction Efficiency from Mie-scattering look-up table Applied to particles distribution in 4 size modes – provisionally!! First evaluation of AOD with satellite / AERONET sun-photometer data and extinction vertical profiles with EARLINET LIDAR data

42% overestimation …. despite general underestimation of aerosol mass AOD at 550 nm (2012) EMEP-MAFOR EMEP bulk-mass AATSR (2011) Bias map Bias map 25% underestimation … can be explained by PNC underestimation and provisional Mie-implementation 42% overestimation …. despite general underestimation of aerosol mass

AOD 550nm: Model vs. AERONET EMEP bulk-mass EMEP-MAFOR Correlation Correlation Spatial 0.56 0.68 Correlation

EMEP-MAFOR calculated aerosol extinction profiles compared with EARLINET measured (533 nm; seasonal means 2012)

Summary of main findings First results from EMEP-MAFOR for PNC and size distribution are in fair agreement with observations…given the model is still under development. A number of caveats: Discrepancy in PNC seasonality: Summer – too many of smallest (<20 nm) particles and too few of >50 nm in the model Model predicts too frequent new particle formation in summer with efficient initial growth 1-5 nm to 15-20nm, which then then stops Winter – model max for >50nm (largely due to seasonal variation of anthropogenic emissions), observed max - summer Missing particle sources in winter (wood burning for residential heating) and in summer (agricultural residuals burning, SOA from Biogenic VOSc EMEP-MAFOR currently underestimated 50-200 nm sized particles in summer, independent of nucleation & condensation configuration. Based on the event analysis it cannot be decided whether biogenic or aromatic organics are involved in nucleation. However, on average too many events are predicted if nucleation depends on biogenic organics. We have indications that EMEP model’s BVOC chemistry at night is the reason for interruption of particle growth during simulated events at Hyytiala.

«Golden Day Events» Hyytiälä, 24-30 March 2003 Observations: Figure from: O’Dowd et al., ACP, 2009 Model (Ref): Growth stops in the night Now let’s have a look at the event series, the Golden Days from March 2003, showing a series of banana type growth. The sequential plot for the same time period from the reference simulation reveals that practically almost all features of the observed distribution are captured by the model, although with somewhat lower numbers. The timing is perfect. But: Growth of the particles stops at the beginning of the night. We are still in the process of further investigating this. The most likely reason is the monoterpene chemistry in the model at night. The growth of nucleated particles terminates too early BVOC chemistry at night identified as possible reason for interruption of particle growth and the improvements have recently been made

Summary of main findings EMEP-MAFOR reasonably describes AOD (satellites, AERONET) and Extinction profiles (EARLINET) EMEP standard model tends to overestimate AOD (30- 40%) though the aerosol mass is underestimated – exaggerated effect rel. humidity?? EMEP-MAFOR underestimates AOD ( by 25%) Can be explained by underestimation of Aitken/ accumulation PNC, missing SOA contribution, uncertainties in anthropogenic PN

Outlook of further development: Improvement of size distribution calculations: improvement of SOA formation (more testing BVOC and aromatic VOCs with measurements) Implementation of size-resolved PM emissions implementation of dynamic formation of size resolved ammonium nitrate (condensation-evaporation) Improvement of extinction: Calculate Mie-scattering based on full size distribution (16 sections) using improved refractive indices Comparison with multi-year measurements of AOD and Extinction profiles (satellites, Aeronet, Earlinet etc.)

Thank you for your attention! EMEP-MAFOR currently underestimated 50-200 nm sized particles in summer, independent of nucleation & condensation configuration. Based on the event analysis it cannot be decided whether biogenic or aromatic organics are involved in nucleation. However, on average too many events are predicted if nucleation depends on biogenic organics. We have indications that EMEP model’s BVOC chemistry at night is the reason for interruption of particle growth during simulated events at Hyytiala.