Sources and distribution of sea salt aerosol from the Tropics to the Poles

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1 Sources and distribution of sea salt aerosol from the Tropics to the Poles Lyatt Jaeglé Department of Atmospheric Sciences University of Washington, Seattle contributions from present and past graduate students: Jiayue Huang, Maurizio Di Pierro Collaborators Patricia Quinn Pacific Marine Environmental Laboratory, NOAA, Seattle Tim Bates Pacific Marine Environmental Laboratory, NOAA, Seattle Becky Alexander Dept. Atmospheric Sciences, University of Washington What is the distribution of sea salt aerosol over the world s oceans and in polar regions?

2 Sea salt aerosol Plays important roles in chemistry and climate of marine atmosphere Climate Scattering sunlight: 35-80% of light extinction in marine atmosphere; ~50% globally TOA radiative forcing: -0.5 to -5 W/m 2 Dominant source of cloud condensation nuclei Influence forcing from anthropogenic aerosols Chemistry Sink of gases and aerosols (sulfur/ nitrogen/mercury cycles) Source of trace gases (bromine, chlorine) Source of organic aerosols Site for heterogeneous chemical reactions Halogen activation (Cl2, BrCl, Br2, ClNO2) indirect effect CCN Nitrogen (HNO3, N2O5) Sulfur (H2SO4, SO2) hν O3, CH4, hydrocarbons, DMS, mercury Emission Deposition

3 Sea spray aerosol formation Sea spray is produced by windinduced wave breaking and bubble bursting film jet Spume droplets (>20 µm) (wind tearing off breaking wave crests) direct Lewis & Schwartz (2004) Film droplets (<1 µm) Jet droplets (1-20 µm) indirect (bubble bursting)

4 Emissions of sea salt aerosol (SSA) Laboratory (wave tanks + bubble air) & surf zone observations Conflicting results for sea salt source functions, large uncertainties at small (<0.1μm) and large (>5 μm) sizes Emissions proportional to windspeed ~ u emissions affected by accuracy of windspeed (2006) df/dlog(r) (m -2 s -1 ) m (2003) (2006) (2001) O Dowd & De Leeuw, Phil. Trans. R. Soc. A. (2007) 1 [Monahan and O Muircheartaigh, 1980] 8 source functions for SSA production CCN scatteringchemistry radius (μm)

5 Sea salt emissions & burden estimates Emissions remain highly uncertain: 5,000 Tg/yr (x/ 4) [Lewis & Schwartz, 2004] 16 chemical transport model intercomparison: Sea salt burdens ranged from 3 to 18 Tg (mean±standard deviation: 7.5±4 Tg) [Textor et al., 2006] Comparison of sea salt emissions in 12 models: 2,000 Tg/yr ~ 10,000 Tg/yr De Leeuw et al., Rev. Geophys. (2011)

6 This study Goal: Improve constraints on emissions + burden of sea salt aerosols In situ observations of sea salt mass concentrations Satellite observations of aerosol optical depth GEOS-Chem global chemical transport model NOAA RV Ron Brown Aqua Satellite MODIS GEOS-Chem model Surface observations

7 Observations & Model In situ measurements of sea salt mass concentrations: 6 PMEL cruises ( ) 15 stations, U. Miami network [Savoie & Prospero, 1977] 4 stations in polar regions: Barrow, Alert, Neumayer, Dumont d Urville QuikSCAT annual mean surface wind speed (m s -1 ) GEOS-Chem model GEOS-5 and Merra NASA GMAO meteorology, 2ºx2.5º Aerosol-oxidant simulation: O3-NOx-hydrocarbons, aerosol precursors (SO2, NH3); aerosols (sulfate-ammonium-nitrate, black carbon, organic carbon, dust, sea salt) Sea salt simulation Gong (2003) sea salt source function 2 bins: rdry= μm, μm

8 Comparison to PMEL cruises: Pacific RITS (1993) MODEL Coarse mode sea salt obs SST Model too high over Roaring Forties & N. Pacific Model too low over tropical Pacific ACE1 (1995) Wind speed (m s -1 )

9 Comparison to PMEL cruises: Atlantic & Indian MODEL ICEALOT (2008) Coarse mode sea salt obs Model x2-3 too high over N. Atlantic Model too low over tropical Atlantic & Indian Ocean Aerosols99-INDOEX (1999) Wind speed (m s -1 )

10 Dependence of model bias on SST PMEL coarse mode u10m>6 m s -1 Ratio of observed to modeled sea salt mass concentrations as a function of SST 3 rd order polynomial fit cold waters (<10ºC) model > obs warm waters (>23ºC) model < obs

11 Potential physical mechanisms for SST dependence of SSA production seawater properties kinematic viscosity of seawater decreases by a factor of 2.2 between 0ºC and 30ºC at warmer SST (lower viscosity) air bubbles rise faster to the surface T influence on gas-exchange (bubbles/water) number and size distribution of bubbles reaching surface depend on temperature. kinematic viscosity x10 7 m 2 /s temperature, C lab and field observations increasing SSA production (r>0.5 µm) with increasing water temperature: x2 3 increase between 5 C and 25 C [Bowyer, 1984; Bowyer, 1990; Woolf et al., 1987; Mårtensson et al., 2003] whitecap coverage increases with water temperature [Bortkovskii,1983] number of particles produced Bowyer [1990] temperature, C

12 Dependence of model bias on SST PMEL coarse mode u10m>6 m s -1 Ratio of observed to modeled sea salt mass concentrations as a function of SST 3 rd order polynomial fit cold waters (<10ºC) model > obs warm waters (>23ºC) model < obs Derive a new empirical sea salt source function by multiplying Gong (2003) by SST dependent scaling factor (3 rd order polynomial) Improved simulation: standard (+64%, r=0.55) vs new SST model (+33%, r=0.71) Jaeglé et al. Global distribution of sea salt aerosols: New constraints from in situ and remote sensing observations, ACP, 2011.

13 U. Miami stations confirm SST dependence Tropical stations have significant model underestimate High southern latitude stations display large model overestimate New SST source function: model bias reduced from +32% to -5% Sea surface temperature SST MODEL Standard MODEL Obs. sea salt mass Standard MODEL SST MODEL

14 MODIS Aqua Coarse AOD MODIS Aqua AOD ( ) exclude cloud fraction>50% Standard Model SST-dependent Model dust + coarse mode sea salt Standard model overestimates AOD over high latitude oceans & underestimates AOD over tropical oceans Empirical SST source function reproduces spatial pattern of AOD better

15 What about polar regions?

16 What about polar regions? Comparison to in situ mass concentration observations Barrow, Alaska (71 N, 157 W) submicron sea salt aerosol Obs 0.57 μg/m 3 Model 0.08 μg/m 3 SSMI sea ice concentration December Neumayer, Antarctica (71 S, 8.3 W) sea salt aerosol Obs 1.0 μg/m 3 Model 0.73 μg/m 3 SSMI sea ice concentration June Modeled sea salt has wrong seasonality and is 5-10 times too low during winter!

17 Sources of sea salt over sea ice? High interest in potential sources of sea salt in polar regions: origin of bromine radicals surface ozone and mercury depletion events Two proposed sources of sea salt aerosol over sea ice: wind-blown frost flowers [Rankin et al., 2002] and/or sublimation of salty blowing snow [Yang et al., 2008] Source of sea salt ions in the polar boundary layer Blowing snow event in Arctic Abbatt et al., Atmos. Chem. Phys. (2012) Halogen activation via interactions with environmental ice and snow in the polar lower troposphere and other regions Photo Credit: Vicki Sahanatien

18 Blowing snow source in GEOS-Chem Following Yang et al. (2008), we implement the bulk blowing snow sublimation flux of Déry and Yau (1999, 2001): Qs=f(RH, u10m, temp, snow age). We assume a snow salinity of 0.1 psu (Arctic) 0.03 psu (Antarctic) and 5 sea salt particles/snowflake. Submicron sea salt aerosol emissions Arctic (>60 N) open ocean = 0.98 Tg/year blowing snow = 1.01 Tg/year Winter SSA emissions (<1μm) open ocean blowing snow Antarctic (>60 S) open ocean = 1.7 Tg/year blowing snow = 2.3 Tg/year kg/km 2 /d Blowing snow emissions in polar regions: x2-3 increase in submicron emissions Huang and Jaeglé, Improving constraints on the sources and distributions of sea salt aerosol in polar regions, in prep.

19 Barrow With blowing snow source Neumayer Alert Barrow, Alaska (71 N) Obs 0.57 μg/m 3 Model 0.08 μg/m 3 +blowing snow 0.44 μg/m 3 blowing snow model Dumont d Urville Neumayer (71 S) Obs 1.0 μg/m 3 Model 0.73 μg/m 3 +blowing snow 1.32 μg/m 3 blowing snow model Alert, Canada (82 N) Obs 0.52 μg/m 3 Model 0.13 μg/m 3 +blowing snow 0.7 μg/m 3 Dumont D Urville (67 S) Obs 1.2 μg/m 3 Model 1.2 μg/m 3 +blowing snow 1.9 μg/m 3 Next steps: impact of assumptions on snow salinity, first-year vs multi-year sea ice; comparison satellite observations: CALIOP onboard CALIPSO

20 µg/m Global distribution of sea salt aerosol Surface sea salt concentrations (submicron) Standard model SST model surface concentrations (µg/m 3 ) Standard model SST model SST+blowing snow + Blowing snow <10% change in global sea salt emissions and sea salt burden, but Large spatial shift: 40% decrease in burden at mid lats; 50% increase in tropics; very large increase poleward of 70 N/S

21 Funding: NASA Atmospheric Composition and Modeling Analysis Conclusions & implications Evidence for sea surface temperature dependence of coarse mode sea salt aerosol emissions across multiple data sets Source from blowing snow needed to explain observed sea salt aerosol in winter over polar regions New view of sea salt distribution. Implications: stronger halogen source in tropics & sea ice covered regions stronger radiative forcing of sea salt aerosols larger response to climate change? surface concentrations (µg/m 3 ) Standard model SST model SST+blowing

22 Funding: NASA Atmospheric Composition and Modeling Analysis Conclusions & implications Evidence for sea surface temperature dependence of coarse mode sea salt aerosol emissions across multiple data sets Source from blowing snow needed to explain observed sea salt aerosol in winter over polar regions New view of sea salt distribution. Implications: stronger halogen source in tropics & sea ice covered regions stronger radiative forcing of sea salt aerosols larger response to climate change? Ice core at Dome C: Sea salt flux surface concentrations (µg/m 3 ) Standard model SST model SST+blowing ssna+ flux δd (temperature) Wolff et al. (2000)

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