Southern Ocean MBL CCN Budget: Contribution from Primary Sea Spray Aerosol Organics. Trish Quinn NOAA PMEL
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1 Southern Ocean MBL CCN Budget: Contribution from Primary Sea Spray Aerosol Organics Trish Quinn NOAA PMEL
2 Marine Biota Climate Feedback Loop Charlson et al., Nature, Aerosol Indirect Effect Cloud Condensation Nuclei (CCN) SO 4 = Particle growth condensation, coagulation, cloud processing Cloud Droplets (increased cloud albedo) decreased surface temperature decreased incident radiation H 2 SO 4 DMS DMS Biological activity Wind speed Phytoplankton Production of DMS (+/?)
3 ACE 1: First Aerosol Characterization Experiment Southern Ocean, November December 1995
4 ACE 1: First Aerosol Characterization Experiment Southern Ocean, November December 1995 Overarching goals: Determine the amount of biogenic sulfur (DMS) released from the ocean to the atmosphere. Assess the rates and efficiencies of sulfur gas oxidation in the marine atmosphere. Investigate the rates and efficiencies of the processes controlling the formation, growth, distribution, and removal of particles in the marine atmosphere.
5 ACE 1: First Aerosol Characterization Experiment Southern Ocean, November December 1995 Overarching goals: Determine the amount of biogenic sulfur (DMS) released from the ocean to the atmosphere. Assess the rates and efficiencies of sulfur gas oxidation in the marine atmosphere. Investigate the rates and efficiencies of the processes controlling the formation, growth, distribution, and removal of particles in the marine atmosphere. But what came out of ACE 1 was evidence for sources of CCN beyond DMS and particle nucleation in the Marine Boundary Layer (MBL).
6 ACE 1: Sea salt number size distribution based on single particle analysis Based on single particle mass spectrometry measurements at Cape Grim: Unreacted sea salt Unreacted sea salt dominates the particle number concentration 30 to 100 sea-salt containing particles cm -3 Very few pure sulfate particles CCN size range TEM analysis on samples collected on MacQuarie Island revealed the occurrence of sea salt containing particles at the smallest detectable diameter of 80 nm. (Murphy et al., Nature, 1998)
7 Sea salt recognized as a source of CCN to the Southern Ocean MBL In addition, single particle mass spectrometer measurements detected internally mixed particles containing sea salt and organics for Dp > 160 nm. (Middlebrook et al., JGR, 1998)
8 ACE 1: Revised view of particle nucleation from DMS derived H 2 SO 4 Raes, JGR, 1995 Clarke et al., JGR, 1998 Particle production in cloud outflow regions followed by subsidence and particle growth prevents a local marine biota climate feedback loop.
9 Free troposphere: Long range transport of continental emissions Homogeneous nucleation of DMS oxidation products Quinn & Bates, Nature (2011) H 2 SO 4 SO 4 = Entrainment rate SO 4 = Sea salt Cloud Condensation Nuclei Organics DMS SO 2 DMS Biological activity Wind speed Gas phase organics Phytoplankton Marine boundary layer: Particle growth condensation, coagulation, cloud processing Secondary organic aerosol formation Wind speed Bubble bursting Sea salt DOM Biological activity Surfactants Wind speed Bubble bursting Marine aggregates
10 What is the CCN budget over the Southern Ocean? What are the best approaches for modeling the sources and climate impacts of CCN over the Southern Ocean?
11 Continental SO 4 = (Long range transport) Summer: 20 30% H 2 SO 4 Summer: 20 30% Winter: 10% Cloud Condensation Nuclei Summer: 35 48% H 2 SO 4 Winter: 80 90% Summer: 6% DMS Sea spray (D p < 70 nm) Sea spray (D p > 70 nm) DMS Phytoplankton Global CTM, size resolved microphysics Did not include organics Korhonen et al., JGR, 2008
12 Free troposphere: Long range transport of continental emissions Homogeneous nucleation of DMS oxidation products Quinn & Bates, Nature (2011) H 2 SO 4 SO 4 = Entrainment rate SO 4 = Sea salt Cloud Condensation Nuclei Organics DMS SO 2 DMS Biological activity Wind speed Gas phase organics Phytoplankton Marine boundary layer: Particle growth condensation, coagulation, cloud processing Secondary organic aerosol formation Wind speed Bubble bursting Sea salt DOM Seawater carbon pool Biological activity Surfactants Bubble bursting Marine aggregates
13 Global annual average emission rate of submicron organic carbon in sea spray aerosol based on chlorophyll MODIS composite image of chlorophyll for Spring 2010 NASA/GSFC/OBPG Modeled annual average submicron emission rate of OC in sea spray aerosol based on monthly average climatological chlorophyll (Gantt et al., ACP, 2011) Global emissions of sea spray aerosol organics based on chlorophyll look a lot like global maps of chlorophyll. What about emission of sea spray organics in low chlorophyll ocean regions?
14 Evidence for emission of sea spray organic carbon from low chlorophyll waters Sea spray aerosol generated from oligotrophic (low chlorophyll) Sargasso Seawater Organic carbon is detectable at all size ranges Freshly emitted sea spray aerosol The enrichment of organic carbon relative to seawater increases with decreasing particle size. Particle diameter, um Keene et al., JGR, 2007
15 Organic Carbon Enrichment Factor for Sea Spray Aerosol Relative to Seawater EF OC = [(OC as C) / Na + ] SSA [(OC as C) / Na + ] seawater
16 10 5 Published values of EF OC for freshly emitted sea spray aerosol EF OC Chl a, g L Particle size range D p < 0.18 um D p < 0.25 um D p < 1.0 um Bulk aerosol No correlation between nascent SSA EF OC and chlorophyll on a regional basis High EF OC values in high and low Chl a waters Highest organic enrichments occur in the size range relevant for CCN activation (D 2 < 0.2 m) WACS Station 1 WACS Station 2 CalNex Low Chlor CalNex High Chlor Quinn et al., Nat. Geo., 2014 Sargasso Sea MAP Facchini et al., GRL, 2008 Hoffman and Duce, JGR, 1976 Keene et al., JGR, 2007
17 10 5 Published values of EF OC for freshly emitted sea spray aerosol EF OC Chl a, g L Particle size range D p < 0.18 um D p < 0.25 um D p < 1.0 um Bulk aerosol The large EF OC for the lowchlorophyll Sargasso Sea reveals a pool of surface seawater organic matter that is not directly associated with Chl a and phytoplankton biomass, but is available for incorporation into nascent SSA. WACS Station 1 WACS Station 2 CalNex Low Chlor CalNex High Chlor Quinn et al., Nat. Geo., 2014 Sargasso Sea MAP Facchini et al., GRL, 2008 Hoffman and Duce, JGR, 1976 Keene et al., JGR, 2007
18 10 5 Published values of EF OC for freshly emitted sea spray aerosol EF OC Chl a, g L Particle size range D p < 0.18 um D p < 0.25 um D p < 1.0 um Bulk aerosol WACS Station 1 WACS Station 2 CalNex Low Chlor CalNex High Chlor Quinn et al., Nat. Geo., 2014 Sargasso Sea MAP Facchini et al., GRL, 2008 Hoffman and Duce, JGR, 1976 Keene et al., JGR, 2007 The large EF OC for the lowchlorophyll Sargasso Sea reveals a pool of surface seawater organic matter that is not directly associated with Chl a and phytoplankton biomass, but is available for incorporation into nascent SSA. Is there any difference in CCN activity between high and low chlorophyll waters (which would imply a difference in organic composition)?
19 CCN/CN CCN activity of freshly emitted sea spray aerosol from high and low chlorophyll waters a) D p = 40 nm CCN/CN b) D p = 50 nm WACS High Chlor (Sta 1) Low Chlor (Sta 2) Calibration aerosol Ammonium Sulfate NaCl Sargasso Seawater SS (%) c) D p = 60 nm SS (%) d) D p = 100 nm CCN activity increases with increasing particle size CCN/CN CCN/CN No significant difference in CCN activity for high and low chlorophyll waters SS (%) SS (%) Does the uniformity in CCN activity apply globally?
20 Organic volume fraction of sea spray aerosol based on CCN activity No difference between high and low surface seawater chlorophyll appa appa NaCl Sea Sweep SSA Sea Sweep SSA Organic Volume Fraction Organic Volume Fraction D dry, nm These data are based on measurements in the North Atlantic. How representative are they globally? The answer depends on the variability in surface seawater DOC concentration and composition
21 Seawater Organic Carbon Pool POC ~ 10% of TOC ~ 90% of TOC Phytoplankton (Chlorophyll) Senescence Extracellular release Viral lysis VOCs UV oxidation Bacteria DOC Consumption Bacterial lysis Sorption Vertical mixing & advection Microzooplankton Consumption Grazing Sloppy feeding Excretory release Macrozooplankton Detritus Sinking particulates (also POC)
22 POC Seawater Organic Carbon Pool ~ 10% of TOC Is there enough variability in surface seawater ~ 90% of TOC DOC concentration and composition to result Phytoplankton in differences in CCN activity? (Chlorophyll) Senescence Extracellular release Viral lysis VOCs UV oxidation Bacteria DOC Consumption Bacterial lysis Sorption Vertical mixing & advection Microzooplankton Consumption Grazing Sloppy feeding Excretory release Macrozooplankton Detritus Sinking particulates (also POC)
23 Classes of DOC in the ocean based on lifetime Lifetime (years) CO 2 ~25 Pg C y Labile DOC lost by rapid microbial turnover (short lived) DOC sources Recalcitrant DOC (Longer Lived) ,000 40,000 SLDOC SRDOC RDOC URDOC ~2 Pg C y 1 CO 2 and other losses Hansell, Annu. Rev. Mar. Sci., 2013.
24 Classes of DOC in the ocean based on lifetime Lifetime (years) CO 2 ~25 Pg C y Labile DOC (short lived) DOC sources Recalcitrant DOC (Longer Lived) HMW carbohydrates, smaller sugars, amino acids Carboxyl rich alicyclics Polycyclic aromatics ,000 40,000 SLDOC SRDOC RDOC URDOC ~2 Pg C y 1 Differences in composition have not been distinguished Much of seawater DOC remains uncharacterized CO 2 and other losses Hansell, Ann. Rev. Mar. Sci., 2013.
25 Profiles of seawater DOC concentration and fractions Influence of ocean dynamics Sargasso Sea (August) Southern Ross Sea (January) Contributions of DOC fractions to surface seawater carbon pool differ for the N. Atlantic and Southern Ocean Hansell, Ann. Rev. Mar. Sci., Higher SLDOC concentration likely due to a higher rate of productivity. The lack of a permanent pycnocline in the Ross Sea prevents an observable accumulation of SRDOC.
26 Observed concentrations of DOC Lowest concentrations are observed at the surface in subpolar seas and in the Southern Ocean (> 50S) where deeper vertical mixing dilutes surface accumulated fractions with low DOC concentrations from depth. Will the difference in DOC fractions and the lower concentrations be reflected in the organic content of CCN and in CCN activity? Hansell, Ann. Rev. Mar. Sci., 2013.
27 Based on limited data from the North Atlantic, any differences in surface seawater DOC concentration and composition do not result in differences in CCN activity. Organics SOCRATES provides an opportunity to assess the Southern Ocean MBL CCN budget and, in particular, the impact of organics on CCN for comparison to the N. Atlantic. Will require a host of seawater and atmospheric measurements from multiple platforms.
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