Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo

Sulfate and organic mass in sea spray explain more than half of the variability in Southern Ocean cloud droplet concentration. Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties—ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in Nd is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35o to 45oS) and by organic matter in sea spray aerosol at higher latitudes (45o to 55oS). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m–2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.

[1]  S. Ghan,et al.  A simple model of global aerosol indirect effects , 2013 .

[2]  Michael Schulz,et al.  Radiative forcing by aerosols as derived from the AeroCom present-day and pre-industrial simulations , 2006 .

[3]  A. C. Lewis,et al.  Evaluation of the global oceanic isoprene source and its impacts on marine organic carbon aerosol , 2008 .

[4]  A. Nenes,et al.  Effects of Ocean Ecosystem on Marine Aerosol-Cloud Interaction , 2010 .

[5]  J. K. Moore,et al.  Variable C : N : P stoichiometry of dissolved organic matter cycling in the Community Earth System Model , 2014 .

[6]  W. Collins,et al.  Description of the NCAR Community Atmosphere Model (CAM 3.0) , 2004 .

[7]  J. Burrows,et al.  Evidence of a natural marine source of oxalic acid and a possible link to glyoxal , 2011 .

[8]  Andrew Gettelman,et al.  A new two-moment bulk stratiform cloud microphysics scheme in the Community Atmosphere Model, version 3 (CAM3). Part I: Description and numerical tests , 2008 .

[9]  S. Gassó,et al.  What controls CCN seasonality in the Southern Ocean? A statistical analysis based on satellite‐derived chlorophyll and CCN and model‐estimated OH radical and rainfall , 2006 .

[10]  G. Mann,et al.  Importance of tropospheric volcanic aerosol for indirect radiative forcing of climate , 2012 .

[11]  U. Lohmann,et al.  Atmospheric Composition Change: Climate-Chemistry Interactions , 2009 .

[12]  R. Sarda-Estève,et al.  Long-term observations of carbonaceous aerosols in the Austral Ocean atmosphere: Evidence of a biogenic marine organic source , 2009 .

[13]  D. Ceburnis,et al.  Wind speed dependent size-resolved parameterization for the organic mass fraction of sea spray aerosol , 2011 .

[14]  Adina Paytan,et al.  Atmospheric iron deposition: global distribution, variability, and human perturbations. , 2009, Annual review of marine science.

[15]  Larry L. Stowe,et al.  Characterization of tropospheric aerosols over the oceans with the NOAA advanced very high resolution radiometer optical thickness operational product , 1997 .

[16]  K. Prather,et al.  Size-dependent changes in sea spray aerosol composition and properties with different seawater conditions. , 2013, Environmental science & technology.

[17]  Taro Takahashi,et al.  Skill metrics for confronting global upper ocean ecosystem-biogeochemistry models against field and remote sensing data , 2009 .

[18]  K. Taylor,et al.  Quantifying components of aerosol‐cloud‐radiation interactions in climate models , 2014 .

[19]  Tami C. Bond,et al.  Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom , 2006 .

[20]  P. Quinn,et al.  Carbohydrate-like composition of submicron atmospheric particles and their production from ocean bubble bursting , 2009, Proceedings of the National Academy of Sciences.

[21]  G. Mann,et al.  Natural aerosol direct and indirect radiative effects , 2013 .

[22]  E. Bigg Sources, nature and influence on climate of marine airborne particles , 2007 .

[23]  R. Charlson,et al.  Geographically coherent patterns of albedo enhancement and suppression associated with aerosol sources and sinks , 2015 .

[24]  D. L. Roberts,et al.  A climate model study of indirect radiative forcing by anthropogenic sulphate aerosols , 1994, Nature.

[25]  P. Quinn,et al.  The case against climate regulation via oceanic phytoplankton sulphur emissions , 2011, Nature.

[26]  I. Isaksen,et al.  Sulfur cycle and sulfate radiative forcing simulated from a coupled global climate-chemistry model , 2009 .

[27]  Y. Kaufman,et al.  Measurements of the relationship between submicron aerosol number and volume concentration , 1998 .

[28]  Olivier Boucher,et al.  The sulfate‐CCN‐cloud albedo effect , 1995 .

[29]  D. Hartmann,et al.  Observed Southern Ocean Cloud Properties and Shortwave Reflection. Part I: Calculation of SW Flux from Observed Cloud Properties* , 2014 .

[30]  J. Dachs,et al.  Potential for a biogenic influence on cloud microphysics over the ocean: a correlation study with satellite-derived data , 2012 .

[31]  G. Mann,et al.  Large contribution of natural aerosols to uncertainty in indirect forcing , 2013, Nature.

[32]  Philip Stier,et al.  DMS cycle in the marine ocean-atmosphere system – a global model study , 2005 .

[33]  S. Warren,et al.  Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate , 1987, Nature.

[34]  Z. Ristovski,et al.  Observation of the suppression of water uptake by marine particles , 2010 .

[35]  Thomas M. Smith,et al.  An Improved In Situ and Satellite SST Analysis for Climate , 2002 .

[36]  Harri Kokkola,et al.  Cloud formation of particles containing humic‐like substances , 2006 .

[37]  M. D. Stokes,et al.  Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol , 2013, Proceedings of the National Academy of Sciences.

[38]  Yen-Ting Hwang,et al.  Link between the double-Intertropical Convergence Zone problem and cloud biases over the Southern Ocean , 2013, Proceedings of the National Academy of Sciences.

[39]  N. Mahowald,et al.  Global Iron Connections Between Desert Dust, Ocean Biogeochemistry, and Climate , 2005, Science.

[40]  G. Mann,et al.  Influence of oceanic dimethyl sulfide emissions on cloud condensation nuclei concentrations and seasonality over the remote Southern Hemisphere oceans: A global model study , 2008 .

[41]  P. Adams,et al.  Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations , 2011 .

[42]  J. Gras Cloud condensation nuclei over the Southern Ocean , 1990 .

[43]  M. Lawrence,et al.  Ice nuclei in marine air: biogenic particles or dust? , 2013 .

[44]  W. Collins,et al.  The Community Earth System Model: A Framework for Collaborative Research , 2013 .

[45]  S. Twomey Pollution and the Planetary Albedo , 1974 .

[46]  J. Hansen,et al.  A parameterization for the absorption of solar radiation in the earth's atmosphere , 1974 .

[47]  Jorgen B. Jensen,et al.  Microphysical and short‐wave radiative structure of stratocumulus clouds over the Southern Ocean: Summer results and seasonal differences , 1998 .

[48]  O. Torres,et al.  ENVIRONMENTAL CHARACTERIZATION OF GLOBAL SOURCES OF ATMOSPHERIC SOIL DUST IDENTIFIED WITH THE NIMBUS 7 TOTAL OZONE MAPPING SPECTROMETER (TOMS) ABSORBING AEROSOL PRODUCT , 2002 .

[49]  A. J. Kettle,et al.  An updated climatology of surface dimethlysulfide concentrations and emission fluxes in the global ocean , 2011 .

[50]  B. Wang,et al.  Stimulation of ice nucleation by marine diatoms , 2011 .

[51]  W. Collins,et al.  PORT, a CESM tool for the diagnosis of radiative forcing , 2012 .

[52]  Michael Schulz,et al.  Global dust model intercomparison in AeroCom phase I , 2011 .

[53]  Aravind Joshi,et al.  Proceedings of the 9th international joint conference on Artificial intelligence - Volume 2 , 1985 .

[54]  R. Sander,et al.  Photochemical production of hydroxyl radical and hydroperoxides in water extracts of nascent marine aerosols produced by bursting bubbles from Sargasso seawater , 2008 .

[55]  W. Collins,et al.  An AeroCom Initial Assessment - Optical Properties in Aerosol Component Modules of Global Models , 2005 .

[56]  F. Azam,et al.  Impact of marine biogeochemistry on the chemical mixing state and cloud forming ability of nascent sea spray aerosol , 2013 .

[57]  Athanasios Nenes,et al.  Phytoplankton and Cloudiness in the Southern Ocean , 2006, Science.

[58]  T. Lenton,et al.  Quantification of DMS aerosol-cloud-climate interactions using ECHAM 5-HAMMOZ model in current climate scenario , 2010 .

[59]  Damien Garcia,et al.  Robust smoothing of gridded data in one and higher dimensions with missing values , 2010, Comput. Stat. Data Anal..

[60]  P. Rasch,et al.  A physically based framework for modeling the organic fractionation of sea spray aerosol from bubble film Langmuir equilibria , 2014 .

[61]  H. Maring,et al.  Chemical and physical characteristics of nascent aerosols produced by bursting bubbles at a model air-sea interface , 2007 .

[62]  J. Gras,et al.  Seasonal relationship between cloud condensation nuclei and aerosol methanesulphonate in marine air , 1991, Nature.

[63]  S. Macko,et al.  Concentrations, isotopic compositions, and sources of size‐resolved, particulate organic carbon and oxalate in near‐surface marine air at Bermuda during spring , 2003 .

[64]  Robert Wood,et al.  The effect of solar zenith angle on MODIS cloud optical and microphysical retrievals within marine liquid water clouds , 2014 .

[65]  D. Erickson,et al.  A sea-state based source function for size- and composition-resolved marine aerosol production , 2011 .

[66]  E. Mlawer,et al.  Radiative transfer for inhomogeneous atmospheres: RRTM, a validated correlated-k model for the longwave , 1997 .

[67]  D. Ceburnis,et al.  Biogenically driven organic contribution to marine aerosol , 2004, Nature.

[68]  P. Quinn,et al.  Light‐enhanced primary marine aerosol production from biologically productive seawater , 2014 .

[69]  K. Trenberth,et al.  Simulation of Present-Day and Twenty-First-Century Energy Budgets of the Southern Oceans , 2010 .

[70]  Paul G. Falkowski,et al.  Natural Versus Anthropogenic Factors Affecting Low-Level Cloud Albedo over the North Atlantic , 1992, Science.

[71]  D. Hartmann,et al.  Observed Southern Ocean Cloud Properties and Shortwave Reflection. Part II: Phase Changes and Low Cloud Feedback* , 2014 .

[72]  T. Lenton,et al.  Quantification of DMS aerosol-cloud-climate interactions using the ECHAM5-HAMMOZ model in a current climate scenario , 2010 .

[73]  E. Bigg,et al.  The composition of fragments of bubbles bursting at the ocean surface , 2008 .

[74]  D. Ceburnis,et al.  Primary marine organic aerosol: A dichotomy of low hygroscopicity and high CCN activity , 2011 .

[75]  M. Chipperfield,et al.  The relationship between aerosol and cloud drop number concentrations in a global aerosol microphysics model , 2009 .

[76]  L. Russell,et al.  Polysaccharides, Proteins, and Phytoplankton Fragments: Four Chemically Distinct Types of Marine Primary Organic Aerosol Classified by Single Particle Spectromicroscopy , 2010 .

[77]  S. Kreidenweis,et al.  Influence of sea-salt on aerosol radiative properties in the Southern Ocean marine boundary layer , 1998, Nature.

[78]  Prashant Kumar,et al.  On the effect of dust particles on global cloud condensation nuclei and cloud droplet number , 2011 .

[79]  D. Ceburnis,et al.  Primary submicron marine aerosol dominated by insoluble organic colloids and aggregates , 2008 .

[80]  Axel Lauer,et al.  © Author(s) 2006. This work is licensed under a Creative Commons License. Atmospheric Chemistry and Physics Analysis and quantification of the diversities of aerosol life cycles , 2022 .

[81]  P. Quinn,et al.  Contribution of sea surface carbon pool to organic matter enrichment in sea spray aerosol , 2014 .

[82]  Yi Liu,et al.  A three-dimensional gap filling method for large geophysical datasets: Application to global satellite soil moisture observations , 2012, Environ. Model. Softw..

[83]  P. Quinn,et al.  Sources and composition of submicron organic mass in marine aerosol particles , 2014 .