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The ionic data reported in this file were generated by William Keene (wck@virginia.edu) and John Maben and the OCwe data were generated by David Kieber (djkieber@esf.edu). Please direct any related questions accordingly.

Sampling and Analytical Methods: Samples were collected on RV/Endeavor cruise 589. Locations, times, and conditions at the four hydrographic stations are available under Supplemental Documentation. During some periods, size-resolved mPMA was sampled from the generator’s headspace at 30 L min-1 with two non-rotating Multi-Orifice Uniform Deposit Impactors (MOUDIs, [Marple et al., 1991]) operated in parallel. Substrates and back filters from one impactor were analyzed for major ions and those from the other impactor were analyzed for water extractable organic carbon (OCwe). The aerodynamic cut diameters for the impactor’s size fractions were 18, 10, 5.6, 3.2, 1.8, 1.0, 0.56, 0.32, and 0.18 µm. Impactors were configured with precombusted 47-mm diameter aluminum substrates and 37-mm diameter quartz backup filters.

During some periods, bulk mPMA was sampled in parallel at 30 L min-1 on two precombusted 47-mm quartz filters, one of which was analyzed for major ions, OCwe, and surfactants and the other for total OC and radiocarbon age.

During two periods, bulk mPMA was sampled in parallel at 30 L min-1 on two 90-mm Teflon filters. One sample was analyzed for major ions and OCwe and the other was stored for photochemical manipulation experiments.

After recovery, samples of size-resolved and bulk mPMA for analysis of major ions were transferred to precleaned 10-mL HDPE tubes, stored frozen, subsequently extracted in 5 mL deionized water (DIW), and analyzed at the University of Virginia (UVA) using a Dionex duel channel model ICS 3000 high-performance ion chromatograph (IC). The anion channel was configured with Thermo Scientific Dionex guard (IonPac AG 18: 4 x 50 mm) and analytical separator (IonPac AS 18: 4 x 250mm) columns and electrolytically regenerated suppressor (AERS 500: 4mm). The cation channel was configured Dionex Guard (IonPac CG16: 5 x 50mm) and analytical separator (IonPac CG16: 5 x 250mm) columns and a Thermo Scientific Dionex electrolytically regenerated suppressor (CERS 500: 4mm).

Size-segregated mPMA sampled with cascade impactors and in bulk on quartz filters for analysis of OCwe were transferred to precombusted 10-mL Pyrex tubes, extracted immediately after recovery in 5 mL DIW, stored frozen, and analyzed in triplicate with a Shimadzu Model TOC-V CSH carbon analyzer at the State University of New York (SUNY).

Bulk mPMA sampled on Teflon filters were extracted immediately after recovery in five sequential aliquots of DIW (total of 25 mL). Subsamples of extracts were stored frozen on site and analyzed for major ions at UVA and for OCwe at SUNY using methods described above.

Data for mPMA samples were corrected based on median concentrations of analytes measured in dynamic handling blanks (N = 5 for impactor and 8 for bulk samples) that were loaded and unloaded during the campaign and subsequently processed and analyzed using procedures identical to those used for samples.

Unfiltered seawater for analysis of major ions was sampled in precleaned 10-mL HDPE tubes, stored frozen, and analyzed by IC at UVA.

Average detection limits (DLs) for mPMA analytes were estimated following Keene et al. [1989, JGR] and are summarized (see Supplemental Documents)

Average precisions for inorganic mPMA analytes are estimated to be ±4% of the measured concentrations or ±0.5*DLs, whichever are the greater absolute values. Precisions for OCwe correspond to the standard deviations for triplicate measurements.

Measured concentrations of all ionic constituents in seawater were substantially higher than estimated DLs. Average precisions are approximately ±2% of the measured concentrations.

Refer to the following papers for additional details regarding the design and operation of the marine aerosol generator, analytical methods, and data quality.

1d:Tbe5,The oceans hold a massive quantity of organic carbon that is greater than all terrestrial organic carbon biomass combined. Nearly all marine organic carbon is dissolved and more than 95% is refractory, and cycled through the oceans several times before complete removal. Refractory dissolved organic carbon (RDOC) concentrations are uniform with depth in the water column and represent the "background" carbon present throughout the oceans. However, very little is known regarding RDOC production and removal processes. One potential removal pathway is through adsorption of RDOC onto surfaces of rising bubbles produced by breaking waves and ejection via bubble bursting into the atmosphere. Building on prior research, the investigators will evaluate the importance of ocean- atmosphere processing in recycling marine RDOC during a research cruise in the northwestern Atlantic Ocean. Results of the research will provide important insights regarding the coupled ocean-atmosphere loss of RDOC, thereby improving understanding of and ability to predict the role of RDOC in oceanic and atmospheric biogeochemistry, the global carbon cycle, and Earth's climate. The research will involve three early career faculty, and will provide training for undergraduate and graduate researchers. Recent results based on a limited set of observations indicate that the organic matter (OM) associated with primary marine aerosol (PMA) produced by bursting bubbles from breaking waves at the sea surface is comprised partly to wholly of RDOC rather than OM of recent biological origin as has been widely assumed. The injection of RDOC into the atmosphere in association with PMA and its subsequent photochemical oxidation is a potentially important and hitherto unrecognized sink for RDOC in the oceans of sufficient magnitude to close the marine carbon budget and help resolve a long-standing conundrum regarding removal mechanisms for marine RDOC. This project will involve a shipboard investigation and modeling study to (1) quantify the relative contributions of marine refractory dissolved organic carbon (RDOC) to primary marine aerosol organic matter (PMA OM) produced from near-surface seawater in biologically productive and oligotrophic regions and from North Atlantic Deep Water, and to (2) determine the importance of atmospheric photochemical processing as a recycling pathway for RDOC. To test these hypotheses, a high-capacity aerosol generator will be deployed at four hydrographic stations in the NW Atlantic Ocean to characterize (1) the natural abundance of 14C in PMA and in surface and deep seawater; (2) the surface tension and physical properties of bubble plumes; (3) size-resolved production fluxes, chemical composition, organic carbon enrichments, spectral absorbance, and photochemical evolution of PMA; and (4) the carbon content, optical properties, and physical properties of seawater. The importance of RDOC recycling via PMA production and photochemical evolution will be interpreted with model calculations. EN589 Cruise Track6:["$","$L1b",null,{"dataset":{"_id":"750917","description":"

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Campaign sequence number corresponding to a given set of generator operating conditions as detailed in the companion file (EN589 Marine Aerosol Generator Operating Conditions).

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unique sample identification or number; any combination of alpha numeric characters; precise definition is file dependent

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Sample type: Size-resolved mPMA sampled with a cascade impactor (CI); bulk mPMA sampled on a quartz filter (B); bulk mPMA sampled on a Teflon filter for photochemical manipulation experiments (P); or seawater (S).

","units":{"_id":"","name":"unitless"},"type":{"_id":"1742","name":"sample_type","description":"

text description of type of sample collected (rock, bio, fluid, etc)

"}},{"_id":"750943","name":"Sample_ID","format":"","frictionlessType":"","description":"

Sample ID number

","units":{"_id":"","name":"unitless"},"type":{"_id":"960","name":"sample","description":"

unique sample identification or number; any combination of alpha numeric characters; precise definition is file dependent

"}},{"_id":"750944","name":"CI_50_Aerodynamic_Cut_Diam","format":"","frictionlessType":"","description":"

Aerodynamic cut diameter for CI samples (µm at ambient relative humidity).

","units":{"_id":"","name":"micrometers"},"type":{"_id":"1073","name":"no_bcodmo_term","description":"

An association with a community-wide standard parameter has not yet been made.

"}},{"_id":"750945","name":"S_Sample_Location","format":"","frictionlessType":"","description":"

Location at which seawater was sampled (I denotes inlet to generator; O denotes outlet from generator). Duplicate measurements at the same time and location are denoted by 'Dup'.

","units":{"_id":"","name":"unitless"},"type":{"_id":"1073","name":"no_bcodmo_term","description":"

An association with a community-wide standard parameter has not yet been made.

"}},{"_id":"750946","name":"ISO_DateTime_local_start","format":"","frictionlessType":"","description":"

Size-resolved and bulk mPMA sample start date and time or seawater sampling date and time; ISO 8601:2004E format.

","units":{"_id":"","name":"unitless"},"type":{"_id":"1909","name":"ISO_DateTime_Local","description":"

Date/Time (Local) ISO formatted
\nThis standard is based on ISO 8601:2004(E) and takes on any of the following forms:
\nYYYY-MM-DDTHH:MM:SS[.xx]
\n2009-08-30T09:05:00[.xx] (local time)
\n2009-08-30T14:05:00[.xx]Z (UTC time)
\n2009-08-30T14:05:00[.xx]-05:00
\nThe dashes and the colons can be dropped.
\nThe T can also be dropped \"by mutual agreement\", but one needs the trailing Z if the time is UTC.

Note the Time Zone (TZ) as +/-HH:MM
\nTime Zone signage is for conversion from local to UTC
\nWest Coast USA in summer is +7 (add 7 hrs to local time for UTC)

"}},{"_id":"750947","name":"ISO_DateTime_local_end","format":"","frictionlessType":"","description":"

Size-resolved and bulk mPMA sample stop date and time; ISO 8601:2004E format.

","units":{"_id":"","name":"unitless"},"type":{"_id":"1909","name":"ISO_DateTime_Local","description":"

Note the Time Zone (TZ) as +/-HH:MM
\nTime Zone signage is for conversion from local to UTC
\nWest Coast USA in summer is +7 (add 7 hrs to local time for UTC)

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Cl- concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"661641","name":"chloride","description":"

Chloride ion Cl-

"}},{"_id":"750949","name":"Br","format":"","frictionlessType":"","description":"

Br- concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"661634","name":"bromides","description":"

Bromides including Br-

"}},{"_id":"750950","name":"SO4","format":"","frictionlessType":"","description":"

SO42- concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"1904","name":"SO4","description":"

Concentration or quantity of sulfate (SO4)

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Na+ concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"527965","name":"Na","description":"

Sodium (Na). Concentrations may be reported in parts per million, nanomoles per liter, or other units. Refer to dataset metadata for units.

"}},{"_id":"750952","name":"K","format":"","frictionlessType":"","description":"

K+ concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"527968","name":"K","description":"

K (potassium) concentration. May be reported in parts per million, nanomoles/Liter, or other units. Refer to dataset metadata for units.

"}},{"_id":"750953","name":"Mg","format":"","frictionlessType":"","description":"

Mg2+ concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"527967","name":"Mg","description":"

Mg (magnesium) concentration. May be reported in parts per million, nanomoles/Liter, or other units. Refer to dataset metadata for units.

"}},{"_id":"750954","name":"Ca","format":"","frictionlessType":"","description":"

Ca2+ concentration: For mPMA in nmol m-3 air; for seawater in µM.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"527969","name":"Ca","description":"

Calcium (Ca). Concentrations may be reported in parts per million, nanomoles per liter, or other units. Refer to dataset metadata for units.

"}},{"_id":"750955","name":"OCwe","format":"","frictionlessType":"","description":"

Water-extractable organic carbon (OCwe) concentration for mPMA in nmol C m-3 air.

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"1185","name":"C_org","description":"

Organic carbon (in water, sediment, aerosol, and others); atomic carbon that is incorporated into covalently-bonded carbon compounds.

"}},{"_id":"750956","name":"OCwe_STD","format":"","frictionlessType":"","description":"

OCwe precision for mPMA in nmol C m-3 air

","units":{"_id":"","name":"nanomol/cubic meter (nmol m-3) for mPMA; micromol (µM) for S"},"type":{"_id":"1185","name":"C_org","description":"

Organic carbon (in water, sediment, aerosol, and others); atomic carbon that is incorporated into covalently-bonded carbon compounds.

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Comments

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free text comments, may only have meaning to submitting PI

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general latitude of sampling; north is positive [added by BCO-DMO from supplemental doc]

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latitude, in decimal degrees, North is positive, negative denotes South; Reported in some datasets as degrees, minutes

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general longitude of sampling; east is positive [added by BCO-DMO from supplemental doc]

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longitude, in decimal degrees, East is positive, negative denotes West; Reported in some datsets as degrees, minutes

"}}],"related_publications":[{"id":"750877","citation":"Keene, W. C., Long, M. S., Reid, J. S., Frossard, A. A., Kieber, D. J., Maben, J. R., … Bates, T. S. (2017). Factors That Modulate Properties of Primary Marine Aerosol Generated From Ambient Seawater on Ships at Sea. Journal of Geophysical Research: Atmospheres, 122(21), 11,961–11,990. doi:10.1002/2017jd026872\r\n","relation_type":["Methods"],"relation_desc":""},{"id":"750876","citation":"Keene, W. C., Maring, H., Maben, J. R., Kieber, D. J., Pszenny, A. A. P., Dahl, E. E., … Sander, R. (2007). Chemical and physical characteristics of nascent aerosols produced by bursting bubbles at a model air-sea interface. Journal of Geophysical Research, 112(D21). doi:10.1029/2007jd008464\r\n","relation_type":["Methods"],"relation_desc":""},{"id":"750959","citation":"Keene, W. C., Talbot, R. W., Andreae, M. O., Beecher, K., Berresheim, H., Castro, M., … Winiwarter, W. (1989). An intercomparison of measurement systems for vapor and particulate phase concentrations of formic and acetic acids. Journal of Geophysical Research, 94(D5), 6457. doi:10.1029/jd094id05p06457\r\n","relation_type":["Methods"],"relation_desc":""},{"id":"750878","citation":"Kieber, D. J., Keene, W. C., Frossard, A. A., Long, M. S., Maben, J. R., Russell, L. M., … Bates, T. S. (2016). Coupled ocean-atmosphere loss of marine refractory dissolved organic carbon. Geophysical Research Letters, 43(6), 2765–2772. doi:10.1002/2016gl068273\r\n","relation_type":["Methods"],"relation_desc":""},{"id":"750875","citation":"Long, M. S., Keene, W. C., Kieber, D. J., Frossard, A. A., Russell, L. M., Maben, J. R., … Bates, T. S. (2014). Light-enhanced primary marine aerosol production from biologically productive seawater. Geophysical Research Letters, 41(7), 2661–2670. doi:10.1002/2014gl059436\r\n","relation_type":["Methods"],"relation_desc":""},{"id":"750960","citation":"Marple, V. A., Rubow, K. 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