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. Marine biogenic particle contributions to atmosphericaerosol concentrations are not well understood though they are important fordetermining cloud optical and cloud-nucleating properties. Here we examinethe relationship between marine aerosol measurements (with satellites andmodel fields of ocean biology) and meteorological variables during the NorthAtlantic Aerosols and Marine Ecosystems Study (NAAMES). NAAMES consisted offour field campaigns between November 2015 and April 2018 that aligned withthe four major phases of the annual phytoplankton bloom cycle. The FLEXible PARTicle (FLEXPART)Lagrangian particle dispersion model is used to spatiotemporally connect these variablesto ship-based aerosol and dimethyl sulfide (DMS)observations. We find that correlations between some aerosol measurementswith satellite-measured and modeled variables increase with increasingtrajectory length, indicating that biological and meteorological processes overthe air mass history are influential for measured particle properties andthat using only spatially coincident data would miss correlative connectionsthat are lagged in time. In particular, the marine non-refractory organicaerosol mass correlates with modeled marine net primary production whenweighted by 5 d air mass trajectory residence time (r=0.62). Thisresult indicates that non-refractory organic aerosol mass is influenced bybiogenic volatile organic compound (VOC) emissions that are typicallyproduced through bacterial degradation of dissolved organic matter,zooplankton grazing on marine phytoplankton, and as a by-product ofphotosynthesis by phytoplankton stocks during advection into the region.This is further supported by the correlation of non-refractory organic masswith 2 d residence-time-weighted chlorophyll a (r=0.39), a proxy forphytoplankton abundance, and 5 d residence-time-weighted downwardshortwave forcing (r=0.58), a requirement for photosynthesis. Incontrast, DMS (formed through biological processes in the seawater) andprimary marine aerosol (PMA) concentrations showed better correlations withexplanatory biological and meteorological variables weighted with shorterair mass residence times, which reflects their localized origin as primaryemissions. Aerosol submicron number and mass negatively correlate with seasurface wind speed. The negative correlation is attributed to enhanced PMAconcentrations under higher wind speed conditions. We hypothesized that theelevated total particle surface area associated with high PMA concentrationsleads to enhanced rates of condensation of VOC oxidation products onto PMA.Given the high deposition velocity of PMA relative to submicron aerosol,PMA can limit the accumulation of secondary aerosol mass. This studyprovides observational evidence for connections between marine aerosols andunderlying ocean biology through complex secondary formation processes,emphasizing the need to consider air mass history in future analyses.

Linking marine phytoplankton emissions, meteorological processes, and downwind particle properties with FLEXPART