Sea Spray Aerosol: Where Marine Biology Meets Atmospheric Chemistry

Schiffer, Jamie M.; Mael, Liora E.; Prather, Kimberly A.; Amaro, Rommie E.; Grassian, Vicki H.

doi:10.1021/acscentsci.8b00674

Cited by 44 publications

(52 citation statements)

References 72 publications

(140 reference statements)

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“…[ 24,27 ] Second, molecular dynamics (MD) simulations have been successfully implemented to model physicochemical phenomena such as ice nucleation on sea‐spray aerosols and water coverage mobility on atmospheric aerosols. [ 28–31 ] While these two approaches are paramount to understanding the chemistry of aerosols as it pertains to climate and the environment, recent work has required the use of quantum mechanical (QM) methods to advance our understanding of aerosol phenomena at a molecular level.…”

Section: Introductionmentioning

confidence: 99%

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Leonardi

Ricker

Gale

et al. 2020

Int J of Quantum Chemistry

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Aerosols significantly influence atmospheric processes such as cloud nucleation, heterogeneous chemistry, and heavy-metal transport in the troposphere. The chemical and physical complexity of atmospheric aerosols results in large uncertainties in their climate and health effects. In this article, we review recent advances in scientific understanding of aerosol processes achieved by the application of quantum chemical calculations. In particular, we emphasize recent work in two areas: new particle formation and heterogeneous processes. Details in quantum chemical methods are provided, elaborating on computational models for prenucleation, secondary organic aerosol formation, and aerosol interface phenomena. Modeling of relative humidity effects, aerosol surfaces, and chemical kinetics of reaction pathways is discussed. Because of their relevance, quantum chemical calculations and field and laboratory experiments are compared. In addition to describing the atmospheric relevance of the computational models, this article also presents future challenges in quantum chemical calculations applied to aerosols.

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Section: Introductionmentioning

confidence: 99%

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Leonardi

Ricker

Gale

et al. 2020

Int J of Quantum Chemistry

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“…Wave action generates sea salt particles that are ubiquitous in coastal areas and can also be carried significant distances inland . These particles are complex in composition and contain both inorganic salts and organics, but are primarily NaCl, with smaller amounts of bromide and iodide. Schroeder and Urone showed many decades ago that NO 2 at Torr concentrations reacts with NaCl to generate nitrosyl chloride (ClNO) which in the atmosphere would rapidly photolyze, generating chlorine atoms.…”

Section: Reactions Of Gases With Particles As a Means Of Altering Thementioning

confidence: 99%

Multiphase chemistry in the troposphere: It all starts … and ends … with gases

Finlayson-Pitts

2019

Int J of Chemical Kinetics

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When the phenomena of smog and acid deposition were first recognized, it was largely gas phase chemists and photochemists who leapt into the fray to untangle the sources and chemistry involved. Over time, the importance of multiphase chemistry was recognized, as illustrated in a dramatic manner with the discovery of the Antarctic ozone hole which is driven by heterogeneous chemistry on polar stratospheric clouds. Since then, it has become clear that multiphase chemistry is central to both the lower and upper atmosphere and that this deeply intertwines interactions between the gas and condensed phases in the atmosphere. As a result, it can be argued that multiphase atmospheric chemistry begins … and ends… with gases. This paper is based on the 2018 Polanyi Medal award presentation at the 25th International Symposium on Gas Kinetics & Related Phenomena and traces research carried out in the author's laboratory on multiphase chemistry over a number of decades. While a great deal has been learned about these processes, they remain one of the areas of greatest uncertainty in understanding atmospheric composition, air quality, chemistry, and climate change.

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“…For the North Atlantic, observations indicate that primary SSAs make a limited (less than 30 %) contribution to cloud condensation nuclei (CCN) (Quinn et al, 2017(Quinn et al, , 2019Zheng et al, 2018) with no direct connection between SSA emissions and plankton ecosystems, because the organic SSA appears to arise from the ocean's large pool of dissolved organic carbon (Quinn et al, 2014;Bates et al, 2020). SSA, however, could modify the CCN number that activates to form cloud droplets (Fossum et al, 2020), act as ice nuclei (Wilson et al, 2015;De-Mott et al, 2016;Irish et al, 2017), and be more closely linked with biogenic activity in other regions (Ault et al, 2013;Cravigan et al, 2015;O'Dowd et al, 2015;Quinn et al, 2015Quinn et al, , 2019Wang et al, 2015;Schiffer et al, 2018;Christiansen et al, 2019). Recent studies have highlighted knowledge gaps related to sea spray emissions, particularly related to the submicron sizes (e.g., Bian et al, 2019;Regayre et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

“…Aerosol number and mass concentrations are reported at standard temperature and pressure. A proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) (Müller et al, 2014;Schiller, 2018) was used aboard the NASA C-130 to measure volatile organic compounds including DMS and acetonitrile. Both observational and model data for periods when acetonitrile concentrations exceed 200 ppt are filtered out following Singh et al (2012) to remove significant biomass burning contributions that are not the focus of this study.…”

Section: Introductionmentioning

confidence: 99%

Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

et al. 2021

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Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.

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Sea Spray Aerosol: Where Marine Biology Meets Atmospheric Chemistry

Cited by 44 publications

References 72 publications

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Particle formation and surface processes on atmospheric aerosols: A review of applied quantum chemical calculations

Multiphase chemistry in the troposphere: It all starts … and ends … with gases

Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

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