scholarly journals Regional variation of the dimethyl sulfide oxidation mechanism in the summertime marine boundary layer in the Gulf of Maine

Author(s):  
Hans D. Osthoff ◽  
Timothy S. Bates ◽  
James E. Johnson ◽  
William C. Kuster ◽  
Paul Goldan ◽  
...  
2018 ◽  
Vol 18 (23) ◽  
pp. 17615-17635 ◽  
Author(s):  
Guangjie Zheng ◽  
Yang Wang ◽  
Allison C. Aiken ◽  
Francesca Gallo ◽  
Michael P. Jensen ◽  
...  

Abstract. The response of marine low cloud systems to changes in aerosol concentration represents one of the largest uncertainties in climate simulations. Major contributions to this uncertainty are derived from poor understanding of aerosol under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse marine boundary layer (MBL) clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In this study, we examine MBL aerosol properties, trace gas mixing ratios, and meteorological parameters measured at the Atmospheric Radiation Measurement Climate Research Facility's ENA site on Graciosa Island, Azores, Portugal, during a 3-year period from 2015 to 2017. Measurements impacted by local pollution on Graciosa Island and during occasional intense biomass burning and dust events are excluded from this study. Submicron aerosol size distribution typically consists of three modes: Aitken (At, diameter Dp<∼100 nm), accumulation (Ac, Dp within ∼100 to ∼300 nm), and larger accumulation (LA, Dp>∼300 nm) modes, with average number concentrations (denoted as NAt, NAc, and NLA below) of 330, 114, and 14 cm−3, respectively. NAt, NAc, and NLA show contrasting seasonal variations, suggesting different sources and removal processes. NLA is dominated by sea spray aerosol (SSA) and is higher in winter and lower in summer. This is due to the seasonal variations of SSA production, in-cloud coalescence scavenging, and dilution by entrained free troposphere (FT) air. In comparison, SSA typically contributes a relatively minor fraction to NAt (10 %) and NAc (21 %) on an annual basis. In addition to SSA, sources of Ac-mode particles include entrainment of FT aerosols and condensation growth of Aitken-mode particles inside the MBL, while in-cloud coalescence scavenging is the major sink of NAc. The observed seasonal variation of NAc, being higher in summer and lower in winter, generally agrees with the steady-state concentration estimated from major sources and sinks. NAt is mainly controlled by entrainment of FT aerosol, coagulation loss, and growth of Aitken-mode particles into the Ac-mode size range. Our calculation suggests that besides the direct contribution from entrained FT Ac-mode particles, growth of entrained FT Aitken-mode particles in the MBL also represent a substantial source of cloud condensation nuclei (CCN), with the highest contribution potentially reaching 60 % during summer. The growth of Aitken-mode particles to CCN size is an expected result of the condensation of sulfuric acid, a product from dimethyl sulfide oxidation, suggesting that ocean ecosystems may have a substantial influence on MBL CCN populations in the ENA.


2018 ◽  
Author(s):  
Guangjie Zheng ◽  
Yang Wang ◽  
Allison C. Aiken ◽  
Francesca Gallo ◽  
Mike Jensen ◽  
...  

Abstract. The response of marine low cloud systems to changes in aerosol concentration represents one of the largest uncertainties in climate simulations. Major contributions to this uncertainty derive from poor understanding of aerosol under natural conditions and the perturbation by anthropogenic emissions. The Eastern North Atlantic (ENA) is a region of persistent but diverse marine boundary layer (MBL) clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In this study, we examine MBL aerosol properties, trace gas mixing ratios, and meteorological parameters measured at the Atmospheric Radiation Measurement Climate Research Facility’s ENA site on Graciosa Island, Azores, Portugal from 2015 to 2017. Measurements impacted by local pollutions on Graciosa Island and during occasional intense biomass burning and dust events are excluded from this analysis. Submicron aerosol size distribution typically consists of three modes: Aitken (At), Accumulation (Ac), and Larger Accumulation (LA) modes, with average number concentrations (denoted as NAt, NAc and NLA below) of 330, 114, and 14 cm−3, respectively. NAt, NAc and NLA show contrasting seasonal variations, suggesting different sources and removal processes. NLA is dominated by sea spray aerosol (SSA), and is higher in winter and lower in summer. This is due to the seasonal variations of SSA production, coalescence scavenging, and dilution by entrained free troposphere (FT) air. In comparison, SSA typically contributes a relatively minor fraction to NAt (10 %) and NAc (21 %) on an annual basis. In addition to SSA, sources of Ac mode particles include entrainment of FT aerosols and condensation growth of At mode particles inside MBL, while coalescence scavenging is the major sink of NAc. The observed seasonal variation of NAc, being higher in summer and lower in winter, generally agrees with the estimate based on the major sources and sink. NAt is mainly controlled by entrainment of FT aerosol, coagulation loss, and growth of At mode particles into Ac mode size range. Our calculation suggests besides the direct contribution from entrained FT Ac mode particles, growth of entrained FT At mode particles in the MBL also represent a substantial source of cloud condensation nuclei (CCN), with the highest contribution potentially reaching nearly 60 % during summer. The growth of At mode particles to CCN size is expected a result of the condensation of sulfuric acid from dimethyl sulfide oxidation, suggesting that ocean ecosystems may have a substantial influence on MBL CCN populations in ENA.


1992 ◽  
Vol 19 (11) ◽  
pp. 1125-1127 ◽  
Author(s):  
A. R. Bandy ◽  
D. L. Scott ◽  
B. W. Blomquist ◽  
S. M. Chen ◽  
D. C. Thornton

1990 ◽  
Vol 4 (4) ◽  
pp. 367-379 ◽  
Author(s):  
A. A. P. Pszenny ◽  
G. R. Harvey ◽  
C. J. Brown ◽  
R. F. Lang ◽  
W. C. Keene ◽  
...  

ACS Omega ◽  
2021 ◽  
Vol 6 (3) ◽  
pp. 2410-2419
Author(s):  
Junyao Li ◽  
Narcisse T. Tsona ◽  
Shanshan Tang ◽  
Xiuhui Zhang ◽  
Lin Du

2020 ◽  
Vol 20 (6) ◽  
pp. 4013-4029 ◽  
Author(s):  
Alexander B. Thames ◽  
William H. Brune ◽  
David O. Miller ◽  
Hannah M. Allen ◽  
Eric C. Apel ◽  
...  

Abstract. The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime, influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although the calculated OH reactivity was below the limit of detection for the ATom instrument used to measure OH reactivity throughout much of the free troposphere, the instrument was able to measure the OH reactivity in and just above the marine boundary layer. The mean measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom deployments was 1.9 s−1, which is 0.5 s−1 larger than the mean calculated OH reactivity. The missing OH reactivity, the difference between the measured and calculated OH reactivity, varied between 0 and 3.5 s−1, with the highest values over the Northern Hemisphere Pacific Ocean. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.


2014 ◽  
Vol 119 (14) ◽  
pp. 9142-9167 ◽  
Author(s):  
Rebecca M. C. Simpson ◽  
Steven G. Howell ◽  
Byron W. Blomquist ◽  
Antony D. Clarke ◽  
Barry J. Huebert

2019 ◽  
Author(s):  
Alexander B. Thames ◽  
William H. Brune ◽  
David O. Miller ◽  
Hannah M. Allen ◽  
Eric C. Apel ◽  
...  

Abstract. The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime, influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although the calculated OH reactivity was below the OH reactivity instrument's limit-of-detection for much of the free troposphere, the OHR instrument was able to measure the OH reactivity in and just above the marine boundary layer. The average measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom phases was 1.9 s−1, which 0.5 s−1 larger than the average calculated OH reactivity. Concurrently, missing OH reactivity, the difference between the measured and calculated OH reactivity, was measured to be ~ 0.5–2.0 s−1 at some locations in the tropics and midlatitudes. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.


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