ALBERT

Description: Growth of aerosol particles to sizes at which they can act as cloud condensation nuclei (CCN) is a crucial factor in estimating the current and future impacts of aerosol–cloud–climate interactions. Growth rates (GRs) are typically determined for particles with diameters (dP) smaller than 40 nm immediately after a regional new particle formation (NPF) event. These growth rates are often taken as representatives for the particle growth to CCN sizes (dP 〉 50–100 nm). In modelling frameworks, the concentration of the condensable vapours causing the growth is typically calculated with steady state assumptions, where the condensation sink (CS) is the only loss term for the vapours. Additionally, the growth to CCN sizes is represented with the condensation of extremely low-volatility vapours and gas–particle partitioning of semi-volatile vapours. Here, we use a novel automatic method to determine growth rates from below 10 nm to hundreds of nanometres from a 20-year-long particle size distribution (PSD) data set in boreal forest. With this method, we are able to detect growth rates also at times other than immediately after a NPF event. We show that the GR increases with an increasing oxidation rate of monoterpenes, which is closely coupled with the ambient temperature. Based on our analysis, the oxidation reactions of monoterpenes with ozone, hydroxyl radical and nitrate radical all are capable of producing vapours that contribute to the particle growth in the studied size ranges. We find that GR increases with particle diameter, resulting in up to 3-fold increases in GRs for particles with dP ∼ 100 nm in comparison to those with dP ∼ 10 nm. We use a single particle model to show that this increase in GR can be explained with aerosol-phase reactions, in which semi-volatile vapours form non-volatile dimers. Finally, our analysis reveals that the GR of particles with dP 

Description: We developed a simple algorithm to classify clouds based on global radiation and cloud base height measured by pyranometer and ceilometer, respectively. We separated clouds into seven different classes (stratus, stratocumulus, cumulus, nimbostratus, altocumulus + altostratus, cirrus + cirrocumulus + cirrostratus and clear sky + cirrus). We also included classes for cumulus and cirrus clouds causing global radiation enhancement, and we classified multilayered clouds, when captured by the ceilometer, based on their height and characteristics (transmittance, patchiness and uniformity). The overall performance of the algorithm was nearly 70 % when compared with classification by an observer using total-sky images. The performance was best for clouds having well-distinguishable effects on solar radiation: nimbostratus clouds were classified correctly in 100 % of the cases. The worst performance corresponds to cirriform clouds (50 %). Although the overall performance of the algorithm was good, it is likely to miss the occurrences of high and multilayered clouds. This is due to the technical limits of the instrumentation: the vertical detection range of the ceilometer and occultation of the laser pulse by the lowest cloud layer. We examined the use of clearness index, which is defined as a ratio between measured global radiation and modeled radiation at the top of the atmosphere, as an indicator of clear-sky conditions. Our results show that cumulus, altocumulus, altostratus and cirriform clouds can be present when the index indicates clear-sky conditions. Those conditions have previously been associated with enhanced aerosol formation under clear skies. This is an important finding especially in the case of low clouds coupled to the surface, which can influence aerosol population via aerosol–cloud interactions. Overall, caution is required when the clearness index is used in the analysis of processes affected by partitioning of radiation by clouds.

Description: Growth of aerosol particles to sizes at which they can act as cloud condensation nuclei (CCN) is a crucial factor in estimating the current and future impacts of aerosol cloud climate interactions. Growth rates are typically determined for particles with diameters (dP) smaller than 40 nm immediately after a regional new particle formation (NPF) event. These growth rates are often taken as representatives for the particle growth until CCN sizes (dP 〉 50–100 nm). In modelling frameworks, the concentration of the condensable vapours causing the growth is typically calculated with steady state assumptions, where the condensation sink is the only loss term for the vapours. Additionally, the growth to CCN sizes is represented with the condensation of extremely low-volatile vapours and gas-particle partitioning of semi-volatile vapours. Here, we use a novel automatic method to determine growth rates (GR) from below 10 nm to hundreds of nanometres from a 20-years long particle size distribution data set in Boreal forest. With this method, we are able to detect growth rates also at other times than immediately after a NPF event. We show that the GR increases with an increasing oxidation rate of monoterpenes, which is closely coupled with the ambient temperature. Based on our analysis, the oxidation reactions of monoterpenes with ozone, hydroxyl radical and nitrate radical all are capable of producing vapours that contribute to the particle growth in the studied size ranges. We find that GR increases with particle diameter, resulting in up to three-fold GRs for particles with dP ~ 100 nm in comparison to those with dP ~ 10 nm. We use a single particle model to show that this increase in GR can be explained with aerosol-phase reactions, in which semi-volatile vapours form non-volatile dimers. Finally, our analysis reveals that the GR of particles with dP 

Description: Benzene, toluene, ethylbenzene and xylenes can contribute to hydroxyl reactivity and secondary aerosol formation in the atmosphere. These aromatic hydrocarbons are typically classified as anthropogenic air pollutants, but there is growing evidence of biogenic sources, such as emissions from plants and phytoplankton. Here we use a series of shipborne measurements of the remote marine atmosphere, seawater mesocosm incubation experiments and phytoplankton laboratory cultures to investigate potential marine biogenic sources of these compounds in the oceanic atmosphere. Laboratory culture experiments confirmed marine phytoplankton are a source of benzene, toluene, ethylbenzene, xylenes and in mesocosm experiments their sea-air fluxes varied between seawater samples containing differing phytoplankton communities. These fluxes were of a similar magnitude or greater than the fluxes of dimethyl sulfide, which is considered to be the key reactive organic species in the marine atmosphere. Benzene, toluene, ethylbenzene, xylenes fluxes were observed to increase under elevated headspace ozone concentration in the mesocosm incubation experiments, indicating that phytoplankton produce these compounds in response to oxidative stress. Our findings suggest that biogenic sources of these gases may be sufficiently strong to influence atmospheric chemistry in some remote ocean regions.

Description: One pathway by which the oceans influence climate is via the emission of sea spray that may subsequently influence cloud properties. Sea spray emissions are known to be dependent on atmospheric and oceanic physicochemical parameters, but the potential role of ocean biology on sea spray fluxes remains poorly characterized. Here we show a consistent significant relationship between seawater nanophytoplankton cell abundances and sea-spray derived Cloud Condensation Nuclei (CCN) number fluxes, generated using water from three different oceanic regions. This sensitivity of CCN number fluxes to ocean biology is currently unaccounted for in climate models yet our measurements indicate that it influences fluxes by more than one order of magnitude over the range of phytoplankton investigated.

Description: The goal of the Sea2Cloud project is to study the interplay between surface ocean biogeochemical and physical properties, fluxes to the atmosphere, and ultimately their impact on cloud formation under minimal direct anthropogenic influence. Here we present an interdisciplinary approach, combining atmospheric physics and chemistry with marine biogeochemistry, during a voyage between 41 degrees and 47 degrees S in March 2020. In parallel to ambient measurements of atmospheric composition and seawater biogeochemical properties, we describe semicontrolled experiments to characterize nascent sea spray properties and nucleation from gas-phase biogenic emissions. The experimental framework for studying the impact of the predicted evolution of ozone concentration in the Southern Hemisphere is also detailed. After describing the experimental strategy, we present the oceanic and meteorological context including provisional results on atmospheric thermodynamics, composition, and flux measurements. In situ measurements and flux studies were carried out on different biological communities by sampling surface seawater from subantarctic, subtropical, and frontal water masses. Air-Sea-Interface Tanks (ASIT) were used to quantify biogenic emissions of trace gases under realistic environmental conditions, with nucleation observed in association with biogenic seawater emissions. Sea spray continuously generated produced sea spray fluxes of 34% of organic matter by mass, of which 4% particles had fluorescent properties, and which size distribution resembled the one found in clean sectors of the Southern Ocean. The goal of Sea2Cloud is to generate realistic parameterizations of emission flux dependences of trace gases and nucleation precursors, sea spray, cloud condensation nuclei, and ice nuclei using seawater biogeochemistry, for implementation in regional atmospheric models.