Observationally constrained analysis of sea salt aerosol in the marine atmosphere

Atmospheric sea salt plays important roles in marine cloud formation and atmospheric chemistry. We performed an integrated analysis of NASA GEOS model simulations run with the GOCART aerosol module, in situ measurements from the PALMS and SAGA instruments obtained during the NASA ATom campaign, and aerosol optical depth (AOD) measurements from the AERONET Marine Aerosol Network (MAN) and from MODIS satellite observations to better constrain sea salt in the marine atmosphere. ATom measurements and GEOS model simulations both show that sea salt concentrations over the Pacific and Atlantic oceans have a strong vertical gradient, varying up to 4 orders of magnitude from the marine boundary layer to free troposphere. The modeled residence times suggest that the lifetime of sea salt particles with a dry diameter of less than 3 µm is largely controlled by wet removal, followed by turbulent process. During both boreal summer and winter, the GEOS-simulated sea salt mass mixing ratios agree with SAGA measurements in the marine boundary layer (MBL) and with PALMS measurements above the MBL. However, comparison of AOD from GEOS with AERONET/MAN and MODIS aerosol retrievals indicated that the model underestimated AOD over the oceans where sea salt dominates. The apparent discrepancy of slightly overpredicted concentration and large underpredicted AOD could not be explained by biases in the model RH affecting the particle hygroscopic growth, as modeled RH was found to be comparable to or larger than the in situ measurements. This conundrum could at least partially be explained by the difference in sea salt size distribution; the GEOS simulation has much less sea salt percentage-wise in the smaller particle size range and thus less efficient light extinction than what was observed by PALMS

Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere.

We report airborne measurements of acetaldehyde (CH3CHO) during the first and second deployments of the National Aeronautics and Space Administration (NASA) Atmospheric Tomography Mission (ATom). The budget of CH3CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly-developed online air-sea exchange module. The upper limit of the global ocean net emission of CH3CHO is estimated to be 34 Tg a-1 (42 Tg a-1 if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH3CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH3CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid (PAA) is an ideal indicator of the rapid CH3CHO production in the remote troposphere. The higher-than-expected CH3CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models

The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere

Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40&thinsp;%&ndash;60&thinsp;% of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003&thinsp;&lt;&thinsp;Dp&thinsp;&lt;&thinsp;4.8&thinsp;&micro;m) in the remote marine troposphere between &sim;0.18 and 13&thinsp;km altitude obtained during the NASA Atmospheric Tomography (ATom) mission, we show that high concentrations of newly formed particles in the tropical UT over both the Atlantic and Pacific oceans are associated with outflow regions of deep convective clouds. We focus analysis on observations over the remote Pacific Ocean, which is a region less perturbed by continental emissions than the Atlantic. Comparing aerosol size distribution measurements over the remote Pacific with box model simulations for 32 cases shows that none of the NPF schemes most commonly used in global models, including binary nucleation of sulfuric acid and water (neutral and ion-assisted) and ternary involving sulfuric acid, water, and ammonia, are consistent with observations, regardless of precursor concentrations. Through sensitivity studies, we find that the nucleation scheme among those tested that is able to explain most consistently (21 of 32 cases) the observed size distributions is that of Riccobono et al.&nbsp;(2014), which involves both organic species and sulfuric acid. The method of Dunne et al.&nbsp;(2016), involving charged sulfuric acid&ndash;water&ndash;ammonia nucleation, when coupled with organic growth of the nucleated particles, was most consistent with the observations for 5 of 32 cases. Similarly, the neutral sulfuric acid&ndash;water&ndash;ammonia method of Napari&nbsp;(2002), when scaled with a tuning factor and with organic growth added, was most consistent for 6 of 32 cases. We find that to best reproduce both nucleation and growth rates, the mixing ratios of gas-phase organic precursors generally need to be at least twice that of SO2, a proxy for dimethyl sulfide (DMS). Unfortunately, we have no information on the nature of oxidized organic species that participated in NPF in this region. Global models rarely include organic-driven nucleation and growth pathways in UT conditions where globally significant NPF takes place, which may result in poor estimates of NPF and CCN abundance and contribute to uncertainties in aerosol&ndash;cloud&ndash;radiation effects. Furthermore, our results indicate that the organic aerosol precursor vapors may be important in the tropical UT above marine regions, a finding that should guide future observational efforts. </div

Large hemispheric difference in nucleation mode aerosol concentrations in the lowermost stratosphere at mid- and high latitudes

The details of aerosol processes and size distributions in the stratosphere are important for both heterogeneous chemistry and aerosol&ndash;radiation interactions. Using in situ, global-scale measurements of the size distribution of particles with diameters &gt;&thinsp;3&thinsp;nm from the NASA Atmospheric Tomography Mission (ATom), we identify a mode of aerosol smaller than 12&thinsp;nm in the lowermost stratosphere (LMS) at mid- and high latitudes. This mode is substantial only in the Northern Hemisphere (NH) and was observed in all four seasons. We also observe elevated SO2, an important precursor for new particle formation (NPF) and growth, in the NH LMS. We use box modelling and thermodynamic calculations to show that NPF can occur in the LMS conditions observed on ATom. Aircraft emissions are shown as likely sources of this SO2, as well as a potential source of nucleation mode particles directly emitted by or formed in the plume of the engines. These nucleation mode particles have the potential to grow to larger sizes and to coagulate with larger aerosol, affecting heterogeneous chemistry and aerosol&ndash;radiation interactions. Understanding all sources and characteristics of stratospheric aerosols is important in the context of anthropogenic climate change as well as proposals for climate intervention via stratospheric sulfur injection. This analysis not only adds to the, currently sparse, observations of the global impact of aviation, but also introduces another aspect of climate influence, namely a size distribution shift of the background aerosol distribution in the LMS. </div

Prädiktive ex vivo Erfassung der Reaktivität von Kopf-Hals-Karzinomen auf Kombinationen von Zytostatika

Einleitung: Das Interesse an einer klinischer verwertbaren prädiktiven Chemoreaktivitätsdiagnostik hat in den letzten Jahren stark zugenommen. Allerdings erfassen die eingesetzten Testsysteme bislang ausschließlich das Ansprechen gegenüber Einzelsubstanzen. In der Kopf-Hals-Onkologie kommen aber praktisch ausnahmslos Kombinationen von Zytostatika zum Einsatz. Ziel unserer Studie war es, unser bestehendes ex vivo Testsystem zur Erfassung der Chemoreaktivität gegenüber Einzelsubstanzen so zu modifizieren, dass sich die Synergismen einer Kombinationstherapie ex vivo abbilden und prädiktive Aussagen zur Kombinationsbehandlung zulassen.Methoden: Tumorbiopsate von 12 Kopf-Hals-Karzinomen wurden gemäß (Dollner et al., 2004) aufgearbeitet und ex vivo analysiert. Die epitheliale Chemoreaktivität wurde für die Einzelsubstanzen 5-Fluorouracil, Carboplatin, cis-Platin und Docetaxel, sowie für die klinisch eingesetzten Kombinationen dieser Substanzen quantitativ erfasst. Diese ex vivo Ergebnisse wurden mit den klinischen Verläufen verglichen.Ergebnisse: In vier Fällen ließ sich ex vivo eine Sensibilität gegenüber Substanzkombinationen nachweisen. Das individuelle Ansprechen auf die klinische Kombinationstherapie stimmt hierbei in allen darstellbaren Fällen mit den ex vivo Tests überein. Die Testergebnisse der Einzelsubstanzen entsprechen dem klinischen Verlauf nur im Einzellfall.Schlussfolgerung: Entsprechend der klinisch praktizierten zytostatischen Kombinationstherapie erscheint die prädiktive Chemoreaktivitätsdiagnostik durch die Einführung analoger Kombinationen von Zytostatika im ex vivo Testsystem gegenüber der Testung von Einzelsubstanzen deutlich verbessert