Chemical and physical influences on aerosol activation in liquid clouds: A study based on observations from the Jungfraujoch, Switzerland

A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from four summertime Cloud and Aerosol Characterisation Experiments (CLACE) at the high-altitude site Jungfraujoch (JFJ). It is shown that 79% of the observed variance in droplet numbers can be represented by a model accounting only for the number of potential cloud condensation nuclei (defined as number of particles larger than 80nm in diameter), while the mean errors in the model representation may be reduced by the addition of further explanatory variables, such as the mixing ratios of O3, CO, and the height of the measurements above cloud base. The statistical model has a similar ability to represent the observed droplet numbers in each of the individual years, as well as for the two predominant local wind directions at the JFJ (northwest and southeast). Given the central European location of the JFJ, with air masses in summer being representative of the free troposphere with regular boundary layer in-mixing via convection, we expect that this statistical model is generally applicable to warm clouds under conditions where droplet formation is aerosol limited (i.e. at relatively high updraught velocities and/or relatively low aerosol number concentrations). A comparison between the statistical model and an established microphysical parametrization shows good agreement between the two and supports the conclusion that cloud droplet formation at the JFJ is predominantly controlled by the number concentration of aerosol particles. © 2016 Author(s).

Dynamical states of low temperature cirrus

Athanasios Nenes

Low ice crystal concentration and sustained in-cloud supersaturation, commonly found in cloud observations at low temperature, challenge our understanding of cirrus formation. Heterogeneous freezing from effloresced ammonium sulfate, glassy aerosol, dust and black carbon are proposed to cause these phenomena; this requires low updrafts for cirrus characteristics to agree with observations and is at odds with the gravity wave spectrum in the upper troposphere. Background temperature fluctuations however can establish a "dynamical equilibrium" between ice production and sedimentation loss (as opposed to ice crystal formation during the first stages of cloud evolution and subsequent slow cloud decay) that explains low temperature cirrus properties. This newly-discovered state is favored at low temperatures and does not require heterogeneous nucleation to occur (the presence of ice nuclei can however facilitate its onset). Our understanding of cirrus clouds and their role in anthropogenic climate change is reshaped, as the type of dynamical forcing will set these clouds in one of two "preferred" microphysical regimes with very different susceptibility to aerosol. © 2011 Author(s).

2011

A study of processes that govern the maintenance of aerosols in the marine boundary layer

Athanasios Nenes

We systematically evaluate the relative influence of sources and sinks of particles in the remote marine boundary layer (MBL) to elucidate the principal factors that govern MBL aerosol behavior. Processes considered include: (1) surface flux of dimethyl sulfide (DMS); (2) gas-phase oxidation of DMS to SO2; (3) gas-phase oxidation of SO2 to H2SO4; (4) mass transfer of SO2 and H2SO4 to pre-existing particles; (5) humogenous nucleation of H2SO4/H2O; (6) entrainment of air from the free troposphere; (7) deposition to the sea surface; (8) cycling of air through clouds and rain scavenging; (9) oxidation of SO2 in sea salt aerosols and cloud droplets; and (10) sea-salt particle production at sea surface. The average aerosol number concentration is found to be quite sensitive to the rate of entrainment of aerosol-containing air from the free troposphere. The path that leads to the greatest accumulation of non-sea-salt (nss) sulfate involves SO2 (rather than H2SO4) absorption into existing particles. Because of scavenging of SO2 and H2SO4 by sea-salt aerosol, a considerable fraction of nss-sulfate is internally mixed with sea-salt aerosol. Under the conditions assumed in this study, MBL aerosol number concentration is dominated by free tropospheric aerosol under virtually all conditions, 89% in the base case, and even 69% at a 17 ms-1 wind speed. Aerosol mass, on the other hand, is dominated by sea-salt particles, 62% in the base case and 98% at a wind speed of 17 m s-1. Evaporation of cloud droplets provides 4.6% of the particle number in the base case, but 28% of the particle mass. At the high nucleation rate case considered here, there is notably little change in the overall contributions to aerosol number and mass from the base case; only about 5% of the total particle number is provided by nucleation events. Variation in precipitation frequency also has only a minor effect on the overall contributions. One concludes that the MBL aerosol is remarkably robust in the face of ever-changing conditions. Free tropospheric aerosol entrainment tends to sustain particle number concentrations, and sea salt emissions maintain most of the aerosol mass. Cloud processing, while not a major contributor to aerosol number, does provide, except under high wind conditions, the order of 20% of the aerosol mass. Although nucleation occurs only infrequently and does not contribute appreciably to long-term average aerosol number or mass, nucleation is, nonetheless, the mechanism that replenishes aerosol number in brief, intense episodes when aerosol surface area levels are substantially reduced by precipitation. The relative influence of particle sources and sinks in the remote marine boundary layer (MBL) is evaluated to elucidate the principal factors governing MBL aerosol behavior. Processes considered include: dimethyl sulfide (DMS) surface flux; gas phase DMS oxidation to SO2; gas phase SO2 oxidation to H2SO4; SO2 and H2SO4 mass transfer to preexisting particles; H2SO4/H2O nucleation; air entrainment from the free troposphere; deposition to the sea surface; air through clouds cycling and rain scavenging; SO2 oxidation in sea salt aerosols and cloud droplets; and sea-salt particle production at sea surface. These processes combined result in a remarkably robust MBL aerosol in the face of ever-changing conditions.

Elsevier Sci Ltd1999

Evaluation of global simulations of aerosol particle and cloud condensation nuclei number, with implications for cloud droplet formation

Athanasios Nenes, Julia Schmale

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of −24 % and −35 % for particles with dry diameters >50 and >120 nm, as well as −36 % and −34 % for CCN at supersaturations of 0.2 % and 1.0 %, respectively. However, they seem to behave differently for particles activating at very low supersaturations (

2019

A study of processes that govern the maintenance of aerosols in the marine boundary layer

Athanasios Nenes

Elsevier Sci Ltd1999