ALBERT

Description: The formation of new aerosol from the gas phase is commonly represented in atmospheric modeling with parameterizations of the steady state nucleation rate. Present parameterizations are based on classical nucleation theory or on nucleation rates calculated with a numerical aerosol model. These parameterizations reproduce aerosol nucleation rates calculated with a numerical aerosol model only imprecisely. Additional errors can arise when the nucleation rate is used as a surrogate for the production rate of particles of a given size. We discuss these errors and present a method which allows a more precise calculation of steady state sulfate aerosol formation rates. The method is based on the semi-analytical solution of an aerosol system in steady state and on parameterized rate coefficients for H2SO4 uptake and loss by sulfate aerosol particles, calculated from laboratory and theoretical thermodynamic data.

Description: This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation. Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker in-cloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher Ångström parameters. Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans in Ångström parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aerosol mass concentrations are very similar to those in the old version. The total aerosol water content in HAM2 is considerably closer to the multi-model average from Phase I of the AeroCom intercomparison project. Model deficiencies that require further efforts in the future include (i) positive biases in AOD over the ocean, (ii) negative biases in AOD and aerosol mass concentration in high-latitude regions, and (iii) negative biases in particle number concentration, especially that of the Aitken mode, in the lower troposphere in heavily polluted regions.

Description: Chemical and aerosol processes in the transition from closed- to open-cell circulation in the remote, cloudy marine boundary layer are explored. It has previously been shown that precipitation can initiate a transition from the closed- to the open-cellular state, but that the boundary layer cannot maintain this open-cell state without a resupply of cloud condensation nuclei (CCN). Potential sources of CCN include wind-driven production of sea salt from the ocean, nucleation from the gas phase, and entrainment from the free troposphere. In order to investigate CCN sources in the marine boundary layer and their role in supplying new particles, we have coupled in detail chemical, aerosol, and cloud processes in the WRF/Chem model, and added state-of-the-art representations of sea salt emissions and aerosol nucleation. We conduct numerical simulations of the marine boundary layer in the transition from a closed- to an open-cell state. Results are compared with observations in the Southeast Pacific boundary layer during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The transition from the closed- to the open-cell state generates conditions that are conducive to nucleation by forming a cloud-scavenged, ultra-clean layer below the inversion base. Open cell updrafts loft dimethyl sulfide from the ocean surface into the ultra-clean layer, where it is oxidized during daytime to SO2 and subsequently to H2SO4. Low H2SO4 condensation sink values in the ultra-clean layer allow H2SO4 to rise to concentrations at which aerosol nucleation produces new aerosol in significant numbers. The existence of the ultra-clean layer is confirmed by observations. We find that the observed DMS flux from the ocean in the VOCALS-REx region can support a nucleation source of aerosol in open cells that exceeds sea salt emissions in terms of the number of particles produced. The freshly nucleated, nanometer-sized aerosol particles need, however, time to grow to sizes large enough to act as CCN. In contrast, mechanical production of particles from the ocean surface by near-surface winds provides a steady source of larger particles that are effective CCN at a rate exceeding a threshold for maintenance of open-cell circulation. Entrainment of aerosol from the free troposphere contributes significantly to boundary layer aerosol for the considered VOCALS-REx case, but less than sea salt aerosol emissions.

Description: Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative forcing. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are −1.15 W/m2 for charged H2SO4/H2O nucleation, −0.235 W/m2 for cluster activation, and −0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is −2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with −2.18 W/m2 to total absorbed solar short-wave radiation, compared to −0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative forcing over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local measurements: over southern Finland, where cluster activation proceeds efficiently, we find that charged nucleation of sulfuric acid and water contributes on average less than 10% to ultrafine aerosol concentrations, in good agreement with observations.

Description: Microphysical and meteorological controls on the formation of open and closed cellular structures in the Southeast Pacific are explored using model simulations based on aircraft observations during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The effectiveness of factors such as boundary-layer moisture and temperature perturbations, surface heat and moisture fluxes, large-scale vertical motion and solar heating in promoting drizzle and open cell formation for prescribed aerosol number concentrations is explored. For the case considered, drizzle and subsequent open cell formation over a broad region are more sensitive to the observed boundary-layer moisture and temperature perturbations (+0.9 g kg−1; −1 K) than to a five-fold decrease in aerosol number concentration (150 vs. 30 mg−1). When embedding the perturbations in closed cells, local drizzle and pockets of open cell (POC) formation respond faster to the aerosol reduction than to the moisture increase, but the latter generates stronger and more persistent drizzle. A local negative perturbation in temperature drives a mesoscale circulation that prevents local drizzle formation but promotes it in a remote area where lower-level horizontal transport of moisture is blocked and converges to enhance liquid water path. This represents a potential mechanism for POC formation in the Southeast Pacific stratocumulus region whereby the circulation is triggered by strong precipitation in adjacent broad regions of open cells. A simulation that attempts to mimic the influence of a coastally induced upsidence wave results in an increase in cloud water but this alone is insufficient to initiate drizzle. An increase of surface sensible heat flux is also effective in triggering local drizzle and POC formation. Both open and closed cells simulated with observed initial conditions exhibit distinct diurnal variations in cloud properties. A stratocumulus deck that breaks up due solely to solar heating can recover at night. Precipitation in the open-cell cases depletes the aerosol to the extent that cloud formation is significantly suppressed within one diurnal cycle. A replenishment rate of cloud condensation nuclei of order 1 mg−1 h−1 is sufficient to maintain clouds and prevent the boundary layer from collapsing the following day, suggesting that some local and/or remote aerosol sources is necessary for POCs to be able to last for days.

Description: New particle formation (NPF), which generates nucleation mode aerosol, was observed in the tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL) by in situ airborne measurements over South America (January–March 2005), Australia (November–December 2005), West Africa (August 2006) and Central America (2004–2007). Particularly intense NPF was found at the bottom of the TTL. Measurements with a set of condensation particle counters (CPCs) with different dp50 (50% lower size detection efficiency diameter or "cut-off diameter") were conducted on board the M-55 Geophysica in the altitude range of 12.0–20.5 km and on board the DLR Falcon-20 at up to 11.5 km altitude. On board the NASA WB-57F size distributions were measured over Central America in the 4 to 1000 nm diameter range with a system of nucleation mode aerosol spectrometers. Nucleation mode particle concentrations (NNM) were derived from these measurements which allow for identifying many NPF events with NNM in the range of thousands of particles per cm3. Over Australia and West Africa, we identified NPF in the outflow of tropical convection, in particular of a Mesoscale Convective System (MCS). Newly formed particles with NNM 〉 1000 cm−3 were found to coexist with ice cloud particles (dp 〉 2 μm) as long as cloud particle concentrations remained below 2 cm−3. The occurrence of NPF within the upper troposphere and the TTL was generally confined within 340 K to 380 K potential temperature, but NPF was of particular strength between 350 K and 370 K (i.e. ~1–4 km below the cold point tropopause). Analyses of the aerosol volatility (at 250 °C) show that in the TTL on average 75–90% of the particles were volatile, compared to typically only 50% in the extra-tropical UT, indicative for the particles to mainly consist of H2SO4-H2O and possibly organic compounds. Along two flight segments over Central and South America (24 February 2005 and 7 August 2006, at 12.5 km altitude) in cloud free air, above thin cirrus, particularly high NNM were observed. Recent lifting had influenced the probed air masses, and NNM reached up to 16 000 particles cm−3 (ambient concentration). A sensitivity study using an aerosol model, which includes neutral and ion induced nucleation processes, simulates NNM in reasonable agreement with the in situ observations of clear-air NPF. Based on new, stringent multi-CPC criteria, our measurements corroborate the hypothesis that the tropical UT and the TTL are regions supplying freshly nucleated particles. Our findings narrow the altitude of the main source region to the bottom TTL, i.e. to the level of main tropical convection outflow, and, by means of measurements of carbon monoxide, they indicate the importance of anthropogenic emissions in NPF. After growth and/or coalescence the nucleation mode particles may act as cloud condensation nuclei in the tropical UT, or, upon ascent into the stratosphere, contribute to maintain the stratospheric background aerosol.

Description: The radioactive decay of radon and its progeny can lead to ionization of air molecules and consequently influence aerosol size distribution. In order to provide a global estimate of the radon-related ionization rate, we use the global atmospheric model ECHAM5 to simulate transport and decay processes of the radioactive tracers. A global radon emission map is put together using regional fluxes reported recently in the literature. Near-surface radon concentrations simulated with this new map compare well with measurements. Radon-related ionization rate is calculated and compared to that caused by cosmic rays. The contribution of radon and its progeny clearly exceeds that of the cosmic rays in the mid- and low-latitude land areas in the surface layer. During cold seasons, at locations where high concentration of sulfuric acid gas and low temperature provide potentially favorable conditions for nucleation, the coexistence of high ionization rate may help enhance the particle formation processes. This suggests that it is probably worth investigating the impact of radon-induced ionization on aerosol-climate interaction in global models.

Description: Chemical and aerosol processes in the transition from closed- to open-cell circulation in the remote, cloudy marine boundary layer are explored. It has previously been shown that precipitation can initiate a transition from the closed- to the open-cellular state, but that the boundary layer cannot maintain this open-cell state without a resupply of cloud condensation nuclei (CCN). Potential sources include wind-driven production of sea salt particles from the ocean, nucleation from the gas phase, and entrainment from the free troposphere. In order to investigate aerosol sources in the marine boundary layer and their role in supplying new particles, we have coupled in detail chemical, aerosol, and cloud processes in the WRF/Chem model, and added state-of-the-art representations of sea salt emissions and aerosol nucleation. We introduce the new features of the model and conduct simulations of the marine boundary layer in the transition from a closed- to an open-cell state. Results are compared with observations in the Southeast Pacific boundary layer during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The transition from the closed- to the open-cell state generates conditions that are conducive to nucleation by forming a cloud-scavenged, ultra-clean layer below the inversion base. Open cell wall updrafts loft dimethyl sulfide from the ocean surface into the ultra-clean layer, where it is oxidized during daytime to SO2 and subsequently to H2SO4. Low H2SO4 condensation sink values in the ultra-clean layer allow H2SO4 to rise to concentrations at which aerosol nucleation proceeds efficiently. The existence of the ultra-clean layer is confirmed by observations. We find that the observed DMS flux from the ocean in the VOCALS-REx region can support a nucleation source of aerosol in open cells that exceeds sea salt emissions in terms of the number of particles produced. The freshly nucleated, nanometer-sized aerosol particles need, however, time grow to sizes large enough to act as CCN. In contrast, mechanical production of particles from the ocean surface by near-surface winds provides a steady source of larger particles that are effective CCN at a rate exceeding a threshold for maintenance of open-cell circulation. Entrainment of aerosol from the free troposphere contributes significantly to boundary layer aerosol for the considered VOCALS-REx case, but less than sea salt aerosol emissions.

Description: The radioactive decay of radon and its progeny can lead to ionization of air molecules and consequently influence aerosol size distribution. In order to provide a global estimate of the radon-related ionization rate, we use the global atmospheric model ECHAM5 to simulate transport and decay processes of the radioactive tracers. A global radon emission map is put together using regional fluxes reported recently in the literature. The near-surface radon concentrations simulated with this new map compare well with measurements. Radon-related ionization rate is calculated and compared to that caused by cosmic rays. The contribution of radon and its progeny clearly exceeds that of the cosmic rays in the mid- and low-latitude land areas in the surface layer. In winter, strong radon-related ionization coincides with low temperature in China, USA, and Russia, providing favorable condition for the formation of aerosol particles. This suggests that it is probably useful to include the radon-induced ionization in global models when investigating the interaction between aerosol and climate.

Description: New particle formation which generates ultrafine aerosol was observed in the continental tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL), particularly at the bottom of the TTL, by in situ airborne measurements over South America (January–March, 2005) and West Africa (August, 2006). Measurements with a set of condensation particle counters with different dp50 (50% detection efficiency cut-off particle diameter) were conducted in the altitude range of 12.0–20.5 km on board the high altitude research aircraft M-55 "Geophysica" and at up to 11.5 km altitude on board the research aircraft DLR Falcon-20. Concentrations of ultrafine particles in the size range of 6 to 15 nm were derived from these measurements and several events of new particle formation (NPF) were identified. For two flight segments (24 February 2005 and 7 August 2006, at 12.5 km altitude) when recent lifting had influenced the probed air mass, the concentration of ultrafine particles reached up to 16 000 particles cm−3 (ambient concentration). A sensitivity study by using an aerosol model which includes neutral and ion induced nucleation processes revealed predicted concentrations of ultrafine particles in reasonable agreement with the in situ observations. NPF over South America was observed in cloud free air, above thin cirrus, while over West Africa, in the outflow of a Mesoscale Convective System (MCS), newly formed particles in the range of several hundred per cm3 were found to coexist with ice cloud particles as long as the concentration of cloud particles (dp〉2 μm) remained below 2 cm−3. The occurrence of NPF within the upper troposphere and the TTL was generally confined within an altitude band extending from 340 K to 380 K potential temperature, of particular strength between 350 K and 370 K. By means of a heated aerosol inlet line (at 250 °C) measurements of particle volatility were performed which show that within the TTL over South America and West Africa, on average 10–25% of the particles contained non-volatile cores. In background UT/TTL conditions the fractions of non-volatile particles typically ranged up to 50%. Our measurements provide further evidence for the hypothesis that the tropical UT and the TTL are aerosol source regions supplying freshly nucleated particles which, if lifted, may contribute to maintain the stratospheric background aerosol. These particles can become important for cloud formation in the tropical upper troposphere, if they further grow such that they can act as cloud condensation nuclei.