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- Author or Editor: Frank Stratmann x
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Abstract
A comprehensive sensitivity study was carried out examining the sensitivity of hygroscopic growth and activation as modeled with the Köhler equation. Different parameters in the Köhler equation were varied within the range of their currently known uncertainties. The parameters examined include not only those describing the nature of the soluble substances in a particle/droplet and the surface tension σ of the droplet solution, but also the recently proposed representation of parameters coupling the Raoult and Kelvin terms (i.e., partitioning of solute between the surface and bulk phases, although the recently proposed adsorption to wettable but insoluble material was not considered). The examined variations cause significant changes in both hygroscopic growth and activation. Whereas the hygroscopic growth regime below 95% RH is insensitive toward the surface tension σ, σ has a large influence on the activation, increasing with decreasing particle size. This implies that a cloud condensation nuclei (CCN) closure, connecting particle hygroscopic growth to activation, has to account for an influence of the examined substance on σ of the particle, especially for smaller particles in the size range from 50 to 100 nm. A simple estimate showed that a lowering of σ by only 10% can cause a change in the activated fraction (i.e., in the cloud droplet number concentration) of at least 10%–20%. Where organic molecules are present in sufficient concentration to reduce σ, surface tension may be an important factor in determining the activation of aerosol particles to cloud droplets.
Abstract
A comprehensive sensitivity study was carried out examining the sensitivity of hygroscopic growth and activation as modeled with the Köhler equation. Different parameters in the Köhler equation were varied within the range of their currently known uncertainties. The parameters examined include not only those describing the nature of the soluble substances in a particle/droplet and the surface tension σ of the droplet solution, but also the recently proposed representation of parameters coupling the Raoult and Kelvin terms (i.e., partitioning of solute between the surface and bulk phases, although the recently proposed adsorption to wettable but insoluble material was not considered). The examined variations cause significant changes in both hygroscopic growth and activation. Whereas the hygroscopic growth regime below 95% RH is insensitive toward the surface tension σ, σ has a large influence on the activation, increasing with decreasing particle size. This implies that a cloud condensation nuclei (CCN) closure, connecting particle hygroscopic growth to activation, has to account for an influence of the examined substance on σ of the particle, especially for smaller particles in the size range from 50 to 100 nm. A simple estimate showed that a lowering of σ by only 10% can cause a change in the activated fraction (i.e., in the cloud droplet number concentration) of at least 10%–20%. Where organic molecules are present in sufficient concentration to reduce σ, surface tension may be an important factor in determining the activation of aerosol particles to cloud droplets.
Immersion Freezing of Kaolinite: Scaling with Particle Surface AreaAbstract
This study presents an analysis showing that the freezing probability of kaolinite particles from Fluka scales exponentially with particle surface area for different atmospherically relevant particle sizes. Immersion freezing experiments were performed at the Leipzig Aerosol Cloud Interaction Simulator (LACIS). Size-selected kaolinite particles with mobility diameters of 300, 700, and 1000 nm were analyzed with one particle per droplet. First, it is demonstrated that immersion freezing is independent of the droplet volume. Using the mobility analyzer technique for size selection involves the presence of multiply charged particles in the quasi-monodisperse aerosol, which are larger than singly charged particles. The fractions of these were determined using cloud droplet activation measurements. The development of a multiple charge correction method has proven to be essential for deriving ice fractions and other quantities for measurements in which the here-applied method of size selection is used. When accounting for multiply charged particles (electric charge itself does not matter), both a time-independent and a time-dependent description of the freezing process can reproduce the measurements over the range of examined particle sizes. Hence, either a temperature-dependent surface site density or a single contact angle distribution was sufficient to parameterize the freezing behavior. From a comparison with earlier studies using kaolinite samples from the same provider, it is concluded that the neglect of multiply charged particles and, to a lesser extent, the effect of time can cause a significant overestimation of the ice nucleation site density of one order of magnitude, which translates into a temperature bias of 5–6 K.
Abstract
This study presents an analysis showing that the freezing probability of kaolinite particles from Fluka scales exponentially with particle surface area for different atmospherically relevant particle sizes. Immersion freezing experiments were performed at the Leipzig Aerosol Cloud Interaction Simulator (LACIS). Size-selected kaolinite particles with mobility diameters of 300, 700, and 1000 nm were analyzed with one particle per droplet. First, it is demonstrated that immersion freezing is independent of the droplet volume. Using the mobility analyzer technique for size selection involves the presence of multiply charged particles in the quasi-monodisperse aerosol, which are larger than singly charged particles. The fractions of these were determined using cloud droplet activation measurements. The development of a multiple charge correction method has proven to be essential for deriving ice fractions and other quantities for measurements in which the here-applied method of size selection is used. When accounting for multiply charged particles (electric charge itself does not matter), both a time-independent and a time-dependent description of the freezing process can reproduce the measurements over the range of examined particle sizes. Hence, either a temperature-dependent surface site density or a single contact angle distribution was sufficient to parameterize the freezing behavior. From a comparison with earlier studies using kaolinite samples from the same provider, it is concluded that the neglect of multiply charged particles and, to a lesser extent, the effect of time can cause a significant overestimation of the ice nucleation site density of one order of magnitude, which translates into a temperature bias of 5–6 K.
Abstract
Uncertainty in radiative forcing caused by aerosol–cloud interactions is about twice as large as for CO2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly quantified state of aerosols in the pristine preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to help evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific, and Atlantic Oceans; length of ship track >33,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics [e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations], trace gases, and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, and back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset (https://zenodo.org/communities/spi-ace?page=1&size=20) provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport, and processing occurring over the pristine Southern Ocean.
Abstract
Uncertainty in radiative forcing caused by aerosol–cloud interactions is about twice as large as for CO2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly quantified state of aerosols in the pristine preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to help evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific, and Atlantic Oceans; length of ship track >33,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics [e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations], trace gases, and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, and back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset (https://zenodo.org/communities/spi-ace?page=1&size=20) provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport, and processing occurring over the pristine Southern Ocean.
Abstract
Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, and surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the Arctic Cloud Observations Using Airborne Measurements during Polar Day (ACLOUD) aircraft campaign and the Physical Feedbacks of Arctic Boundary Layer, Sea Ice, Cloud and Aerosol (PASCAL) ice breaker expedition. Both observational studies were performed in the framework of the German Arctic Amplification: Climate Relevant Atmospheric and Surface Processes, and Feedback Mechanisms (AC) project. They took place in the vicinity of Svalbard, Norway, in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft; the icebreaker Research Vessel (R/V) Polarstern; an ice floe camp including an instrumented tethered balloon; and the permanent ground-based measurement station at Ny-Ă…lesund, Svalbard, were employed to observe Arctic low- and mid-level mixed-phase clouds and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above the R/V Polarstern or over the Ny-Ă…lesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.
Abstract
Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, and surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the Arctic Cloud Observations Using Airborne Measurements during Polar Day (ACLOUD) aircraft campaign and the Physical Feedbacks of Arctic Boundary Layer, Sea Ice, Cloud and Aerosol (PASCAL) ice breaker expedition. Both observational studies were performed in the framework of the German Arctic Amplification: Climate Relevant Atmospheric and Surface Processes, and Feedback Mechanisms (AC) project. They took place in the vicinity of Svalbard, Norway, in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft; the icebreaker Research Vessel (R/V) Polarstern; an ice floe camp including an instrumented tethered balloon; and the permanent ground-based measurement station at Ny-Ă…lesund, Svalbard, were employed to observe Arctic low- and mid-level mixed-phase clouds and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above the R/V Polarstern or over the Ny-Ă…lesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.
