ALBERT

Description: Ice surface properties can modify the scattering properties of atmospheric ice crystals and therefore affect the radiative properties of mixed-phase and cirrus clouds. The Ice Roughness Investigation System (IRIS) is a new laboratory setup designed to investigate the conditions under which roughness develops on single ice crystals, based on their size, morphology and growth conditions (relative humidity and temperature). Ice roughness is quantified through the analysis of speckle in 2-D light-scattering patterns. Characterization of the setup shows that a supersaturation of 20 % with respect to ice and a temperature at the sample position as low as −40 ∘C could be achieved within IRIS. Investigations of the influence of humidity show that higher supersaturations with respect to ice lead to enhanced roughness and irregularities of ice crystal surfaces. Moreover, relative humidity oscillations lead to gradual “ratcheting-up” of roughness and irregularities, as the crystals undergo repeated growth–sublimation cycles. This memory effect also appears to result in reduced growth rates in later cycles. Thus, growth history, as well as supersaturation and temperature, influences ice crystal growth and properties, and future atmospheric models may benefit from its inclusion in the cloud evolution process and allow more accurate representation of not just roughness but crystal size too, and possibly also electrification properties.

Description: We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice-nucleating plant structural polymers. These samples include microcrystalline cellulose (MCC), fibrous cellulose (FC) and nanocrystalline cellulose (NCC). Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at 17 different institutions, including nine dry dispersion and 11 aqueous suspension techniques. With a total of 20 methods, we performed systematic accuracy and precision analysis of measurements from all 20 measurement techniques by evaluating T-binned (1 ∘C) data over a wide T range (−36 ∘C 

Description: Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings.In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing.The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters.

Description: The marine aerosol arriving at Barbados (Ragged Point) was characterized during two three-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). By comparison between ground based and airborne measurements it was shown that the former are representative for the marine boundary layer at least up to cloud base. In general, total particle number concentrations (Ntotal) ranged from as low as 100 cm−3 up to 800 cm−3, while number concentrations for cloud condensation nuclei (NCCN) at a supersaturation of 0.26 % ranged from some ten to 600 cm−3. Ntotal and NCCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both, Ntotal and NCCN and could be attributed to long range transport from Africa, by which biomass burning particles from the Sahel region and / or mineral dust particles from the Sahara were advected. The second and third type both had values for NCCN below 200 cm−3, and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50 % of all particles. These Aitken mode particles likely were formed by new particle formation no more than three days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be κ = 0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, at least not during the months when measurements were made. The average κ could be used to derive NCCN from measured number size distributions, showing that this is a valid approach to obtain NCCN. Although the total particulate mass sampled on filters was found to be dominated by Na+ and Cl−, this was found to be contributed by a small number of large particles (〉 500 nm, mostly even in the super-micron size range), in number concentrations below 1 cm−3. Hence it can be concluded that sea-spray does not contribute noticeably to NCCN. This is further supported by finding no correlation between Ntotal and wind speed.

Description: Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice nucleating particles (INPs). Instruments that measure the ice nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for inter-comparisons to ensure instrument differences are not interpreted as scientific findings. In this study, we inter-compare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid treated mineral dust (microcline – a K-feldspar – and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of thermodynamic conditions that can be investigated with the inter-compared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally two continuous flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation nominally presenting deposition nucleation and condensation freezing. The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for ice nucleation in the four instruments, FF (from LACIS and PIMCA-PINC) and activated fraction, AF (from PINC and SPIN) are compared. Measured FFs are up to a factor of three higher than AFs, but not consistent for all aerosol types and temperatures investigated. It showed that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness on factors such as the importance of dispersion methods and the quality of particle size-selection for inter-comparing online INP counters.

Description: It is generally known that ash particles from coal combustion can trigger ice nucleation. However, data on the ice nucleation of ash particles from different sources, including both anthropogenic and natural combustion processes, is still scarce. As coal combustion still fuels the biggest proportion of electric power production worldwide and biomass burning contributes significantly to the global aerosol loading, further data is needed to better assess the ice nucleating efficiency of ash particles. In the framework of this study, we found that ash particles from brown coal (i.e., lignite) burning are more ice active than those from wood burning, with fly ash from a coal-fired power-plant being the most efficient at nucleating ice. Furthermore the effect of particle generation on the freezing behavior was studied. For this, particles were generated either by dispersion of dry sample material, or by atomization of ash-water suspensions, and then led into the Leipzig Aerosol Cloud Interaction Simulator (LACIS) where the immersion freezing behavior was examined. Whereas the immersion freezing behavior of ashes from wood burning was not affected by the particle generation method, it depended on the type of particle generation for ash from brown coal. It was also found that the common practice of treating prepared suspensions in an ultrasonic bath to avoid aggregation of particles led to an enhanced ice nucleation activity. The findings of this study suggest a) that ash from brown coal burning may influence heterogeneous ice nucleation on at least a regional scale and b) that the freezing behavior of ash particles may be altered by a change in sample preparation and/or particle generation.

Description: We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice nucleating plant structural polymers. These samples include micro-crystalline cellulose (MCC), fibrous cellulose (FC) and nano-crystalline cellulose (NCC). Our experimental data show that particles resembling the MCC lab particle occur also in the atmosphere. Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at seventeen different institutions, including nine dry dispersion and eleven aqueous suspension techniques. With a total of twenty methods, we performed systematic accuracy and precision analysis of measurements from all twenty measurement techniques by evaluating T-binned (1 °C) data over a wide T range (−36 °C 

Description: Ice surface properties can modify the scattering properties of atmospheric ice crystals and therefore affect the radiative properties of mixed-phase and cirrus clouds. The Ice Roughness Investigation System (IRIS) is a new laboratory setup designed to investigate the conditions at which roughness develops on single ice crystals, based on their size, morphology and growth conditions (relative humidity and temperature). Ice roughness is quantified through the analysis of speckle in 2-D light scattering patterns. Characterisation of the setup shows that a supersaturation of 20% with respect to ice and a temperature at the sample position as low as −40°C could be achieved within IRIS. Investigations of the influence of humidity show that higher supersaturations with respect to ice lead to enhanced roughness and irregularities of ice crystal surfaces. Moreover, relative humidity oscillations lead to gradual “ratcheting up” of roughness and irregularities, as the crystals undergo repeated growth-sublimation cycles. This memory effect also appears to result in reduced growth rates in later cycles. Thus, growth history, as well as supersaturation and temperature, influences ice crystal growth and properties, and future atmospheric models may benefit from its inclusion in the cloud evolution process, and allow more accurate representation of not just roughness but crystal size too, and possibly also electrification properties.

Description: Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility–Hygroscopicity Tandem Differential Mobility Analyser (VH-TDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most sensitive method. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the pure biological particles. We verified this by modeling the freezing behavior of the mixed particles with the Soccerball model (SBM). It can be concluded that a single INM located on a mineral dust particle determines the freezing behavior of that particle with the result that freezing occurs at temperatures at which pure mineral dust particles are not yet ice active.

Description: The marine aerosol arriving at Barbados (Ragged Point) was characterized during two 3-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). Through a comparison between ground-based and airborne measurements it was shown that the former are representative of the marine boundary layer at least up to cloud base. In general, total particle number concentrations (Ntotal) ranged from as low as 100  up to 800 cm−3, while number concentrations for cloud condensation nuclei (NCCN) at a supersaturation of 0.26 % ranged from some 10 to 600 cm−3. Ntotal and NCCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both Ntotal and NCCN and could be attributed to long-range transport from Africa, by which biomass burning particles from the Sahel region and/or mineral dust particles from the Sahara were advected. The second and third type both had values for NCCN below 200 cm−3 and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50 % of all particles. These Aitken mode particles likely were formed by new particle formation no more than 3 days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be κ  =  0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, which might generally be the case for the months during which measurements were made. The average κ could be used to derive NCCN from measured number size distributions, showing that this is a valid approach to obtain NCCN. Although the total particulate mass sampled on filters was found to be dominated by Na+ and Cl−, this was found to be contributed by a small number of large particles ( 〉  500 nm, mostly even in the super-micron size range). Based on a three-modal fit, a sea spray mode observed in the NSDs was found to contribute 90 % to the total particulate mass but only 4 to 10 % to Ntotal and up to 15 % to NCCN. This is in accordance with finding no correlation between Ntotal and wind speed.