scholarly journals New cloud chamber experiments on the heterogeneous ice nucleation ability of oxalic acid in the immersion mode

2010 ◽  
Vol 10 (12) ◽  
pp. 29449-29512
Author(s):  
R. Wagner ◽  
O. Möhler ◽  
H. Saathoff ◽  
M. Schnaiter ◽  
T. Leisner
Keyword(s):  
Relative Humidity ◽  
Oxalic Acid ◽  
Ice Nucleation ◽  
Cloud Chamber ◽  
Ice Crystals ◽  
Ternary Solution ◽  
Oxalic Acid Dihydrate ◽  
Immersion Freezing ◽  
Expansion Cooling ◽  
Homogeneous Freezing

Abstract. The heterogeneous ice nucleation ability of oxalic acid in the immersion mode has been investigated by controlled expansion cooling runs with airborne, ternary solution droplets composed of, (i), sodium chloride, oxalic acid, and water (NaCl/OA/H2O) and, (ii), sulphuric acid, oxalic acid, and water (H2SO4/OA/H2O). Polydisperse aerosol populations with median diameters ranging from 0.5–0.7 μm and varying solute concentrations were prepared. The expansion experiments were conducted in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at initial temperatures of 244 and 235 K. In the ternary NaCl/OA/H2O system, solid inclusions of oxalic acid, presumably nucleated as oxalic acid dihydrate, were formed by temporarily exposing the ternary solution droplets to a relative humidity below the efflorescence point of NaCl. The matrix of the crystallised NaCl particulates triggered the precipitation of the organic crystals which later on remained as solid inclusions in the solution droplets when the relative humidity was again raised above the deliquescence point of NaCl. The embedded oxalic acid crystals reduced the critical ice saturation ratio required for the homogeneous freezing of pure NaCl/H2O solution droplets at a temperature of around 231 K from 1.38 to about 1.32. Aqueous solution droplets with OA inclusions larger than about 0.27 μm in diameter efficiently nucleated ice by condensation freezing when they were activated to micron-sized cloud droplets at 241 K, i.e., they froze well above the homogeneous freezing temperature of pure water droplets of about 237 K. Our results on the immersion freezing potential of oxalic acid corroborate the findings from a recent study with emulsified aqueous solutions containing crystalline oxalic acid. In those experiments, the crystallisation of oxalic acid diyhdrate was triggered by a preceding homogeneous freezing cycle with the emulsion samples. The expansion cooling cycles with ternary H2SO4/OA/H2O solution droplets were aimed to analyse whether those findings can be transferred to ice nucleation experiments with airborne oxalic acid containing aerosol particles. Under our experimental conditions, the efficiency by which the surface of homogeneously nucleated ice crystals triggered the precipitation of oxalic acid dihydrate was very low, i.e., less than one out of a hundred ice crystals that were formed by homogeneous freezing in a first expansion cooling cycle left behind an ice-active organic crystal that acted as immersion freezing nucleus in a second expansion cooling cycle.

scholarly journals New cloud chamber experiments on the heterogeneous ice nucleation ability of oxalic acid in the immersion mode

2011 ◽  
Vol 11 (5) ◽  
pp. 2083-2110 ◽  
Author(s):  
R. Wagner ◽  
O. Möhler ◽  
H. Saathoff ◽  
M. Schnaiter ◽  
T. Leisner
Keyword(s):  
Relative Humidity ◽  
Oxalic Acid ◽  
Ice Nucleation ◽  
Cloud Chamber ◽  
Ice Crystals ◽  
Ternary Solution ◽  
Oxalic Acid Dihydrate ◽  
Immersion Freezing ◽  
Expansion Cooling ◽  
Homogeneous Freezing

Abstract. The heterogeneous ice nucleation ability of oxalic acid in the immersion mode has been investigated by controlled expansion cooling runs with airborne, ternary solution droplets composed of, (i), sodium chloride, oxalic acid, and water (NaCl/OA/H2O) and, (ii), sulphuric acid, oxalic acid, and water (H2SO4/OA/H2O). Polydisperse aerosol populations with median diameters ranging from 0.5–0.7 μm and varying solute concentrations were prepared. The expansion experiments were conducted in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at initial temperatures of 244 and 235 K. In the ternary NaCl/OA/H2O system, solid inclusions of oxalic acid, presumably nucleated as oxalic acid dihydrate, were formed by temporarily exposing the ternary solution droplets to a relative humidity below the efflorescence point of NaCl. The matrix of the crystallised NaCl particulates triggered the precipitation of the organic crystals which later remained as solid inclusions in the solution droplets when the relative humidity was subsequently raised above the deliquescence point of NaCl. The embedded oxalic acid crystals reduced the critical ice saturation ratio required for the homogeneous freezing of pure NaCl/H2O solution droplets at a temperature of around 231 K from 1.38 to about 1.32. Aqueous solution droplets with OA inclusions larger than about 0.27 μm in diameter efficiently nucleated ice by condensation freezing when they were activated to micron-sized cloud droplets at 241 K, i.e., they froze well above the homogeneous freezing temperature of pure water droplets of about 237 K. Our results on the immersion freezing potential of oxalic acid corroborate the findings from a recent study with emulsified aqueous solutions containing crystalline oxalic acid. In those experiments, the crystallisation of oxalic acid diyhdrate was triggered by a preceding homogeneous freezing cycle with the emulsion samples. The expansion cooling cycles with ternary H2SO4/OA/H2O solution droplets were aimed to analyse whether those findings can be transferred to ice nucleation experiments with airborne oxalic acid containing aerosol particles. Under our experimental conditions, the efficiency by which the surface of homogeneously nucleated ice crystals triggered the precipitation of oxalic acid dihydrate was very low, i.e., less than one out of a hundred ice crystals that were formed by homogeneous freezing in a first expansion cooling cycle left behind an ice-active organic crystal that acted as immersion freezing nucleus in a second expansion cooling cycle.

scholarly journals High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

2010 ◽  
Vol 10 (16) ◽  
pp. 7617-7641 ◽  
Author(s):  
R. Wagner ◽  
O. Möhler ◽  
H. Saathoff ◽  
M. Schnaiter ◽  
T. Leisner
Keyword(s):  
Oxalic Acid ◽  
Acid Solution ◽  
Active Sites ◽  
Oxalic Acid Solution ◽  
Ice Nucleation ◽  
Sodium Oxalate ◽  
Supersaturated Solution ◽  
Oxalic Acid Dihydrate ◽  
Condensation Mode ◽  
Heterogeneous Ice Nucleation

Abstract. The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers of oxalic acid or its salts may be formed by physical and chemical processing on pre-existing particulates such as mineral dust and soot. Given the broad diversity of the observed heterogeneous ice nucleability of the oxalate species, it is not straightforward to predict whether an oxalate coating layer will improve or reduce the ice nucleation ability of the seed aerosol particles.

scholarly journals The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust

2018 ◽  
Vol 11 (1) ◽  
pp. 233-248 ◽  
Author(s):  
Naama Reicher ◽  
Lior Segev ◽  
Yinon Rudich
Keyword(s):  
Active Surface ◽  
Ice Nucleation ◽  
Saharan Dust ◽  
Dust Particles ◽  
Active Surface Site ◽  
Immersion Freezing ◽  
Measurement Uncertainties ◽  
Homogeneous Freezing ◽  
Validation Experiments

Abstract. The WeIzmann Supercooled Droplets Observation on Microarray (WISDOM) is a new setup for studying ice nucleation in an array of monodisperse droplets for atmospheric implications. WISDOM combines microfluidics techniques for droplets production and a cryo-optic stage for observation and characterization of freezing events of individual droplets. This setup is designed to explore heterogeneous ice nucleation in the immersion freezing mode, down to the homogeneous freezing of water (235 K) in various cooling rates (typically 0.1–10 K min−1). It can also be used for studying homogeneous freezing of aqueous solutions in colder temperatures. Frozen fraction, ice nucleation active surface site densities and freezing kinetics can be obtained from WISDOM measurements for hundreds of individual droplets in a single freezing experiment. Calibration experiments using eutectic solutions and previously studied materials are described. WISDOM also allows repeatable cycles of cooling and heating for the same array of droplets. This paper describes the WISDOM setup, its temperature calibration, validation experiments and measurement uncertainties. Finally, application of WISDOM to study the ice nucleating particle (INP) properties of size-selected ambient Saharan dust particles is presented.

scholarly journals Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures

2005 ◽  
Vol 5 (3) ◽  
pp. 3391-3436 ◽  
Author(s):  
C. M. Archuleta ◽  
P. J. DeMott ◽  
S. M. Kreidenweis
Keyword(s):  
Sulfuric Acid ◽  
Relative Humidity ◽  
Mineral Dust ◽  
Aerosol Particles ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Nucleation Behavior ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. This study examines the potential role of some types of mineral dust and mineral dust with sulfuric acid coatings as heterogeneous ice nuclei at cirrus temperatures. Commercially-available nanoscale powder samples of aluminum oxide, alumina-silicate and iron oxide were used as surrogates for atmospheric mineral dust particles, with and without multilayer coverage of sulfuric acid. A sample of Asian dust aerosol particles was also studied. Measurements of ice nucleation were made using a continuous-flow ice-thermal diffusion chamber (CFDC) operated to expose size-selected aerosol particles to temperatures between −45 and −60°C and a range of relative humidity above ice-saturated conditions. Pure metal oxide particles supported heterogeneous ice nucleation at lower relative humidities than those required to homogeneously freeze sulfuric acid solution particles at sizes larger than about 50 nm. The ice nucleation behavior of the same metal oxides coated with sulfuric acid indicate heterogeneous freezing at lower relative humidities than those calculated for homogeneous freezing of the diluted particle coatings. The effect of soluble coatings on the ice activation relative humidity varied with the respective uncoated core particle types, but for all types the heterogeneous freezing rates increased with particle size for the same thermodynamic conditions. For a selected size of 200 nm, the natural mineral dust particles were the most effective ice nuclei tested, supporting heterogeneous ice formation at an ice relative humidity of approximately 135%, irrespective of temperature. Modified homogeneous freezing parameterizations and theoretical formulations are shown to have application to the description of heterogeneous freezing of mineral dust-like particles with soluble coatings.

scholarly journals Some ice nucleation characteristics of Asian and Saharan desert dust

2006 ◽  
Vol 6 (1) ◽  
pp. 1509-1537 ◽  
Author(s):  
P. R. Field ◽  
O. Möhler ◽  
P. Connolly ◽  
M. Krämer ◽  
R. Cotton ◽  
...  
Keyword(s):  
Ice Nucleation ◽  
Cloud Chamber ◽  
Ice Crystals ◽  
Nucleation Event ◽  
Secondary Nucleation ◽  
Desert Dust ◽  
Nucleation Mode ◽  
Primary Nucleation ◽  
Condensation Mode ◽  
Deposition Mode

Abstract. The large (7 m×4 m cylinder) AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber facility at Forschungszentrum, Karlsruhe, Germany was used to test the ice nucleating ability of two desert dust samples from the Sahara and Asia. At temperatures warmer than −40°C droplets were formed before ice crystals formed, there was no deposition nucleation observed. At temperatures colder than −40°C both dust samples exhibited dual nucleation events that were observed during the same expansion experiment. The primary nucleation event occurred at ice saturation ratios of 1.1 to 1.3 and is likely to be a deposition nucleation mode. The secondary nucleation event occurred at ice saturation ratios between 1.35 and 1.5. It is unclear whether this ice nucleation event is via a further deposition mode or a condensation mode. The activated fractions of desert dust ranged from ~5–10% at −20°C to 20–40% at temperatures colder than −40°C. There was no obvious difference between the nucleation behaviour of the two dust samples.

scholarly journals Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures

2005 ◽  
Vol 5 (10) ◽  
pp. 2617-2634 ◽  
Author(s):  
C. M. Archuleta ◽  
P. J. DeMott ◽  
S. M. Kreidenweis
Keyword(s):  
Sulfuric Acid ◽  
Relative Humidity ◽  
Mineral Dust ◽  
Aerosol Particles ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Nucleation Behavior ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. This study examines the potential role of some types of mineral dust and mineral dust with sulfuric acid coatings as heterogeneous ice nuclei at cirrus temperatures. Commercially-available nanoscale powder samples of aluminum oxide, alumina-silicate and iron oxide were used as surrogates for atmospheric mineral dust particles, with and without multilayer coverage of sulfuric acid. A sample of Asian dust aerosol particles was also studied. Measurements of ice nucleation were made using a continuous-flow ice-thermal diffusion chamber (CFDC) operated to expose size-selected aerosol particles to temperatures between -45 and -60°C and a range of relative humidity above ice-saturated conditions. Pure metal oxide particles supported heterogeneous ice nucleation at lower relative humidities than those required to homogeneously freeze sulfuric acid solution particles at sizes larger than about 50 nm. The ice nucleation behavior of the same metal oxides coated with sulfuric acid indicate heterogeneous freezing at lower relative humidities than those calculated for homogeneous freezing of the diluted particle coatings. The effect of soluble coatings on the ice activation relative humidity varied with the respective uncoated core particle types, but for all types the heterogeneous freezing rates increased with particle size for the same thermodynamic conditions. For a selected size of 200 nm, the natural mineral dust particles were the most effective ice nuclei tested, supporting heterogeneous ice formation at an ice relative humidity of approximately 135%, irrespective of temperature. Modified homogeneous freezing parameterizations and theoretical formulations are shown to have application to the description of heterogeneous freezing of mineral dust-like particles with soluble coatings.

scholarly journals Deposition nucleation viewed as homogeneous or immersion freezing in pores and cavities

2014 ◽  
Vol 14 (4) ◽  
pp. 2071-2104 ◽  
Author(s):  
C. Marcolli
Keyword(s):  
Water Vapor ◽  
Relative Humidity ◽  
Clay Minerals ◽  
Liquid Water ◽  
Vapor Deposition ◽  
Ice Nucleation ◽  
Classical View ◽  
Immersion Freezing ◽  
Kelvin Effect ◽  
Mcm 41

Abstract. Heterogeneous ice nucleation is an important mechanism for the glaciation of mixed phase clouds and may also be relevant for cloud formation and dehydration at the cirrus cloud level. It is thought to proceed through different mechanisms, namely contact, condensation, immersion and deposition nucleation. Conceptually, deposition nucleation is the only pathway that does not involve liquid water, but occurs by direct water vapor deposition onto a surface. This study challenges this classical view by putting forward the hypothesis that what is called deposition nucleation is in fact pore condensation and freezing (PCF) occurring in voids and cavities that may form between aggregated primary particles and host water at relative humidity RHw < 100% because of the inverse Kelvin effect. Homogeneous ice nucleation is expected to occur below 235 K when at least one pore is filled with water. Ice nucleation in pores may also happen in immersion mode but with a lower probability because it requires at least one active site in a water filled pore. Therefore a significant enhancement in ice nucleation efficiency is expected when temperature falls below 235 K. For a deposition nucleation process from water vapor no discontinuous change in ice nucleation efficiency should occur at T = 235 K because no liquid water is involved in this process. Studies on freezing in confinement carried out on mesoporous silica materials such as SBA-15, SBA-16, MCM-41, zeolites and KIT have shown that homogeneous ice nucleation occurs abruptly at T = 230–235 K in pores with diameters (D) of 3.5–4 nm or larger but only gradually at T = 210–230 K in pores with D = 2.5–3.5 nm. Pore analysis of clay minerals shows that kaolinites exhibit pore structures with pore diameters (Dp) of 20–50 nm. The mesoporosity of illites and montmorillonites is characterized by pores with Dp = 2–5 nm. The number and size of pores is distinctly increased in acid treated montmorillonites like K10. Water adsorption isotherms of MCM-41 show that pores with Dp = 3.5–4 nm fill with water at RHw = 56–60% in accordance with an inverse Kelvin effect. Water in such pores should freeze homogeneously for T < 235 K even before relative humidity with respect to ice (RHi) reaches ice saturation. Ice crystal growth by water vapor deposition from the gas phase is therefore expected to set in as soon as RHi > 100%. Pores with D > 7.5 nm fill with water at RHi > 100% for T < 235 K and are likely to freeze homogeneously as soon as they are filled with water. Given the pore structure of clay minerals, PCF should be highly efficient for T < 235 K and may occur at T > 235 K in particles that exhibit active sites for immersion freezing within pores. Most ice nucleation studies on clay minerals and mineral dusts indeed show a strong increase in ice nucleation efficiency when temperature is decreased below 235 K in accordance with PCF and are not explicable by the classical view of deposition nucleation. PCF is probably also the prevailing ice nucleation mechanism below water saturation for glassy, soot, and volcanic ash aerosols. No case could be identified that gives clear evidence of ice nucleation by water vapor deposition onto a solid surface.

scholarly journals Heterogeneous ice nucleation activity of bacteria: new laboratory experiments at simulated cloud conditions

2008 ◽  
Vol 5 (2) ◽  
pp. 1445-1468 ◽  
Author(s):  
O. Möhler ◽  
D. G. Georgakopoulos ◽  
C. E. Morris ◽  
S. Benz ◽  
V. Ebert ◽  
...  
Keyword(s):  
Pseudomonas Syringae ◽  
Cloud Condensation Nuclei ◽  
Bacterial Species ◽  
Ice Nucleation ◽  
Cloud Chamber ◽  
Bacterial Cells ◽  
Spray Formation ◽  
Temperature Range ◽  
Expansion Cooling ◽  
Activation Conditions

Abstract. The ice nucleation activities of five different Pseudomonas syringae, Pseudomonas viridiflava and Erwinia herbicola bacterial species and of SnomaxTM were investigated in the temperature range between −5 and −15°C. Water suspensions of these bacteria were directly spray into the cloud chamber of the AIDA facility of Forschungszentrum Karlsruhe at a temperature of −5.7°. At this temperature, about 1% of the SnomaxTM cells induced freezing of the spray droplets before they evaporated in the cloud chamber. The other suspensions of living cells didn't induce any measurable ice concentration during spray formation at −5.7°. The remaining aerosol was exposed to typical cloud activation conditions in subsequent experiments with expansion cooling to about −11°C. During these experiments, the bacterial cells first acted as cloud condensation nuclei to form cloud droplets and then eventually acted as ice nuclei to freeze the droplets. The results indicate that the bacteria investigated in the present study are mainly ice active in the temperature range between −7 and −11°C with an INA fraction of the order of 10−4. The ice nucleation efficiency of SnomaxTM cells was much larger with an INA fraction of 0.2 at temperatures around −8°C.

scholarly journals Probing ice clouds by broadband mid-infrared extinction spectroscopy: case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber

2006 ◽  
Vol 6 (12) ◽  
pp. 4775-4800 ◽  
Author(s):  
R. Wagner ◽  
S. Benz ◽  
O. Möhler ◽  
H. Saathoff ◽  
U. Schurath
Keyword(s):  
Size Distribution ◽  
Particle Number ◽  
Ice Nucleation ◽  
Number Concentration ◽  
Cloud Chamber ◽  
Ice Crystals ◽  
Ice Clouds ◽  
Number Size Distribution ◽  
Ice Particles ◽  
Infrared Extinction

Abstract. Series of infrared extinction spectra of ice crystals were recorded in the 6000–800 cm−1 wavenumber regime during expansion cooling experiments in the large aerosol and cloud chamber AIDA of Forschungszentrum Karlsruhe. Either supercooled sulphuric acid solution droplets or dry mineral dust particles were added as seed aerosols to initiate ice formation after having established ice supersaturated conditions inside the chamber. The various ice nucleation runs were conducted at temperatures between 237 and 195 K, leading to median sizes of the nucleated ice particles of 1–15 µm. The measured infrared spectra were fitted with reference spectra from T-matrix calculations to retrieve the number concentration as well as the number size distribution of the generated ice clouds. The precise evaluation of the time-dependent ice particle number concentrations, i.e., the rates of new ice particle formation, is of particular importance to quantitatively analyse the ice nucleation experiments in terms of nucleation rates and ice activation spectra. The ice particles were modelled as finite circular cylinders with aspect ratios ranging from 0.5 to 3.0. Benefiting from the comprehensive diagnostic tools for the characterisation of ice clouds which are available at the AIDA facility, the infrared retrieval results with regard to the ice particle number concentration could be compared to independent measurements with various optical particle counters. This provided a unique chance to quantitatively assess potential errors or solution ambiguities in the retrieval procedure which mainly originate from the difficulty to find an appropriate shape representation for the aspherical particle habits of the ice crystals. Based on these inter-comparisons, we demonstrate that there is no standard retrieval approach which can be routinely applied to all different experimental scenarios. In particular, the concept to account for the asphericity of the ice crystals, the a priori constraints which might be imposed on the unknown number size distribution of the ice crystals (like employing an analytical distribution function), and the wavenumber range which is included in the fitting algorithm should be carefully adjusted to each single retrieval problem.

scholarly journals High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

2010 ◽  
Vol 10 (4) ◽  
pp. 11513-11575
Author(s):  
R. Wagner ◽  
O. Möhler ◽  
H. Saathoff ◽  
M. Schnaiter ◽  
T. Leisner
Keyword(s):  
Oxalic Acid ◽  
Acid Solution ◽  
Active Sites ◽  
Oxalic Acid Solution ◽  
Ice Nucleation ◽  
Sodium Oxalate ◽  
Supersaturated Solution ◽  
Oxalic Acid Dihydrate ◽  
Condensation Mode ◽  
Heterogeneous Ice Nucleation

Abstract. The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers of oxalic acid or its salts may be formed by physical and chemical processing on pre-existing particulates such as mineral dust and soot. Given the broad diversity of the observed heterogeneous ice nucleability of the oxalate species, it is not straightforward to predict whether an oxalate coating layer will improve or reduce the ice nucleation ability of the seed aerosol particles.

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