Surface modification of mineral dust particles by sulphuric acid processing: implications for ice nucleation abilities

Reitz, P.; Spindler, C.; Mentel, Thomas F.; Poulain, Laurent; Wex, Heike; Mildenberger, K.; Niedermeier, D.; Hartmann, S.; Clauß, T.; Stratmann, Frank; Sullivan, R. C.; DeMott, Paul J.; Petters, M. D.; Sierau, B.; Schneider, Johannes

doi:10.5194/acp-11-7839-2011

Cited by 61 publications

(77 citation statements)

References 54 publications

(70 reference statements)

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“…Some of the laboratory experiments included particle coatings with secondary organic aerosol, which appeared to have no signifi-cant impact on immersion freezing (to be elaborated on in a future publication). Additionally, we may note that a number of previous studies suggest little influence of aging on immersion freezing of activated cloud droplets by mineral dusts, unless reactions occur between the condensed species and the mineral surface that impact the efficiency of active sites (Sullivan et al, 2010a, b;Niedermeier et al, 2011a;Reitz et al, 2011). Our investigations support that a calibration factor on CFDC INP concentrations is needed to account for instrumental factors if the intent is to describe the full expression of condensation/immersion freezing by natural mineral dust particles.…”

Section: Discussionsupporting

confidence: 61%

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

et al. 2015

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Abstract. Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105 % relative humidity with respect to water (RH w ) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of nonspecific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 µm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RH w of 105 % vs. maximum fractions active at higher RH w . Instrumental factors that affect activation behavior vs. RH w in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.Published by Copernicus Publications on behalf of the European Geosciences Union.

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Section: Discussionsupporting

confidence: 61%

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

et al. 2015

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“…This approach allows for aerosol particle number concentrations to be evaluated by particle composition as well as the probing of internal mixing state that cannot be done by bulk analysis techniques (e.g. Pratt and Prather, 2010;Zelenyuk et al, 2010;Reitz et al, 2011). The type of material that can be analysed is determined by the power and wavelength of the pulsed laser system, whilst the temporal resolution is related to the probability that a particle will be coincident with the laser pulse in the ion source, a phenomenon often referred to as hit rate.…”

Section: Introductionmentioning

confidence: 99%

Evaluating the influence of laser wavelength and detection stage geometry on optical detection efficiency in a single-particle mass spectrometer

et al. 2016

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Abstract. Single-particle mass spectrometry (SPMS) is a useful tool for the online study of aerosols with the ability to measure size-resolved chemical composition with a temporal resolution relevant to atmospheric processes. In SPMS, optical particle detection is used for the effective temporal alignment of an ablation laser pulse with the presence of a particle in the ion source, and it gives the option of aerodynamic sizing by measuring the offset of particle arrival times between two detection stages. The efficiency of the optical detection stage has a strong influence on the overall instrument performance.A custom detection laser system consisting of a highpowered fibre-coupled Nd:YAG solid-state laser with a collimated beam was implemented in the detection stage of a laser ablation aerosol particle time-of-flight (LAAP-TOF) singleparticle mass spectrometer without major modifications to instrument geometry. The use of a collimated laser beam permitted the construction of a numerical model that predicts the effects of detection laser wavelength, output power, beam focussing characteristics, light collection angle, particle size, and refractive index on the effective detection radius (R) of the detection laser beam. We compare the model predictions with an ambient data set acquired during the Ice in Clouds Experiment -Dust (ICE-D) project.The new laser system resulted in an order-of-magnitude improvement in instrument sensitivity to spherical particles in the size range 500-800 nm compared to a focussed 405 nm laser diode system. The model demonstrates that the limit of detection in terms of particle size is determined by the scattering cross section (C sca ) as predicted by Mie theory. In addition, if light is collected over a narrow collection angle, oscillations in the magnitude of C sca with respect to particle diameter result in a variation in R, resulting in large particlesize-dependent variation in detection efficiency across the particle transmission range. This detection bias is imposed on the aerodynamic size distributions measured by the instrument and accounts for some of the detection bias towards sea salt particles in the ambient data set.

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“…Our study is related to the investigations described in Sullivan et al (2010a) and Reitz et al (2011). Sullivan et al (2010a) determined the IN ability of the particles in the deposition nucleation and immersion/condensation freezing mode at two distinct temperatures: −25 • C and −30 • C using the Continuous Flow thermal gradient Diffusion Chamber (CFDC).…”

Section: Introductionmentioning

confidence: 99%

Experimental study of the role of physicochemical surface processing on the IN ability of mineral dust particles

et al. 2011

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Abstract. During the measurement campaign FROST 2 (FReezing Of duST 2), the Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the influence of various surface modifications on the ice nucleating ability of Arizona Test Dust (ATD) particles in the immersion freezing mode. The dust particles were exposed to sulfuric acid vapor, to water vapor with and without the addition of ammonia gas, and heat using a thermodenuder operating at 250 • C. Size selected, quasi monodisperse particles with a mobility diameter of 300 nm were fed into LACIS and droplets grew on these particles such that each droplet contained a single particle. Temperature dependent frozen fractions of these droplets were determined in a temperature range between −40 • C ≤T ≤−28 • C. The pure ATD particles nucleated ice over a broad temperature range with their freezing behavior being separated into two freezing branches characterized through different slopes in the frozen fraction vs. temperature curves. Coating the ATD particles with sulfuric acid resulted in the particles' IN potential significantly decreasing in the first freezing branch (T >−35 • C) and a slight increase in the second branch (T ≤−35 • C). The addition of water vapor after the sulfuric acid coating caused the disappearance Correspondence to: D. Niedermeier (niederm@tropos.de) of the first freezing branch and a strong reduction of the IN ability in the second freezing branch. The presence of ammonia gas during water vapor exposure had a negligible effect on the particles' IN ability compared to the effect of water vapor. Heating in the thermodenuder led to a decreased IN ability of the sulfuric acid coated particles for both branches but the additional heat did not or only slightly change the IN ability of the pure ATD and the water vapor exposed sulfuric acid coated particles. In other words, the combination of both sulfuric acid and water vapor being present is a main cause for the ice active surface features of the ATD particles being destroyed. A possible explanation could be the chemical transformation of ice active metal silicates to metal sulfates. The strongly enhanced reaction between sulfuric acid and dust in the presence of water vapor and the resulting significant reductions in IN potential are of importance for atmospheric ice cloud formation. Our findings suggest that the IN concentration can decrease by up to one order of magnitude for the conditions investigated.

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Surface modification of mineral dust particles by sulphuric acid processing: implications for ice nucleation abilities

Cited by 61 publications

References 54 publications

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

Evaluating the influence of laser wavelength and detection stage geometry on optical detection efficiency in a single-particle mass spectrometer

Experimental study of the role of physicochemical surface processing on the IN ability of mineral dust particles

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