Ice Nucleation in Sulfuric Acid and Ammonium Sulfate Particles

Cirrus clouds are composed of ice particles and are expected to form in the upper troposphere when highly dilute sulfate aerosols cool and become supersaturated with respect to ice. In the laboratory we have used Fourier transform infrared spectroscopy to monitor ice nucleation from sulfate particles for relevant compositions of sulfuric acid/water and ammonium sulfate/water aerosols. Measured freezing temperatures are presented as a function of aerosol composition, and results are compared to existing aerosol data. We find that sulfuric acid solution aerosol exhibits greater supercooling than ammonium sulfate solution aerosol of similar weight percent. Ice saturation ratios based on these measurements are also reported. We find that ammonium sulfate solution aerosol exhibits a relatively constant ice saturation of S∼1.48 for ice nucleation from 232 to 222 K, while sulfuric acid solution aerosol shows an increase in ice saturation from S∼1.53 to S∼1.6 as temperature decreases from 220 K to 200 K. These high-saturation ratios imply selective nucleation of ice from sulfate aerosols

Aerosol microphysical impact on summertime convective precipitation in the Rocky Mountain region

We present an aerosol-cloud-precipitation modeling study of convective clouds using the Weather Research and Forecasting model fully coupled with Chemistry (WRF-Chem) version 3.1.1. Comparison of the model output with measurements from a research site in the Rocky Mountains in Colorado revealed that the fraction of organics in the model is underpredicted. This is most likely due to missing processes in the aerosol module in the model version used, such as new particle formation and growth of secondary organic aerosols. When boundary conditions and domain-wide initial conditions of aerosol loading are changed in the model (factors of 0.1, 0.2, and 10 of initial aerosol mass of SO4-2, NH4+, and NO3-), the domain-wide precipitation changes by about 5%. Analysis of the model results reveals that the Rocky Mountain region and Front Range environment is not conducive for convective invigoration to play a major role, in increasing precipitation, as seen in some other studies. When localized organic aerosol emission are increased to mimic new particle formation, the resulting increased aerosol loading leads to increases in domain-wide precipitation, opposite to what is seen in the model simulations with changed boundary and initial conditions

Phase Changes in Internally Mixed Maleic Acid/Ammonium Sulfate Aerosols

A temperature controlled flow tube system equipped with Fourier transform infrared (FTIR) detection of particle phase and relative humidity was used to measure the deliquescence and efflorescence of ammonium sulfate, maleic acid, and internally mixed maleic acid/ammonium sulfate particles. Our results indicate that maleic acid aerosols begin to take up water starting at a low relative humidity, ∼20%, and continue the constant uptake of water until the final deliquescence relative humidity (DRH), 89%, is reached. Internally mixed particles containing maleic acid and ammonium sulfate were found to deliquesce at a lower relative humidity (RH) than either of the pure species. Efflorescence studies indicated that while pure maleic acid particles crystallize at ∼18% RH, pure ammonium sulfate and all mixed aerosols effloresce at or just below 30% RH. Taken together, our results suggest that the presence of water-soluble organics internally mixed with ammonium sulfate aerosol could increase the range of conditions under which the aerosol is a solution

Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol

Ice nucleation abilities of surface collected mineral dust particles from the Sahara (SD) and Asia (AD) are investigated for the temperature (T) range 253–233 K and for supersaturated relative humidity (RH) conditions in the immersion freezing regime. The dust particles were also coated with a proxy of secondary organic aerosol (SOA) from the dark ozonolysis of α-pinene to better understand the influence of atmospheric coatings on the immersion freezing ability of mineral dust particles. The measurements are conducted on polydisperse particles in the size range 0.01–3 µm with three different ice nucleation chambers. Two of the chambers follow the continuous flow diffusion chamber (CFDC) principle (Portable Ice Nucleation Chamber, PINC) and the Colorado State University CFDC (CSU-CFDC), whereas the third was the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) cloud expansion chamber. From observed activated fractions (AFs) and ice nucleation active site (INAS) densities, it is concluded within experimental uncertainties that there is no significant difference between the ice nucleation ability of the particular SD and AD samples examined. A small bias towards higher INAS densities for uncoated versus SOA-coated dusts is found but this is well within the 1σ (66 % prediction bands) region of the average fit to the data, which captures 75 % of the INAS densities observed in this study. Furthermore, no systematic differences are observed between SOA-coated and uncoated dusts in both SD and AD cases, regardless of coating thickness (3–60 nm). The results suggest that any differences observed are within the uncertainty of the measurements or differences in cloud chamber parameters such as size fraction of particles sampled, and residence time, as well as assumptions in using INAS densities to compare polydisperse aerosol measurements which may show variable composition with particle size. Coatings with similar properties to that of the SOA in this work and with coating thickness up to 60 nm are not expected to impede or enhance the immersion mode ice nucleation ability of mineral dust particles.ISSN:1680-7375ISSN:1680-736

Carlsbad Caverns National Park Air Quality Study 2019

This data set includes fine particle and gas precursor measurements from Carlsbad Caverns National Park. The study was designed to examine the influence of regional sources, including urban emissions, oil and gas development, wildfires, and soil dust on air quality in the park. Field measurements of aerosols, trace gases and deposition were conducted from 25 July through 5 September 2019.Carlsbad Caverns National Park in southeastern New Mexico is adjacent to the Permian Basin, one of the most productive oil and gas regions in the country. The 2019 Carlsbad Caverns Air Quality Study (CarCavAQS) was designed to examine the influence of regional sources, including urban emissions, oil and gas development, wildfires, and soil dust on air quality in the park. Field measurements of aerosols, trace gases, and deposition were conducted from 25 July through 5 September 2019.This work was supported by the National Park Service Q5 [P20AC00679]

Rapidly evolving ultrafine and fine mode biomass smoke physical properties: Comparing laboratory and field results

Combining field and laboratory results, we present biomass smoke physical properties. We report sub-0.56 µm diameter (Dp) particle sizing (fast mobility particle sizer, FMPS) plus light absorption and scattering at 870nm (photoacoustic extinctiometer). For Dp\u3c200 \u3enm, the FMPS characterized sizing within ±20% compared to standards. As compared to the traditional scanning mobility particle sizer, the FMPS responded most accurately to single-mode polydispersions with mean Dp\u3c200 \u3enm, which characterized the smoke sampled here. Smoke was measured from laboratory fresh emissions (seconds to hours old), the High Park Fire (hours to\u3c1 \u3eday), and from regional biomass burning (several days). During a High Park Fire episode, light extinction rapidly reached a maximum of σep = 569 ± 21Mm-1 (10 min) with aerosol single scattering albedo peaking at ω= 0.955 ± 0.004. Concurrently, number concentration and size peaked with maximum Dp = 126nm and a unimodal distribution with σg = 1.5. Long-range transported smoke was substantially diluted (Ntot factor of 7 lower) and shifted larger (maximum Dp = 143) and wider (σg = 2.2). We compared ambient data to laboratory burns with representative western U.S. forest fuels (coniferous species Ponderosa pine and Alaska black spruce). Smoldering pine produced an aerosol dominated by larger, more strongly light scattering particles (Dp\u3e100 nm), while flaming combustion produced very high number concentrations of smaller (Dp ~ 50 nm) absorbing particles. Due to smoldering and particle growth processes, Dp approached 100nm within 3 h after emission. Increased particle cross-sectional area and Mie scattering efficiency shifted the relative importance of light absorption (flaming maximum) and light scattering (smoldering maximum), increasing ω over time. Measurements showed a consistent picture of smoke properties from emission to aging

An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08)

The Amazon Basin provides an excellent environment for studying the sources, transformations, and properties of natural aerosol particles and the resulting links between biological processes and climate. With this framework in mind, the Amazonian Aerosol Characterization Experiment (AMAZE-08), carried out from 7 February to 14 March 2008 during the wet season in the central Amazon Basin, sought to understand the formation, transformations, and cloud-forming properties of fine- and coarse-mode biogenic aerosol particles, especially as related to their effects on cloud activation and regional climate. Special foci included (1) the production mechanisms of secondary organic components at a pristine continental site, including the factors regulating their temporal variability, and (2) predicting and understanding the cloud-forming properties of biogenic particles at such a site. In this overview paper, the field site and the instrumentation employed during the campaign are introduced. Observations and findings are reported, including the large-scale context for the campaign, especially as provided by satellite observations. New findings presented include: (i) a particle number-diameter distribution from 10 nm to 10 Î1/4m that is representative of the pristine tropical rain forest and recommended for model use; (ii) the absence of substantial quantities of primary biological particles in the submicron mode as evidenced by mass spectral characterization; (iii) the large-scale production of secondary organic material; (iv) insights into the chemical and physical properties of the particles as revealed by thermodenuder-induced changes in the particle number-diameter distributions and mass spectra; and (v) comparisons of ground-based predictions and satellite-based observations of hydrometeor phase in clouds. A main finding of AMAZE-08 is the dominance of secondary organic material as particle components. The results presented here provide mechanistic insight and quantitative parameters that can serve to increase the accuracy of models of the formation, transformations, and cloud-forming properties of biogenic natural aerosol particles, especially as related to their effects on cloud activation and regional climate. © 2010 Author(s)

Aerosol microphysical impact on summertime convective precipitation in the Rocky Mountain region

We present an aerosol-cloud-precipitation modeling study of convective clouds using the Weather Research and Forecasting model fully coupled with Chemistry (WRF-Chem) version 3.1.1. Comparison of the model output with measurements from a research site in the Rocky Mountains in Colorado revealed that the fraction of organics in the model is underpredicted. This is most likely due to missing processes in the aerosol module in the model version used, such as new particle formation and growth of secondary organic aerosols. When boundary conditions and domain-wide initial conditions of aerosol loading are changed in the model (factors of 0.1, 0.2, and 10 of initial aerosol mass of SO4-2, NH4+, and NO3-), the domain-wide precipitation changes by about 5%. Analysis of the model results reveals that the Rocky Mountain region and Front Range environment is not conducive for convective invigoration to play a major role, in increasing precipitation, as seen in some other studies. When localized organic aerosol emission are increased to mimic new particle formation, the resulting increased aerosol loading leads to increases in domain-wide precipitation, opposite to what is seen in the model simulations with changed boundary and initial conditions

Final Technical Report for "Ice nuclei relation to aerosol properties: Data analysis and model parameterization for IN in mixed-phase clouds" (DOE/SC00002354)

Clouds play an important role in weather and climate. In addition to their key role in the hydrologic cycle, clouds scatter incoming solar radiation and trap infrared radiation from the surface and lower atmosphere. Despite their importance, feedbacks involving clouds remain as one of the largest sources of uncertainty in climate models. To better simulate cloud processes requires better characterization of cloud microphysical processes, which can affect the spatial extent, optical depth and lifetime of clouds. To this end, we developed a new parameterization to be used in numerical models that describes the variation of ice nuclei (IN) number concentrations active to form ice crystals in mixed-phase (water droplets and ice crystals co-existing) cloud conditions as these depend on existing aerosol properties and temperature. The parameterization is based on data collected using the Colorado State University continuous flow diffusion chamber in aircraft and ground-based campaigns over a 14-year period, including data from the DOE-supported Mixed-Phase Arctic Cloud Experiment. The resulting relationship is shown to more accurately represent the variability of ice nuclei distributions in the atmosphere compared to currently used parameterizations based on temperature alone. When implemented in one global climate model, the new parameterization predicted more realistic annually averaged cloud water and ice distributions, and cloud radiative properties, especially for sensitive higher latitude mixed-phase cloud regions. As a test of the new global IN scheme, it was compared to independent data collected during the 2008 DOE-sponsored Indirect and Semi-Direct Aerosol Campaign (ISDAC). Good agreement with this new data set suggests the broad applicability of the new scheme for describing general (non-chemically specific) aerosol influences on IN number concentrations feeding mixed-phase Arctic stratus clouds. Finally, the parameterization was implemented into a regional cloud-resolving model to compare predictions of ice crystal concentrations and other cloud properties to those observed in two intensive case studies of Arctic stratus during ISDAC. Our implementation included development of a prognostic scheme of ice activation using the IN parameterization so that the most realistic treatment of ice nuclei, including their budget (gains and losses), was achieved. Many cloud microphysical properties and cloud persistence were faithfully reproduced, despite a tendency to under-predict (by a few to several times) ice crystal number concentrations and cloud ice mass, in agreement with some other studies. This work serves generally as the basis for improving predictive schemes for cloud ice crystal activation in cloud and climate models, and more specifically as the basis for such a scheme to be used in a Multi-scale Modeling Format (MMF) that utilizes a connected system of cloud-resolving models on a global grid in an effort to better resolve cloud processes and their influence on climate