Anthony J. Prenni

Predicting global atmospheric ice nuclei distributions and their impacts on climate

Knowledge of cloud and precipitation formation processes remains incomplete, yet global precipitation is predominantly produced by clouds containing the ice phase. Ice first forms in clouds warmer than -36 °C on particles termed ice nuclei. We combine observations from field studies over a 14-year period, from a variety of locations around the globe, to show that the concentrations of ice nuclei active in mixed-phase cloud conditions can be related to temperature and the number concentrations of particles larger than 0.5 μm in diameter. This new relationship reduces unexplained variability in ice nuclei concentrations at a given temperature from ∼103 to less than a factor of 10, with the remaining variability apparently due to variations in aerosol chemical composition or other factors. When implemented in a global climate model, the new parameterization strongly alters cloud liquid and ice water distributions compared to the simple, temperature-only parameterizations currently widely used. The revised treatment indicates a global net cloud radiative forcing increase of ∼1 W m-2 for each order of magnitude increase in ice nuclei concentrations, demonstrating the strong sensitivity of climate simulations to assumptions regarding the initiation of cloud glaciation.

Measurements of the concentration and composition of nuclei for cirrus formation

This article addresses the need for new data on indirect effects of natural and anthropogenic aerosol particles on atmospheric ice clouds. Simultaneous measurements of the concentration and composition of tropospheric aerosol particles capable of initiating ice in cold (cirrus) clouds are reported. Measurements support that cirrus formation occurs both by heterogeneous nucleation by insoluble particles and homogeneous (spontaneous) freezing of particles containing solutions. Heterogeneous ice nuclei concentrations in the cirrus regime depend on temperature, relative humidity, and the concentrations and physical and chemical properties of aerosol particles. The cirrus-active concentrations of heterogeneous nuclei measured in November over the western U.S. were <0.03 cm–3. Considering previous modeling studies, this result suggests a predominant potential impact of these nuclei on cirrus formed by slow, large-scale lifting or small cooling rates, including subvisual cirrus. The most common heterogeneous ice nuclei were identified as relatively pure mineral dusts and metallic particles, some of which may have origin through anthropogenic processes. Homogeneous freezing of large numbers of particles was detected above a critical relative humidity along with a simultaneous transition in nuclei composition toward that of the sulfate-dominated total aerosol population. The temperature and humidity conditions of the homogeneous nucleation transition were reasonably consistent with expectations based on previous theoretical and laboratory studies but were highly variable. The strong presence of certain organic pollutants was particularly noted to be associated with impedance of homogeneous freezing.

Rainforest aerosols as biogenic nuclei of clouds and precipitation in the Amazon.

Clean or Dirty Aerosols strongly affect atmospheric properties and processes—including visibility, cloud formation, and radiative behavior. Knowing their effects in both clean and polluted air is necessary in order to understand their influence (see the Perspective by Baltensperger). Clarke and Kapustin (p. 1488) examine vertical atmospheric profiles collected above the Pacific Ocean, where air quality is affected by the transport of polluted air from the west, and find significant regional enhancements in light scattering, aerosol mass, and aerosol number associated with combustion. Aerosol particle concentrations in this region can exceed values in clean, unperturbed regions by over an order of magnitude. Thus combustion affects hemispheric aerosol optical depth and the distribution of cloud condensation nuclei. Pöschl et al. (p. 1513) discuss the composition of aerosols above the Amazon Basin, in the pristine conditions of the rainy season. The aerosols in this region are derived mostly from gaseous biogenic precursors, plants, and microorganisms, and particle concentration is orders of magnitude lower than in polluted continental regions. The majority of cloud condensation nuclei in the Amazon during the wet season are derived from biogenic precursors. The Amazon is one of the few continental regions where atmospheric aerosol particles and their effects on climate are not dominated by anthropogenic sources. During the wet season, the ambient conditions approach those of the pristine pre-industrial era. We show that the fine submicrometer particles accounting for most cloud condensation nuclei are predominantly composed of secondary organic material formed by oxidation of gaseous biogenic precursors. Supermicrometer particles, which are relevant as ice nuclei, consist mostly of primary biological material directly released from rainforest biota. The Amazon Basin appears to be a biogeochemical reactor, in which the biosphere and atmospheric photochemistry produce nuclei for clouds and precipitation sustaining the hydrological cycle. The prevailing regime of aerosol-cloud interactions in this natural environment is distinctly different from polluted regions.

Impacts of Nucleating Aerosol on Florida Storms. Part I: Mesoscale Simulations

Abstract Toward the end of the Cirrus Regional Study of Tropical Anvils and Cirrus Layer–Florida Area Cirrus Experiment (CRYSTAL–FACE) field campaign held during July 2002, high concentrations of Saharan dust, which can serve as cloud condensation nuclei (CCN), giant CCN (GCCN), and ice-forming nuclei (IFN) were observed over the peninsula of Florida. To investigate the impacts of enhanced aerosol concentrations on the characteristics of convective storms and their subsequent anvil development, sensitivity tests are conducted using the Regional Atmospheric Modeling System (RAMS) model, in which the initialization profiles of CCN, GCCN, and IFN concentrations are varied. These variations are found to have significant effects on the storm dynamics and microphysical processes, as well as on the surface precipitation. Updrafts are consistently stronger as the aerosol concentrations are increased. The anvils cover a smaller area but are better organized and have larger condensate mixing ratio maxima in the cas...

The Mixed-Phase Arctic Cloud Experiment

The Mixed-Phase Arctic Cloud Experiment (M-PACE) was conducted from 27 September through 22 October 2004 over the Department of Energys Atmospheric Radiation Measurement (ARM) Climate Research Facility (ACRF) on the North Slope of Alaska. The primary objectives were to collect a dataset suitable to study interactions between microphysics, dynamics, and radiative transfer in mixed-phase Arctic clouds, and to develop/evaluate cloud property retrievals from surface-and satellite-based remote sensing instruments. Observations taken during the 1977/98 Surface Heat and Energy Budget of the Arctic (SHEBA) experiment revealed that Arctic clouds frequently consist of one (or more) liquid layers precipitating ice. M-PACE sought to investigate the physical processes of these clouds by utilizing two aircraft (an in situ aircraft to characterize the microphysical properties of the clouds and a remote sensing aircraft to constraint the upwelling radiation) over the ACRF site on the North Slope of Alaska. The measureme...

Water uptake of internally mixed particles containing ammonium sulfate and dicarboxylic acids

Abstract There is increasing evidence that organic compounds comprise a significant fraction of tropospheric particles at all altitudes. The presence of these compounds can affect the particles’ ability to take up water and to form ice in the atmosphere. In this paper we present studies that investigate the hygroscopic behavior of internal mixtures of ammonium sulfate and low molecular weight dicarboxylic acids. We find that the ammonium sulfate dominates water uptake behavior for mixtures that contain 100:1 and 10:1 mass ratios of ammonium sulfate:dicarboxylic acid. However, for 1:1 mixtures, the dicarboxylic acids play an important role in determining water uptake characteristics. Observed water contents can be predicted within experimental uncertainties by assuming that each component contributes independently to the total particle water content, in accord with previous measurements for the pure components.

Can Ice-Nucleating Aerosols Affect Arctic Seasonal Climate?

Mixed-phase stratus clouds are ubiquitous in the Arctic and play an important role in climate in this region. However, climate and regional models have generally proven unsuccessful at simulating Arctic cloudiness, particularly during the colder months. Specifically, models tend to underpredict the amount of liquid water in mixed-phase clouds. The Mixed-Phase Arctic Cloud Experiments (M-PACE), conducted from late September through October 2004 in the vicinity of the Department of Energys Atmospheric Radiation Measurement (ARM) North Slope of Alaska field site, focused on characterizing low-level Arctic stratus clouds. Ice nuclei (IN) measurements were made using a continuous-flow ice thermal diffusion chamber aboard the University of North Dakotas Citation II aircraft. These measurements indicated IN concentrations that were significantly lower than those used in many models. Using the Regional Atmospheric Modeling System (RAMS), we show that these low IN concentrations, as well as inadequate parameteri...

Infrared spectroscopic study of the deliquescence and efflorescence of ammonium sulfate aerosol as a function of temperature

The deliquescence and efflorescence phase transitions of ammonium sulfate aerosols have been studied as a function of relative humidity (RH) over the temperature range from 234 K to 295 K. Polydisperse submicrometer ammonium sulfate particles produced by atomization were monitored in a temperature-controlled flow tube system using Fourier transform infrared spectroscopy. The relative humidity in the aerosol flow was controlled using a sulfuric acid bath conditioner and the addition of a known flow of dry nitrogen. The relative humidity was measured using a dew point hygrometer and infrared absorption features. The deliquescence transition was observed to be nearly independent of temperature, changing from 80% RH at 294.8 K to 82% RH at 258.0 K near the ice saturation line, in good agreement with previous results. The relative humidity at the efflorescence transition also increased slightly (32% to 39%) with decreasing temperature (294.8 K to 234.3 K). These results suggest that once a crystalline ammonium sulfate particle deliquesces, the droplet can exist as a metastable solution droplet over a broad region of temperature and water pressures under the conditions in the upper troposphere. The persistence of metastable ammonium sulfate solution droplets may have important implications for cirrus cloud formation and heterogeneous reaction rates in the upper troposphere.

Ice Initiation by Aerosol Particles: Measured and Predicted Ice Nuclei Concentrations versus Measured Ice Crystal Concentrations in an Orographic Wave Cloud

The initiation of ice in an isolated orographic wave cloud was compared with expectations based on ice nucleating aerosol concentrations and with predictions from new ice nucleation parameterizations applied in a cloud parcel model. Measurements of ice crystal number concentrations were found to be in good agreement both with measured number concentrations of ice nuclei feeding the clouds and with ice nuclei number concentrations determined from the residual nuclei of cloud particles collected by a counterflow virtual impactor. Using lognormal distributions fitted to measured aerosol size distributions and measured aerosol chemical compositions, ice nuclei and ice crystal concentrations in the wave cloud were reasonably well predicted in a 1D parcel model framework. Two different empirical parameterizations were used in the parcel model: a parameterization based on aerosol chemical type and surface area and a parameterization that links ice nuclei number concentrations to the number concentrations of particles with diameters larger than 0.5 μm. This study shows that aerosol size distribution and composition measurements can be used to constrain ice initiation by primary nucleation in models. The data and model results also suggest the likelihood that the dust particle mode of the aerosol size distribution controls the number concentrations of the heterogeneous ice nuclei, at least for the lower temperatures examined in this case.

Freezing of polar stratospheric clouds in orographically induced strong warming events

Results from laboratory experiments and microphysical modeling are presented that suggest a potential freezing nucleation mechanism for polar stratospheric cloud (PSC) particles above the water ice frost point (Tice). The mechanism requires very high HNO3 concentrations of about 58 wt% in the droplets, and leads to the freezing of nitric acid dihydrate (NAD) in a highly selective manner in the smallest droplets of an ensemble. In the stratosphere such liquid compositions are predicted to occur in aerosol droplets which are warmed adiabatically with rates of about +150 K/h from below 190 K to 194 K. Such rapid temperature changes have been observed in mountain leewaves that occur frequently in the stratosphere, clearly demonstrating the need for a stratospheric gravity wave climatology.