Paul J. DeMott

New primary ice-nucleation parameterizations in an explicit cloud model

Abstract Two new primary ice-nucleation parameterizations are examined in the Regional Atmospheric Modeling System (RAMS) cloud model via sensitivity tests on a wintertime precipitation event in the Sierra Nevada region. A model combining the effects of deposition and condensation-freezing nucleation is formulated based on data obtained from continuous-flow diffusion chambers. The data indicate an exponential variation of ice-nuclei concentrations with ice supersaturation reasonably independent of temperatures between −7° and −20°C. Predicted ice concentrations from these measurements exceed values predicted by the widely used temperatures dependent Fletcher approximation by as much as one order of magnitude at temperatures warmer than −20°C. A contact-freezing nucleation model is also formulated based on laboratory data gathered by various authors using techniques that isolated this nucleation mode. Predicted contact nuclei concentrations based on the newer measurements are as much as three orders of mag...

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.

Dust and Biological Aerosols from the Sahara and Asia Influence Precipitation in the Western U.S.

Action at a Distance Snowfall in the Sierra Nevada provides a large fraction of the water that California receives as precipitation. Knowing what factors influence the amount of snow that falls is thus critical for projecting how water availability may change in the future. Aerosols have an important effect on cloud processes and precipitation. Creamean et al. (p. 1572, published online 28 February) found that dust and biological aerosols originating from as far away as the Sahara facilitate ice nuclei formation and ice-induced precipitation in the Sierra Nevada and show how dust and biological articles from places as distant as Africa and Asia can influence precipitation over the western United States. Dust and biological aerosols from the Sahara and Asia can act as ice nuclei for precipitation in California’s Sierra Nevada. Winter storms in California’s Sierra Nevada increase seasonal snowpack and provide critical water resources and hydropower for the state. Thus, the mechanisms influencing precipitation in this region have been the subject of research for decades. Previous studies suggest Asian dust enhances cloud ice and precipitation, whereas few studies consider biological aerosols as an important global source of ice nuclei (IN). Here, we show that dust and biological aerosols transported from as far as the Sahara were present in glaciated high-altitude clouds coincident with elevated IN concentrations and ice-induced precipitation. This study presents the first direct cloud and precipitation measurements showing that Saharan and Asian dust and biological aerosols probably serve as IN and play an important role in orographic precipitation processes over the western United States.

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...

An empirical parameterization of heterogeneous ice nucleation for multiple chemical species of aerosol

A novel, flexible framework is proposed for parameterizing the heterogeneous nucleation of ice within clouds. It has empirically derived dependencies on the chemistry and surface area of multiple species of ice nucleus (IN) aerosols. Effects from variability in mean size, spectral width, and mass loading of aerosols are represented via their influences on surface area. The parameterization is intended for application in largescale atmospheric and cloud models that can predict 1) the supersaturation of water vapor, which requires a representation of vertical velocity on the cloud scale, and 2) concentrations of a variety of insoluble aerosol species. Observational data constraining the parameterization are principally from coincident field studies of IN activity and insoluble aerosol in the troposphere. The continuous flow diffusion chamber (CFDC) was deployed. Aerosol species are grouped by the parameterization into three basic types: dust and metallic compounds, inorganic black carbon, and insoluble organic aerosols. Further field observations inform the partitioning of measured IN concentrations among these basic groups of aerosol. The scarcity of heterogeneous nucleation, observed at humidities well below water saturation for warm subzero temperatures, is represented. Conventional and inside-out contact nucleation by IN is treated with a constant shift of their freezing temperatures. The empirical parameterization is described and compared with available field and laboratory observations and other schemes. Alternative schemes differ by up to five orders of magnitude in their freezing fractions (30°C). New knowledge from future observational advances may be easily assimilated into the scheme’s framework. The essence of this versatile framework is the use of data concerning atmospheric IN sampled directly from the troposphere.

Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol

The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60–180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties.

The susceptibility of ice formation in upper tropospheric clouds to insoluble aerosol components

Ice may form by both homogeneous and heterogeneous freezing nucleation processes in clouds at temperatures below -35°C. Most investigations have focused on the former process. This paper presents results from adiabatic parcel model calculations that include the effects of both freezing processes in unactivated solution droplets. Uncertainties in predicting the homogeneous freezing rates are discussed and used to select solution drop composition and freezing characteristics that bracket those expected in the upper troposphere. The heterogeneous freezing rates of insoluble atmospheric aerosols are parameterized based on published freezing rates of carbonaceous particles. Process model simulations show that the potential variability in ice formation in cirrus clouds is much greater if heterogeneous freezing nucleation is considered in addition to homogeneous freezing. The impact of insoluble aerosols on ice formation is inferred to increase with insoluble particle size and with the fraction of soluble aerosols containing insoluble components. The maximum impact of heterogeneous nucleation is indicated for vertical motions less than 0.2 m s -1 and for insoluble components being associated with at least 10% of all soluble aerosols. The wide range of ice crystal concentrations observed in cirrus is most consistent with the occurrence of both heterogeneous and homogeneous ice formation processes. These conclusions are partially supported by existing observations of aerosols and cloud microphysical characteristics in upper tropospheric clouds but require new measurements for confirmation.

Single particle analyses of ice nucleating aerosols in the upper troposphere and lower stratosphere

A newly developed instrument was deployed on the NASA DC-8 airborne laboratory during the Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS, Spring 1996) to detect and collect heterogeneous ice nucleating particles (IN) in the upper troposphere and lower stratosphere. The elemental compositions of both ambient particles and IN were determined with single particle analysis using analytical electron microscopy. IN collected during flights on May 4 and 8 had enhanced number fractions of metallic, crustal, and carbonaceous particles, compared with the ambient aerosol population, and were relatively deficient in sulfur-containing particles. IN sampled within aircraft exhaust and contrails had higher number fractions of metallic particles, which includes those rich in Zn, Al, and Ti, than the IN sampled in air that was not immediately affected by aircraft exhaust.