Will Cantrell

Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze

Every year, from December to April, anthropogenic haze spreads over most of the North Indian Ocean, and South and Southeast Asia. The Indian Ocean Experiment (INDOEX) documented this Indo-Asian haze at scales ranging from individual particles to its contribution to the regional climate forcing. This study integrates the multiplatform observations (satellites, aircraft, ships, surface stations, and balloons) with one- and four-dimensional models to derive the regional aerosol forcing resulting from the direct, the semidirect and the two indirect effects. The haze particles consisted of several inorganic and carbonaceous species, including absorbing black carbon clusters, fly ash, and mineral dust. The most striking result was the large loading of aerosols over most of the South Asian region and the North Indian Ocean. The January to March 1999 visible optical depths were about 0.5 over most of the continent and reached values as large as 0.2 over the equatorial Indian ocean due to long-range transport. The aerosol layer extended as high as 3 km. Black carbon contributed about 14% to the fine particle mass and 11% to the visible optical depth. The single-scattering albedo estimated by several independent methods was consistently around 0.9 both inland and over the open ocean. Anthropogenic sources contributed as much as 80% (±10%) to the aerosol loading and the optical depth. The in situ data, which clearly support the existence of the first indirect effect (increased aerosol concentration producing more cloud drops with smaller effective radii), are used to develop a composite indirect effect scheme. The Indo-Asian aerosols impact the radiative forcing through a complex set of heating (positive forcing) and cooling (negative forcing) processes. Clouds and black carbon emerge as the major players. The dominant factor, however, is the large negative forcing (-20±4 W m^(−2)) at the surface and the comparably large atmospheric heating. Regionally, the absorbing haze decreased the surface solar radiation by an amount comparable to 50% of the total ocean heat flux and nearly doubled the lower tropospheric solar heating. We demonstrate with a general circulation model how this additional heating significantly perturbs the tropical rainfall patterns and the hydrological cycle with implications to global climate.

Production of ice in tropospheric clouds: A review

Ice in the troposphere affects a variety of processes, including the formation of precipitation, and cloud lifetime, albedo, dynamics, and electrification. A lack of understanding of the ways in which ice is created and multiplied hampers progress in understanding all of these processes. We survey the state of knowledge, starting with homogeneous nucleation, where current formulations for freezing from both pure water and solutions have considerable predictive power. However, debate still exists on the underlying mechanisms of nucleation. Using the concepts and framework that homogeneous nucleation provides, heterogeneous nucleation, where neither a commonly agreed upon theory nor even standard measurement technique exists, is considered. Investigators have established the ice-nucleating characteristics of broad classes of substances, such as mineral dust and soot, which are important ice nuclei in t he atmosphere, but a coherent theory of why these substances act as they do has yet to emerge. All ice in ...

Intercomparison Study of the Size-Dependent Counting Efficiency of 26 Condensation Particle Counters

ABSTRACT Particle detection efficiency curves for 26 condensation particle counters were determined during a calibration workshop in preparation for the Aerosol Characterization Experiment 1 (ACE1). Three different types of commercially available particle counters, the ultrafine condensation particle counter (TSI-3025) and the condensation particle counters (TSI-3010 and TSI-3760 or TS1-7610) were investigated at default temperature and flow settings as well as for other flow rates and temperature differences between the saturator and the condenser. Furthermore, the pulse-height-analysis ultrafine condensation particle counter and a TSI-3010 modified to achieve a higher temperature difference were calibrated. In this study, the large number of particle counters investigated provided the opportunity to obtain a more statistically significant picture of the performance of different particle counters for different operating conditions.

Closure between aerosol particles and cloud condensation nuclei at Kaashidhoo Climate Observatory

Predicting the cloud condensation nuclei (CCN) supersaturation spectrum from aerosol properties is a fairly straightforward matter, as long as those properties are simple. During the Indian Ocean Experiment we measured CCN spectra, size-resolved aerosol chemical composition, and aerosol number distributions and attempted to reconcile them using a modified form of Kohler theory. We obtained general agreement between our measured and modeled CCN spectra. However, the agreement was not as good during a time period when organic carbon comprised a quarter of the total mass of the aerosol in the submicron size range. The modeled concentrations overpredict those actually measured during that time period. This suggests that some component, presumably organic material, can inhibit the uptake of water by the electrolytic fraction of the mass.

Cloud condensation nuclei spectra derived from size distributions and hygroscopic properties of the aerosol in coastal south-west Portugal during ACE-2

In this work we propose and test a method to calculate cloud condensation nuclei (CCN) spectra basedon aerosol number size distributions and hygroscopic growth factors. Sensitivity studies show thatthis method can be used in a wide variety of conditions except when the aerosol consist mainly oforganic compounds. One crucial step in the calculations, estimating soluble ions in an aerosol particlebased on hygroscopic growth factors, is tested in an internal hygroscopic consistency study. The resultsshow that during the second Aerosol Characterization Experiment (ACE-2) the number concentrationof inorganic ions analyzed in impactor samples could be reproduced from measured growth factorswithin the measurement uncertainties at the measurement site in Sagres, Portugal. CCN spectra were calculated based on data from the ACE-2 field experiment at the Sagres site.The calculations overestimate measured CCN spectra on average by approximately 30%, which iscomparable to the uncertainties in measurements and calculations at supersaturations below 0.5%. Thecalculated CCN spectra were averaged over time periods when Sagres received clean air masses and airmasses influenced by aged and recent pollution. Pollution outbreaks enhance the CCN concentrationsat supersaturations near 0.2% by a factor of 3 (aged pollution) to 5 (recent pollution) compared to theclean marine background concentrations. In polluted air masses, the shape of the CCN spectra changes.The clean spectra can be approximated by a power function, whereas the polluted spectra are betterapproximated by an error function.

Relationships between cloud condensation nuclei spectra and aerosol particles on a south‐north transect of the Indian Ocean

Do anthropogenic emissions affect cloud microphysical properties? One parameter needed to answer the preceding question is a link between the aerosol number distribution and the cloud condensation nuclei (CCN) supersaturation spectrum for polluted and unpolluted air masses. On a south-north cruise in the Indian Ocean in March of 1998, we found that measured CCN spectra and CCN spectra calculated from the ambient aerosol number distributions disagreed by as much as a factor of 2. The aerosol soluble fraction inferred from the relationship between measured and calculated CCN spectra ranged from 0.2 to 0.05 and exhibited a broad minimum at the Intertropical Convergence Zone (ITCZ). The concentration of CCN, non-sea-salt SO42 ,N H 4 , black carbon, and organic carbon increased by an order of magnitude as we passed through the ITCZ.

A new instrument for measuring cloud condensation nuclei: Cloud condensation nucleus “remover”

This communique describes a new and novel instrument for measuring concentrations of natural cloud condensation nuclei (CCN) from the free atmosphere. It simultaneously provides the size spectrum of nucleated particles, a useful parameter for gaining insight into the composition of the CCN. The supersaturation spectrum N(S), where N is the number concentration of droplets nucleated at supersaturation S, is readily obtained. This parameter is one of the keys to evaluating aerosol influence on cloud microphysics and on the possible modulations of cloud albedo. Laboratory evaluations show that the instrument has good measurement accuracy and precision, even at low CCN concentrations found in the clean troposphere. The instrument is rugged and reliable.

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

Significance Atmospheric aerosol concentration is linked to cloud brightness and lifetime through the modulation of precipitation. Generally speaking, larger cloud droplets and wider-droplet size distributions form precipitation more efficiently. We create steady-state clouds in the laboratory through a balance of constant aerosol injection and cloud-droplet removal due to settling. As aerosol concentration is decreased, the cloud-droplet mean diameter increases, as expected, but also the width of the size distribution increases sharply. Theory, simulations, and measurements point to greater supersaturation variability as the cause of this broadening in what can be considered a low aerosol/slow microphysics limit. The influence of aerosol concentration on the cloud-droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud-droplet growth and fallout. As aerosol concentration is increased, the cloud-droplet mean diameter decreases, as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τcτt) for low aerosol concentration; here, τc is the phase-relaxation time and τt is the turbulence-correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τs−1=τc−1+τt−1, and the measurements are in excellent agreement with this finding. The result underscores the importance of droplet size dispersion for aerosol indirect effects: increasing aerosol concentration changes the albedo and suppresses precipitation formation not only through reduction of the mean droplet diameter but also by narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol/slow microphysics limit are likely of leading importance for precipitation formation.

Entropic Aspects of Supercooled Droplet Freezing

The freezing of supercooled water droplets in the atmosphere, with an emphasis on the entropic aspects of the problem, is examined. Supercooled water is a metastable state and, therefore, the associated phase transition must be irreversible. Temperature-dependent heat capacities of supercooled water and ice are used to calculate the entropy difference. That difference is then used to establish a lower bound on the amount of latent heat that can be liberated by the freezing droplets. The calculation is compared with tabulated values of the latent heat of fusion with surprising results. Based on a novel physical picture of the freezing process, the authors suggest a simple estimate for the effective latent heat that is suitable for heat budget calculations of glaciating clouds. In addition, the authors arrive at a quadratic dependence on supercooling, (T ) 2 , for the irreversible contribution to heat exchange during the freezing process. The proportionality factor is estimated as 0.3 J mol 1 K 2 .

Nucleated deliquescence of salt

We have studied deliquescence on the (001) face of single crystals of NaCl and find that it is a nucleated phenomenon. The phase transition occurs only after the relative humidity exceeds that found over the saturated solution by at least 5%. The contrast between our observations and previous measurements using salt powders or crystallites leads us to the conclusion that deliquescence is controlled by the differences in energy required to solvate ions from the smooth (001) face and from the defect-rich surfaces of particulate samples.