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Wojciech W. Grabowski

Abstract

Influence of pollution on dynamics of deep convection continues to be a controversial topic. Arguably, only carefully designed numerical simulations can clearly separate the impact of aerosols from the effects of meteorological factors that affect moist convection. This paper argues that such a separation is virtually impossible using observations because of the insufficient accuracy of atmospheric measurements and the fundamental nature of the interaction between deep convection and its environment. To support this conjecture, results from numerical simulations are presented that apply modeling methodology previously developed by the author. The simulations consider small modifications, difficult to detect in observations, of the initial sounding, surface fluxes, and large-scale forcing tendencies. All these represent variations of meteorological conditions that affect deep convective dynamics independently of aerosols. The setup follows the case of daytime convective development over land based on observations during the Large-Scale Biosphere–Atmosphere (LBA) field project in Amazonia. The simulated observable macroscopic changes of convection, such as the surface precipitation and upper-tropospheric cloudiness, are similar to or larger than those resulting from changes of cloud condensation nuclei from pristine to polluted conditions studied previously using the same modeling case. Observations from Phase III of the Global Atmospheric Research Program Atlantic Tropical Experiment (GATE) are also used to support the argument concerning the impact of the large-scale forcing. The simulations suggest that the aerosol impacts on dynamics of deep convection cannot be isolated from meteorological effects, at least for the daytime development of unorganized deep convection considered in this study.

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Christina S. McCluskey, Thomas C. J. Hill, Camille M. Sultana, Olga Laskina, Jonathan Trueblood, Mitchell V. Santander, Charlotte M. Beall, Jennifer M. Michaud, Sonia M. Kreidenweis, Kimberly A. Prather, Vicki Grassian, and Paul J. DeMott

Abstract

The abundance of atmospheric ice nucleating particles (INPs) is a source of uncertainty for numerical representation of ice-phase transitions in mixed-phase clouds. While sea spray aerosol (SSA) exhibits less ice nucleating (IN) ability than terrestrial aerosol, marine INP emissions are linked to oceanic biological activity and are potentially an important source of INPs over remote oceans. Inadequate knowledge of marine INP identity limits the ability to parameterize this complex INP source. A previous manuscript described abundances of marine INPs in relation to several aerosol composition and ocean biology observations during two laboratory mesocosm experiments. In this study, the abundances and chemical and physical properties of INPs found during the same mesocosm experiments were directly probed in SSA, seawater, and surface microlayer samples. Two unique marine INP populations were found: 1) dissolved organic carbon INPs are suggested to be composed of IN-active molecules, and 2) particulate organic carbon INPs are attributed as intact cells or IN-active microbe fragments. Both marine INP types are likely to be emitted into SSA following decay of phytoplankton biomass when 1) the surface microlayer is significantly enriched with exudates and cellular detritus and SSA particles are preferentially coated with IN-active molecules or 2) diatom fragments and bacteria are relatively abundant in seawater and therefore more likely transferred into SSA. These findings inform future efforts for incorporating marine INP emissions into numerical models and motivate future studies to quantify specific marine molecules and isolate phytoplankton, bacteria, and other species that contribute to these marine INP types.

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Luke B. Hande, C. Hoose, and C. Barthlott

Abstract

A parameterization for contact freezing is presented that combines theoretical expressions for determining the collision efficiency with experimentally determined freezing efficiency results. The parameterization has dependencies on aerosol and cloud droplet physical properties, including electric charges, as well as ambient temperature and humidity. The highest freezing rate is obtained at large aerosol and large cloud droplet sizes, and at cold temperatures and low relative humidities, with typical dust aerosol and droplet properties. The number concentration of ice nucleating particles (INPs) in the contact freezing mode are generally lower than those in the immersion freezing or deposition nucleation mode; however, under certain conditions contact INP concentrations can exceed those of the other modes. The new parameterization is used in a high-resolution, semi-idealized simulation of a deep convective cloud, and a number of sensitivity studies are performed. Results indicate the greatest sensitivity is to the best-fit function to laboratory data. The simulations show that droplet properties and ambient relative humidity contribute significantly to contact freezing.

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Romy Ullrich, Corinna Hoose, Ottmar Möhler, Monika Niemand, Robert Wagner, Kristina Höhler, Naruki Hiranuma, Harald Saathoff, and Thomas Leisner

Abstract

Based on results of 11 yr of heterogeneous ice nucleation experiments at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber in Karlsruhe, Germany, a new empirical parameterization framework for heterogeneous ice nucleation was developed. The framework currently includes desert dust and soot aerosol and quantifies the ice nucleation efficiency in terms of the ice nucleation active surface site (INAS) approach.

The immersion freezing INAS densities n S of all desert dust experiments follow an exponential fit as a function of temperature, well in agreement with an earlier analysis of AIDA experiments. The deposition nucleation n S isolines for desert dust follow u-shaped curves in the ice saturation ratio–temperature (S iT) diagram at temperatures below about 240 K. The negative slope of these isolines toward lower temperatures may be explained by classical nucleation theory (CNT), whereas the behavior toward higher temperatures may be caused by a pore condensation and freezing mechanism. The deposition nucleation measured for soot at temperatures below about 240 K also follows u-shaped isolines with a shift toward higher S i for soot with higher organic carbon content. For immersion freezing of soot aerosol, only upper limits for n S were determined and used to rescale an existing parameterization line.

The new parameterization framework is compared to a CNT-based parameterization and an empirical framework as used in models. The comparison shows large differences in shape and magnitude of the n S isolines especially for deposition nucleation. For the application in models, implementation of this new framework is simple compared to that of other expressions.

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Christina S. McCluskey, Thomas C. J. Hill, Francesca Malfatti, Camille M. Sultana, Christopher Lee, Mitchell V. Santander, Charlotte M. Beall, Kathryn A. Moore, Gavin C. Cornwell, Douglas B. Collins, Kimberly A. Prather, Thilina Jayarathne, Elizabeth A. Stone, Farooq Azam, Sonia M. Kreidenweis, and Paul J. DeMott

Abstract

Emission rates and properties of ice nucleating particles (INPs) are required for proper representation of aerosol–cloud interactions in atmospheric models. Few investigations have quantified marine INP emissions, a potentially important INP source for remote oceanic regions. Previous studies have suggested INPs in sea spray aerosol (SSA) are linked to oceanic biological activity. This proposed link was explored in this study by measuring INP emissions from nascent SSA during phytoplankton blooms during two mesocosm experiments. In a Marine Aerosol Reference Tank (MART) experiment, a phytoplankton bloom was produced with chlorophyll-a (Chl a) concentrations reaching 39 μg L−1, while Chl a concentrations more representative of natural ocean conditions were obtained during the Investigation into Marine Particle Chemistry and Transfer Science (IMPACTS; peak Chl a of 5 μg L−1) campaign, conducted in the University of California, San Diego, wave flume. Dynamic trends in INP emissions occurred for INPs active at temperatures > −30°C. Increases in INPs active between −25° and −15°C lagged the peak in Chl a in both studies, suggesting a consistent population of INPs associated with the collapse of phytoplankton blooms. Trends in INP emissions were also compared to aerosol composition, abundances of microbes, and enzyme activity. In general, increases in INP concentrations corresponded to increases in organic species in SSA and the emissions of heterotrophic bacteria, suggesting that both microbes and biomolecules contribute to marine INP populations. INP trends were not directly correlated with a single biological marker in either study. Direct measurements of INP chemistry are needed to accurately identify particles types contributing to marine INP populations.

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Stacey Kawecki, Geoffrey M. Henebry, and Allison L. Steiner

Abstract

This study examines the effects of urban aerosols on a mesoscale convective system (MCS) in the central Great Plains with the Weather Research and Forecasting Model coupled with chemistry (WRF-Chem). Urban emissions from Kansas City, Missouri, were scaled by factors of 0.5, 1.0, and 2.0 to investigate the impact of urban aerosol load on MCS propagation and strength. The first half of the storm development is characterized by a stationary front to the north of Kansas City (phase I; 1800 UTC 26 May–0600 UTC 27 May), which develops into a squall line south of the urban area (phase II; 0600–1800 UTC 27 May). During phase I, doubling urban emissions shifts the precipitation accumulation, with enhancement downwind of the storm propagation and suppression upwind. During phase II, a squall line develops in the baseline and doubled emissions scenarios but not when emissions are halved. These changes in MCS propagation and strength are a function of cold pool strength, which is determined by microphysical processes and directly influenced by aerosol load. Overall, changes in urban emissions drive changes in cloud microphysics, which trigger large-scale changes in storm morphology and precipitation patterns. These results show that urban emissions can play an important role in mesoscale weather systems.

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Andrew R. Jongeward, Zhanqing Li, Hao He, and Xiaoxiong Xiong

Abstract

Aerosols contribute to Earth’s radiative budget both directly and indirectly, and large uncertainties remain in quantifying aerosol effects on climate. Variability in aerosol distribution and properties, as might result from changing emissions and transport processes, must be characterized. In this study, variations in aerosol loading across the eastern seaboard of the United States and the North Atlantic Ocean during 2002 to 2012 are analyzed to examine the impacts of anthropogenic emission control measures using monthly mean data from MODIS, AERONET, and IMPROVE observations and Goddard Chemistry Aerosol Radiation and Transport (GOCART) model simulation. MODIS observes a statistically significant negative trend in aerosol optical depth (AOD) over the midlatitudes (−0.030 decade−1). Correlation analyses with surface AOD from AERONET sites in the upwind region combined with trend analysis from GOCART component AOD confirm that the observed decrease in the midlatitudes is chiefly associated with anthropogenic aerosols that exhibit significant negative trends from the eastern U.S. coast extending over the western North Atlantic. Additional analysis of IMPROVE surface PM2.5 observations demonstrates statistically significant negative trends in the anthropogenic components with decreasing mass concentrations over the eastern United States. Finally, a seasonal analysis of observational datasets is performed. The negative trend seen by MODIS is strongest during spring (MAM) and summer (JJA) months. This is supported by AERONET seasonal trends and is identified from IMPROVE seasonal trends as resulting from ammonium sulfate decreases during these seasons.

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Jianjun Liu, Zhanqing Li, and Maureen Cribb

Abstract

This study investigates the response of marine boundary layer (MBL) cloud properties to aerosol loading by accounting for the contributions of large-scale dynamic and thermodynamic conditions and quantifies the first indirect effect (FIE). It makes use of 19-month measurements of aerosols, clouds, and meteorology acquired during the Atmospheric Radiation Measurement Mobile Facility field campaign over the Azores. Cloud droplet number concentrations and cloud optical depth (COD) significantly increased with increasing aerosol number concentration . Cloud droplet effective radius (DER) significantly decreased with increasing . The correlations between cloud microphysical properties [, liquid water path (LWP), and DER] and were stronger under more stable conditions. The correlations between , LWP, DER, and were stronger under ascending-motion conditions, while the correlation between COD and was stronger under descending-motion conditions. The magnitude and corresponding uncertainty of the FIE ranged from 0.060 ± 0.022 to 0.101 ± 0.006 depending on the different LWP values. Under more stable conditions, cloud-base heights were generally lower than those under less stable conditions. This enabled a more effective interaction with aerosols, resulting in a larger value for the FIE. However, the dependence of the response of cloud properties to aerosol perturbations on stability varied according to whether ground- or satellite-based DER retrievals were used. The magnitude of the FIE had a larger variation with changing LWP under ascending-motion conditions and tended to be higher under ascending-motion conditions for clouds with low LWP and under descending-motion conditions for clouds with high LWP. A contrasting dependence of FIE on atmospheric stability estimated from the surface and satellite cloud properties retrievals reported in this study underscores the importance of assessing all-level properties of clouds in aerosol–cloud interaction studies.

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Jiwen Fan, Yuan Wang, Daniel Rosenfeld, and Xiaohong Liu

Abstract

Over the past decade, the number of studies that investigate aerosol–cloud interactions has increased considerably. Although tremendous progress has been made to improve the understanding of basic physical mechanisms of aerosol–cloud interactions and reduce their uncertainties in climate forcing, there is still poor understanding of 1) some of the mechanisms that interact with each other over multiple spatial and temporal scales, 2) the feedbacks between microphysical and dynamical processes and between local-scale processes and large-scale circulations, and 3) the significance of cloud–aerosol interactions on weather systems as well as regional and global climate. This review focuses on recent theoretical studies and important mechanisms on aerosol–cloud interactions and discusses the significances of aerosol impacts on radiative forcing and precipitation extremes associated with different cloud systems. The authors summarize the main obstacles preventing the science from making a leap—for example, the lack of concurrent profile measurements of cloud dynamics, microphysics, and aerosols over a wide region on the observation side and the large variability of cloud microphysics parameterizations resulting in a large spread of modeling results on the modeling side. Therefore, large efforts are needed to escalate understanding. Future directions should focus on obtaining concurrent measurements of aerosol properties and cloud microphysical and dynamic properties over a range of temporal and spatial scales collected over typical climate regimes and closure studies, as well as improving understanding and parameterizations of cloud microphysics such as ice nucleation, mixed-phase properties, and hydrometeor size and fall speed.

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Tianmeng Chen, Jianping Guo, Zhanqing Li, Chuanfeng Zhao, Huan Liu, Maureen Cribb, Fu Wang, and Jing He

Abstract

Many efforts have been taken to investigate aerosol–cloud interactions from space, but only a few studies have examined the response of vertical cloud structure to aerosol perturbations. Three-dimensional cloud climatologies of eight different cloud types identified from the CloudSat level-2 cloud product during the warm season (May–September) in 2008–10 over eastern China were first generated and analyzed. Using visibility as a proxy for cloud condensation nuclei, in combination with satellite-observed radar reflectivity, normalized contoured frequency by altitude diagrams of the differences in cloud radar reflectivity Z profiles under polluted and clean conditions were constructed. For shallow cumulus clouds (shallow Cu) Z tends to be inhibited, and it is enhanced in the upper layers for deep cumulus (deep Cu), nimbostratus (Ns), and deep convective clouds (DCC) under polluted conditions. Overall, analyses of the modified center of gravity (MCOG) and cloud-top height (CTH) also point to a similar aerosol effect, except for the nonsignificant changes in MCOGs and CTHs in deep Cu. The impacts of environmental factors such as lower-tropospheric stability and vertical velocity are also discussed for these types of clouds. Although consistent aerosol-induced elevations in MCOGs and CTHs for Ns and DCC clouds are observed, the effect of meteorology cannot be completely ruled out, which merits further analysis.

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