This study focuses on the importance of solute dissolution kinetics for cloud droplet formation. To comprehensively account for the kinetics, a numerical model of the process was developed. Simulations of cloud droplet growth were performed for solute diffusivity, droplet growth rates, dry particle and droplet diameters relevant for ambient conditions. Simulations suggest that high ambient supersaturations and a decrease in solute diffusivity are major contributors to significant decreases in effective solute surface concentrations. The numerical simulations were incorporated into Khler theory to assess the impact of dissolution kinetics on the droplet equilibrium vapor pressure. For CCN composed of partially soluble material, a significant increase was found in the equilibrium supersaturation of CCN.

The current dissertation is motivated by the need for an improved understanding of aerosol water interactions both in subsaturated and supersaturated atmospheric conditions with a strong emphasis on air pollution and climate change modeling. A cloud droplet formation parameterization was developed to i) predict droplet formation from a lognormal representation of aerosol size distribution and composition, and, ii) include a size-dependant mass transfer coefficient for the growth of water droplets which explicitly accounts for the impact of organics on droplet growth kinetics. The parameterization unravels most of the physics of droplet formation and is in remarkable agreement with detailed numerical parcel model simulations, even for low values of the accommodation coefficient. The parameterization offers a much needed rigorous and computationally inexpensive framework for directly linking complex chemical effects on aerosol activation in global climate models. The new aerosol activation parameterization was also tested against observations from highly polluted clouds (within the vicinity of power plant plumes). Remarkable closure was achieved (much less than the 20% measurement uncertainty). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America. Aerosol water interactions in ambient relative humidities less than 100% were studied using a thermodynamic equilibrium model for inorganic aerosol and a three dimensional air quality model. We developed a new thermodynamic equilibrium model, ISORROPIA-II, which predicts the partitioning of semi-volatiles and the phase state of K+/Ca2+/Mg2+/NH4+/Na+/SO42-/NO3-/Cl-/H2O aerosols. A comprehensive evaluation of its performance was conducted against the thermodynamic module SCAPE2 over a wide range of atmospherically relevant conditions. Based on its computational rigor and performance, ISORROPIA-II appears to be a highly attractive alternative for use in large scale air quality and atmospheric transport models. The new equilibrium model was also used to thermodynamically characterize aerosols measured at a highly polluted area. In the ammonia-rich environment of Mexico City, nitrate and chloride primarily partition in the aerosol phase with a 20-min equilibrium timescale; PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. When RH is below 50%, predictions improve substantially if the aerosol follows a deliquescent behavior. The impact of including crustal species (Ca2+, K+, M2+) in equilibrium calculations within a three dimensional air quality model was also studied. A significant change in aerosol water (-19.8%) and ammonium (-27.5%) concentrations was predicted when crustals are explicitly included in the calculations even though they contributed, on average, only a few percent of the total PM2.5 mass, highlighting the need for comprehensive thermodynamic calculations in the presence of dust.

Trace gases and aerosols, or suspended liquid and solid material in the atmosphere, have significant climatological and societal impacts; consequently, accurate representation of their contribution to atmospheric composition is vital to predicting climate change and informing policy actions. Sensitivity analysis allows scientists and environmental decision makers alike to ascertain the role a specific component of the very complex system that is the atmosphere of the Earth. Anthropogenic and natural emissions of gases and aerosol are transported by winds and interact with sunlight, allowing significant transformation before these species reach the end of their atmospheric life on land or in water. The adjoint-based sensitivity method assesses the relative importance of each emissions source to selected results of interest, including aerosol and cloud droplet concentration. In this work, the adjoint of a comprehensive inorganic aerosol thermodynamic equilibrium model was produced to improve the representativeness of regional and global chemical transport modeling. Furthermore, a global chemical transport model adjoint equipped with the adjoint of a cloud droplet activation parameterization was used to explore the footprint of emissions contributing to current and potential future cloud droplet concentrations, which impact the radiative balance of the earth. In future work, these sensitivity relationships can be exploited in optimization frameworks for assimilation of observations of the system, such as satellite-based or in situ measurements of aerosol or precursor trace gas concentrations.

Ship-based cloud remote sensing observations made onboard R/V Meteor during the ElUcidating the RolE of Cloud-Circulation Coupling in ClimAte, EUREC4A, campaign are presented and used to calculate cloud droplet number concentrations. The calculation is based on cloud liquid water path LWP and droplet effective radius reff retrieved from spectral measurements of transmitted solar radiance. It is shown that measurement uncertainties and retrieval assumptions impact the accuracy of the results. A case study indicates that the retrieval of LWP and reff is most affected by 3D-radiative effects in case of shallow cumulus and drizzle, which violates the adiabatic theory and plan-parallel geometry on which the radiative transfer simulations of the retrieval are based. Depending on the cloud thickness, the retrieval of reff might suffers from ambiguity. These retrieval uncertainties and their implications on the estimated cloud droplet number concentration are investigated by a sensitivity study. The analysis showed that most of the uncertainty is introduced by reff, whereas LWP contributes significantly to the uncertainty only for thin clouds. Therefore, it is concluded that only selected cloud cases, which do not violate the retrieval assumption, such as stratiform cloud layers, are suited to apply the retrieval approach in further studies. / Fernerkundungsmessungen von Wolken auf dem Forschungsschiff R/V Meteor während der ElUcidating the RolE of Cloud-Circulation Coupling in ClimAte, EUREC4A, Kampagnewerden vorgestellt und zur Berechnung der Tröpfchenanzahlkonzentration verwendet. Die Berechnung basiert auf Messungen des Flüssigwasserpfads LWP und dem effektiven Tröpfchenradius reff, welche aus spektralen Messungen der transmittierten solaren Strahldichte abgeleitet wurden. Es wird gezeigt, dass Messunsicherheiten und Annahmen bei der Ableitung der Wolkeneigenschaften die Genauigkeit der Ergebnisse beeinflussen. Eine Fallstudie zeigt, dass die Ableitung von LWP und reff am stärksten durch 3-dimensionale Strahlungseffekte von flachen Cumuli und Nieselregen beeinflusst wird. Beides wiederspricht den Idealisierungen von adiabatischen Wolken und einer planparallelen Geometrie, auf denen die Strahlungstransfersimulationen des Verfahrens beruhen. Abhängig von der Wolkendicke kann die Ableitung von reff zusätzlich durch Mehrdeutigkeiten beeinflusst sein.

In this work spectral airborne measurements of upward irradiance and a novel remote sensing technique for the cloud droplet number concentration are used to evaluate the representation of clouds in current operational weather prediction models.

Despite large efforts and decades of research, the scientific understanding of how aerosols impact climate by modulating microphysical cloud properties is still low and associated radiative forcing estimates (RFaci ) vary with a wide spread. But since anthropogenically forced aerosol-cloud interactions (ACI) are considered to oppose parts of the global warming, it is crucial to know their contribution to the total radiative forcing in order to improve climate predictions. To obtain a better understanding and quantification of ACI and the associated radiative effect it as been suggested to use concurrent measurements and observationally constrained model simulations. In this dissertation a joint satellite-reanalysis approach is introduced, bridging the gap between climate models and satellite observations in a bottom-up approach. This methodology involves an observationally constrained aerosol model, refined and concurrent multi-component satellite retrievals, a state-of-the-art aerosol activation parameteriza- tion as well as radiative transfer model. This methodology is shown here to be useful for a quantitative as well as qualitative analysis of ACI and for estimating RFaci . As a result, a 10-year long climatology of cloud condensation nuclei (CCN) (particles from which cloud droplets form) is produced and evaluated. It is the first of its kind providing 3-D CCN concentrations of global coverage for various supersaturations and aerosol species and offering the opportunity to be used for evaluation in models and ACI studies. Further, the distribution and variability of the resulting cloud droplet numbers and their susceptibility to changes in aerosols is explored and compared to previous estimates. In this context, an analysis by cloud regime has been proven useful. Last but not least, the computation and analysis of the present-day regime-based RFaci represents the final conclusion of the bottom-up methodology. Overall, this thesis provides a comprehensive assessment of interactions and uncertainties related to aerosols, clouds and radiation in regimes of liquid water clouds and helps to improve the level of scientific understanding.

Important aspects of the adjustments to aerosol-cloud interactions can be examined using the relationship between cloud droplet number concentration (Nd) and liquid water path (LWP). Specifically, this relation can constrain the role of aerosols in leading to thicker or thinner clouds in response to adjustment mechanisms. This study investigates the satellite retrieved relationship between Nd and LWP for a selected case of mid-latitude continental clouds using high-resolution Large-eddy simulations (LES) over a large domain in weather prediction mode. Since the satellite retrieval uses the adiabatic assumption to derive the Nd, we have also considered adiabatic Nd (NAd) from the LES model for comparison. The joint histogram analysis shows that the NAd-LWP relationship in the LES model and the satellite is in approximate agreement. In both cases, the peak conditional probability (CP) is confined to lower NAd and LWP; the corresponding mean LWP (LWP) shows a weak relation with NAd. The CP shows a larger spread at higher NAd (>50 cm–3), and the LWP increases non-monotonically with increasing NAd in both cases. Nevertheless, both lack the negative NAd-LWP relationship at higher NAd, the entrainment effect on cloud droplets. In contrast, the model simulated Nd-LWP clearly illustrates a much more nonlinear (an increase in LWP with increasing Nd and a decrease in LWP at higher Nd) relationship, which clearly depicts the cloud lifetime and the entrainment effect. Additionally, our analysis demonstrates a regime dependency (marine and continental) in the NAd-LWP relation from the satellite retrievals. Comparing local vs large-scale statistics from satellite data shows that continental clouds exhibit only a weak nonlinear NAd-LWP relationship. Hence a regime-based Nd-LWP analysis is even more relevant when it comes to warm continental clouds and their comparison to satellite retrievals.

<p>A study of air mass origin’s effect on marine stratus and stratocumulus clouds has been performed on clouds north of Scandinavia between 2000 and 2004. The aerosol number size distribution of the air masses has been obtained from measurements in northern Finland. A trajectory model has been used to calculate trajectories to and from the measurement stations. The back trajectories were calculated using the measurement site as receptor to make sure the air masses had the right origin, and forward trajectories were calculated from receptor stations to assure adequate flow conditions. Satellite data of microphysical parameters of clouds from the Moderate Resolution Imaging Spectrometer (MODIS) has been downloaded where the trajectories indicated that clouds could be studied, and where the satellite images displayed low-level clouds. The 25 % days with the highest number of aerosol with a diameter over 80 nm (N₈₀) and the 35% with the lowest N₈₀ have been used to represent polluted and clean conditions respectively. After screening trajectories and satellite imagery, 22 cases of clouds with northerly trajectories that had low N₈₀ values (i.e. clean) and 25 southerly cases with high N₈₀ values (i.e. polluted) where identified for further analysis.</p><p>   The average cloud optical thickness (τ) for all polluted pixels was more than twice that of the clean pixels. This can most likely be related to the differences in aerosol concentrations in accordance with the indirect effect, yet some difference in τ caused by different meteorological situations cannot be ruled out. The mean cloud droplet effective radius (a_ef) was for the polluted pixels 11.2 µm and for the clean pixels 15.5 µm, which results in a difference of 4.3 µm and clearly demonstrates the effect that increased aerosol numbers has on clouds. A non-linear relationship between a_ef and N₈₀ has been obtained which indicates that changes in lower values of aerosol numbers affect a_ef more than changes in larger aerosol loads. The results from this study also indicate that there is a larger difference in the microphysical cloud parameters between the polluted and clean cases in spring and autumn than in summer.</p>

A study of air mass origin’s effect on marine stratus and stratocumulus clouds has been performed on clouds north of Scandinavia between 2000 and 2004. The aerosol number size distribution of the air masses has been obtained from measurements in northern Finland. A trajectory model has been used to calculate trajectories to and from the measurement stations. The back trajectories were calculated using the measurement site as receptor to make sure the air masses had the right origin, and forward trajectories were calculated from receptor stations to assure adequate flow conditions. Satellite data of microphysical parameters of clouds from the Moderate Resolution Imaging Spectrometer (MODIS) has been downloaded where the trajectories indicated that clouds could be studied, and where the satellite images displayed low-level clouds. The 25 % days with the highest number of aerosol with a diameter over 80 nm (N80) and the 35% with the lowest N80 have been used to represent polluted and clean conditions respectively. After screening trajectories and satellite imagery, 22 cases of clouds with northerly trajectories that had low N80 values (i.e. clean) and 25 southerly cases with high N80 values (i.e. polluted) where identified for further analysis.    The average cloud optical thickness (τ) for all polluted pixels was more than twice that of the clean pixels. This can most likely be related to the differences in aerosol concentrations in accordance with the indirect effect, yet some difference in τ caused by different meteorological situations cannot be ruled out. The mean cloud droplet effective radius (aef) was for the polluted pixels 11.2 µm and for the clean pixels 15.5 µm, which results in a difference of 4.3 µm and clearly demonstrates the effect that increased aerosol numbers has on clouds. A non-linear relationship between aef and N80 has been obtained which indicates that changes in lower values of aerosol numbers affect aef more than changes in larger aerosol loads. The results from this study also indicate that there is a larger difference in the microphysical cloud parameters between the polluted and clean cases in spring and autumn than in summer.

科学研究費補助金 研究種目:一般研究(C) 課題番号:63540311 研究代表者:石坂 隆 研究期間:1988-1989年度