An Introduction to Clouds provides a fundamental understanding of clouds, ranging from cloud microphysics to the large-scale impacts of clouds on climate. On the microscale, phase changes and ice nucleation are covered comprehensively, including aerosol particles and thermodynamics relevant for the formation of clouds and precipitation. At larger scales, cloud dynamics, mid-latitude storms and tropical cyclones are discussed leading to the role of clouds on the hydrological cycle and climate. Each chapter ends with problem sets and multiple choice questions that can be completed online, and important equations are highlighted in boxes for ease of reference. Combining mathematical formulations with qualitative explanations of underlying concepts, this accessible book requires relatively little previous knowledge, making it ideal for advanced undergraduate and graduate students in atmospheric science, environmental sciences and related disciplines.

Ice nucleation in the atmosphere influences cloud properties, altering precipitation and the radiative balance, ultimately regulating Earth’s climate. An accepted ice nucleation pathway, known as deposition nucleation, assumes a direct transition of water from the vapor to the ice phase, without an intermediate liquid phase. However, studies have shown that nucleation occurs through a liquid phase in porous particles with narrow cracks or surface imperfections where the condensation of liquid below water saturation can occur, questioning the validity of deposition nucleation. We show that deposition nucleation cannot explain the strongly enhanced ice nucleation efficiency of porous compared with nonporous particles at temperatures below −40 °C and the absence of ice nucleation below water saturation at −35 °C. Using classical nucleation theory (CNT) and molecular dynamics simulations (MDS), we show that a network of closely spaced pores is necessary to overcome the barrier for macroscopic ice-crystal growth from narrow cylindrical pores. In the absence of pores, CNT predicts that the nucleation barrier is insurmountable, consistent with the absence of ice formation in MDS. Our results confirm that pore condensation and freezing (PCF), i.e., a mechanism of ice formation that proceeds via liquid water condensation in pores, is a dominant pathway for atmospheric ice nucleation below water saturation. We conclude that the ice nucleation activity of particles in the cirrus regime is determined by the porosity and wettability of pores. PCF represents a mechanism by which porous particles like dust could impact cloud radiative forcing and, thus, the climate via ice cloud formation.

Ice nucleation by different types of soot particles is systematically investigated over the temperature range from 218 to 253 K relevant for both mixed-phase (MPCs) and cirrus clouds. Soot types were selected to represent a range of physicochemical properties associated with combustion particles. Their ice nucleation ability was determined as a function of particle size using relative humidity (RH) scans in the Horizontal Ice Nucleation Chamber (HINC). We complement our ice nucleation results by a suite of particle characterization measurements, including determination of particle surface area, fractal dimension, temperature-dependent mass loss (ML), water vapor sorption and inferred porosity measurements. Independent of particle size, all soot types reveal absence of ice nucleation below and at water saturation in the MPC regime (T > 235 K). In the cirrus regime (T ≤ 235 K), soot types show different freezing behavior depending on particle size and soot type, but the freezing is closely linked to the soot particle properties. Specifically, our results suggest that if soot aggregates contain mesopores (pore diameters of 2–50 nm) and have sufficiently low water–soot contact angles, they show ice nucleation activity and can contribute to ice formation in the cirrus regime at RH well below homogeneous freezing of solution droplets. We attribute the observed ice nucleation to a pore condensation and freezing (PCF) mechanism. Nevertheless, soot particles without cavities of the right size and/or too-high contact angles nucleate ice only at or well above the RH required for homogeneous freezing conditions of solution droplets. Thus, our results imply that soot particles able to nucleate ice via PCF could impact the microphysical properties of ice clouds.

Significance: Aerosol particles are ubiquitous in the atmosphere and play an important role in air quality and the climate system. These particles can contain mixtures of primary organic aerosol, secondary organic aerosol, and secondary inorganic aerosol. We show that such internally mixed particles can contain three liquid phases. We also demonstrate that the presence of three liquid phases impacts the time needed for the particles to reach equilibrium with the surrounding gas phase and likely impacts the ability of the particles to activate into cloud droplets. A framework is presented for predicting conditions needed for the formation of three liquid phases in the atmosphere. These results will lead to improved representations of aerosols in models for air quality and climate predictions.

Soot particles are generally considered to be poor ice nucleating particles. Involvement of soot in clouds and their release back into the atmosphere can form residual particles with altered cloud forming potential. The impact and extent of such different cloud processing scenarios on ice nucleation is, however, not well understood. In this work, we present the impact of cloud processing of soot aerosols on subsequent ice nucleation cycles at T≤233 K. Coupling of two continuous flow diffusion chambers allows the simulation of different cloud processing scenarios and investigation of subsequent ice nucleation activity of the processed particles. The processing scenarios presented here encompass contrail, cirrus, and mixed‐phase cloud processing, mimicking typical pathways that soot particles can be exposed to in the atmosphere. For all scenarios tested, the processed particles showed an enhanced ice active fraction for T<233 K. The relative humidity with respect to water for the ice nucleation onset was observed to be on average approximately 10% (relative humidity with respect to ice, RH_i≈16%) lower for the cloud‐processed particles compared to the unprocessed soot for which ice nucleation was observed close to or at homogeneous freezing conditions of solution droplets. We attribute the enhanced ice nucleation abilities of the cloud‐processed soot to a pore condensation and freezing mechanism and have identified key parameters governing these changes. Enhanced ice nucleation abilities of soot in cirrus clouds can have significant impacts, given the importance of the atmospheric ice phase for precipitation formation and global climate.