Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron‐sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid‐catalyzed multiphase chemistry of isoprene epoxydiols, particle‐phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process‐related interactions, so that these processes can be accurately represented in atmospheric chemistry‐climate models.

A modal aerosol module (MAM) has been developed for the Community Atmosphere Model version 5 (CAM5), the atmospheric component of the Community Earth System Model version 1 (CESM1). MAM is capable of simulating the aerosol size distribution and both internal and external mixing between aerosol components, treating numerous complicated aerosol processes and aerosol physical, chemical and optical properties in a physically-based manner. Two MAM versions were developed: a more complete version with seven lognormal modes (MAM7), and a version with three lognormal modes (MAM3) for the purpose of long-term (decades to centuries) simulations. In this paper a description and evaluation of the aerosol module and its two representations are provided. Sensitivity of the aerosol lifecycle to simplifications in the representation of aerosol is discussed. Simulated sulfate and secondary organic aerosol (SOA) mass concentrations are remarkably similar between MAM3 and MAM7. Differences in primary organic matter (POM) and black carbon (BC) concentrations between MAM3 and MAM7 are also small (mostly within 10%). The mineral dust global burden differs by 10% and sea salt burden by 30–40% between MAM3 and MAM7, mainly due to the different size ranges for dust and sea salt modes and different standard deviations of the log-normal size distribution for sea salt modes between MAM3 and MAM7. The model is able to qualitatively capture the observed geographical and temporal variations of aerosol mass and number concentrations, size distributions, and aerosol optical properties. However, there are noticeable biases; e.g., simulated BC concentrations are significantly lower than measurements in the Arctic. There is a low bias in modeled aerosol optical depth on the global scale, especially in the developing countries. These biases in aerosol simulations clearly indicate the need for improvements of aerosol processes (e.g., emission fluxes of anthropogenic aerosols and precursor gases in developing countries, boundary layer nucleation) and properties (e.g., primary aerosol emission size, POM hygroscopicity). In addition, the critical role of cloud properties (e.g., liquid water content, cloud fraction) responsible for the wet scavenging of aerosol is highlighted.

Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO₃, NH₃, HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale.