This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. Review pubs.acs.org/CR Multiphase Chemistry at the Atmosphere−Biosphere Interface Inﬂuencing Climate and Public Health in the Anthropocene Ulrich Po schl* and Manabu Shiraiwa* Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany air contaminants (SHCC) and their multiphase chemical interactions at the atmosphere−biosphere interface, including human lungs and skin, plant leaves, cryptogamic covers, soil, and aquatic surfaces. After an overview of diﬀerent groups of SHCC, we address the chemical interactions of reactive oxygen species and reactive nitrogen species (ROS, RNS), primary biological and secondary organic aerosols (PBA, SOA), as well as carbonaceous combustion aerosols (CCA) including soot, black/elemental carbon, polycyclic aromatic hydrocarbons, and related compounds (PAH, PAC). ROS and RNS interact strongly with other SHCC and are central to both atmospheric and physiological processes and their coupling through the atmosphere−biosphere interface, for example, in the formation and aging of biogenic and combustion aerosols as well as in CONTENTS inﬂammatory and allergic immune responses triggered by air pollution. Deposition of atmospheric ROS/RNS and aerosols 1. Introduction and Motivation can damage biological tissues, modify surface microbiomes, and 2. Health- and Climate-Relevant Air Contaminants induce oxidative stress through Fenton-like reactions and 2.1. Reactive Oxygen and Nitrogen Species immune responses. The chemical mechanisms and kinetics are 2.2. Primary Biological Aerosols not yet fully elucidated, but the available evidence suggests that 2.3. Secondary Organic Aerosols multiphase processes are crucial for the assessment, prediction, 2.4. Carbonaceous Combustion Aerosols and handling of air quality, climate, and public health. Caution 2.5. Other Air Contaminants Linking Atmospher- should be taken to avoid that human activities shaping the ic and Physiological Chemistry Anthropocene create a hazardous or pathogenic atmosphere 3. Multiphase Chemical Reactions at Speciﬁc Bio- overloaded with allergenic, corrosive, toxic, or infectious logical Interfaces contaminants. 3.1. Lung Lining Fluid Multiphase chemistry deals with chemical reactions, trans- 3.2. Human Skin port processes, and transformations between gaseous, liquid, 3.3. Plant Surfaces and Cryptogamic Covers and solid matter. These processes are essential for Earth system 3.4. Soil and Aquatic Surfaces science and climate research as well as for life and health 4. Conclusions and Outlook sciences on molecular and global levels, bridging a wide range Author Information of spatial and temporal scales from below nanometers to Corresponding Authors thousands of kilometers and from less than nanoseconds to Notes years and millennia as illustrated in Figure 1. Biographies From a chemical perspective, life and the metabolism of most Acknowledgments living organisms can be regarded as multiphase processes References involving gases like oxygen and carbon dioxide; liquids like water, blood, lymph, and plant sap; and solid or semisolid substances like bone, tissue, skin, wood, and cellular 1. INTRODUCTION AND MOTIVATION membranes. Even primitive forms of life and metabolic activity Multiphase chemistry plays a vital role in the Earth system, under anaerobic conditions generally involve multiple liquid climate, and health. Chemical reactions, mass transport, and and solid or semisolid phases structured by cells, organelles, and phase transitions between gases, liquids, and solids are essential membranes. 2 On global scales, the biogeochemical cycling of for the interaction and coevolution of life and climate. chemical compounds and elements, which can be regarded as Knowledge of the mechanisms and kinetics of these processes the metabolism of planet Earth, also involves chemical is also required to address societally relevant questions of global reactions, mass transport, and phase transitions within and environmental change and public health in the Anthropocene, that is, in the present era of globally pervasive and steeply Special Issue: 2015 Chemistry in Climate increasing human inﬂuence on planet Earth. 1 In this work, we review the current scientiﬁc understanding and recent advances Received: September 1, 2014 in the investigation of short-lived health- and climate-relevant Published: April 9, 2015 © 2015 American Chemical Society DOI: 10.1021/cr500487s Chem. Rev. 2015, 115, 4440−4475

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Multiphase chemistry at the atmosphere-biosphere interface influencing climate and public health in the anthropocene.

Heavy metal and nitrogen concentrations in mosses are declining across Europe whilst some "hotspots" remain in 2010.

This is the nal report of the rst year of the Artwork project. It contains a chapter devoted to each of the major three phases of the project. Chapter 1 contains the nal report on Phase One of the rst year of the Artwork project. The initial phase of the Artwork feasibility study was to perform a comparative analysis of language usage in spoken dialog, the modality of speech-to-speech translation, and in written text, the modality assumed for the development of most current MT systems including the CRL's. The objective was to establish a range of structural, functional and interpersonal characteristics for each modality which can be taken as processing requirements, to see which are associated with both modalities and which are associated with just one of the modalities, and, nally, to identify the relative importance of the diierent characteristics to successfully processing utterances produced under each modality. The tasks involved in carrying out the comparative analysis included: (1) the collection and transcription of the spoken data for the analysis (approximately an hour of taped interviews) and the preparation of the written data (EFE newswire articles), (2) the quantitative analysis of the transcriptions and texts with respect to a number of relevant linguistic characteristics, and (3) the comparison of the resultant analyses for diierences between dialogs and text. In addition, approximately midway through the project it was decided that (4) the impact of protocol on dialog was to be analyzed. Chapter 4 contains the results of tasks 1, 2, 3. Chapter 3, which contains the results of Phase Three of the project, contains the results of task 4. Chapter 2 contains the nal report on Phase Two of the project. The goal of this phase was to identify a number of translation problems that appear to be peculiar to dialog translation as opposed to text translation and to survey current MT system capabilities for dealing with these problems. The chapter is therefore divided into two part: a survey of dialog translation problems and a survey of current MT system techniques for dealing with them. Chapter 3 contains the nal report on Phase Three of the project. According to a revised plan of research, which was agreed to during the fth bimonthly reporting period, Phase Three of the project consists of (1) a study comparing dialogs collected within a push-to-talk protocol with dialogs collected within a cross-talk protocol and (2) identifying …

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Nitrogen concentrations in mosses indicate the spatial distribution of atmospheric nitrogen deposition in Europe.