The Pedosphere as a Sink, Source, and Record of Anthropogenic and Natural Arsenic Atmospheric Deposition.

The Anthropocene has led to global-scale contamination of the biosphere through diffuse atmospheric dispersal of arsenic. This review considers the sources arsenic to soils and its subsequent fate, identifying key knowledge gaps. There is a particular focus on soil classification and stratigraphy, as this is central to the topic under consideration. For Europe and North America, peat core chrono-sequences record massive enhancement of arsenic depositional flux from the onset of the Industrial Revolution to the late 20th century, while modern mitigation efforts have led to a sharp decline in emissions. Recent arsenic wet and dry depositional flux measurements and modern ice core records suggest that it is South America and East Asia that are now primary global-scale polluters. Natural sources of arsenic to the atmosphere are primarily from volcanic emissions, aeolian soil dust entrainment, and microbial biomethylation. However, quantifying these natural inputs to the atmosphere, and subsequent redeposition to soils, is only starting to become better defined. The pedosphere acts as both a sink and source of deposited arsenic. Soil is highly heterogeneous in the natural arsenic already present, in the chemical and biological regulation of its mobility within soil horizons, and in interaction with climatic and geomorphological settings. Mineral soils tend to be an arsenic sink, while organic soils act as both a sink and a source. It is identified here that peatlands hold a considerable amount of Anthropocene released arsenic, and that this store can be potentially remobilized under climate change scenarios. Also, increased ambient temperature seems to cause enhanced arsine release from soils, and potentially also from the oceans, leading to enhanced rates of arsenic biogeochemical cycling through the atmosphere. With respect to agriculture, rice cultivation was identified as a particular concern in Southeast Asia due to the current high arsenic deposition rates to soil, the efficiency of arsenic assimilation by rice grain, and grain yield reduction through toxicity.