A few copper and gold smelters in Chile are behind a large fraction of global arsenic emissions, raising concerns for increased concentrations of arsenic in PM10 in Central and Northern Chile. This concern is amplified by the fact that Northern Chile soils and rivers in general are characterized by a high arsenic content. A monitoring and modeling study has been performed to quantify the regional impact of the smelter emissions. Measured atmospheric arsenic concentrations from 2.4 to 30.7 ng m(-3) were found at seven rural stations, located tens to hundreds of kilometers away from the nearest smelter. Analyses of topsoil and subsoil samples taken from PM 10 monitoring stations revealed levels up to 291 mg kg(-1), the highest values found in the northern Atacama desert in Chile. An absolute principal component analysis of selected trace elements in PM10 shows that the regional impact of anthropogenic smelter emissions on airborne arsenic concentrations is more important than the effect of soil dust resuspension. The dominance of the smelter emissions is larger in Central Chile than in the northern parts. The impact of resuspended soil dust on airborne arsenic levels in rural areas was estimated not to exceed 5 ng m(-3). The model calculations support the dominant role of anthropogenic emissions and give spatial and temporal variations in atmospheric concentrations consistent with the monitored levels at five of the seven stations. At two of the northernmost stations indications were found of unidentified sources other than the smelters and the resuspended soil dust, contributing to about 5 ng m(-3) of total arsenic levels. The study confirms that a strong control or elimination of arsenic emissions from the smelters would lead to arsenic in PM10 levels in Northern and Central Chile comparable to non-polluted areas in other countries. (C) 2002 Elsevier Science Ltd. All rights reserved.