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Abstract

Total environmental and compartmental residence times as a measure for persistence as well as indicators for long-range transport potential (LRTP) have been derived from global geo-referenced modelling and LRTP is characterized in two geographic directions for the first time. A dynamic multicompartment chemistry-transport model (MCTM) was used to study the fate of the insecticides DDT and alpha-hexachlorocyclohexane (alpha-HCH) during the first 2 years upon entry. The indicators for LRTP were defined such as to address the tendencies of substance distributions to migrate ('plume displacement', PD) and to spread into remote areas ('spatial spreading', SS). The indicators deliver values as function of time upon entry. With the aim to address the effect of location of entry on environmental fate, scenarios of emission from the territories of seven countries were studied. It was found that the effect of location of entry on the spatial scale of countries (400-4000 km) is significant for the compartmental distribution and the inter-compartmental mass exchange fluxes (e.g., number of atmospheric cycles, 'hops'). Location of entry introduces uncertainties in the order of a factor of 5 for the total environmental residence time, tau(overall), and a factor of 5-20 for PD and SS. For the 2nd year upon entry into the environment, tau(overall) = 317-1527 days are predicted for DDT and 101-463 days for alpha-HCH. The influence of location of entry does affect the substance ranking, i.e. we cannot simply state that DDT is more persistent than alpha-HCH, but for one scenario studied, application in China, the opposite is predicted. Precipitation patterns proved to be significant, besides other climate parameters, for atmospheric residence time. Integration of the location of entry in chemicals risk assessments is therefore recommended. In general, persistence and some indicators for LRTP, pertinent to their definition, refer to the fate of a large fraction, e.g., 63% ( = 1 - 1/e) or 90%, but not the total substance burden. The choice of this fraction may have the consequence of a normative step which defines the spatial and temporal extensions of a related chemicals risk assessment and may affect substance ranking