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The rainout-determined lifetimes of highly soluble particulate and gaseous atmospheric compounds are investigated using general circulation model simulations in which removal is explicitly calculated in terms of the local, model-produced precipitation rates. Our calculations indicate that because of the episodic and asymmetric nature of rainout, species' lifetimes depend not only on the amount of precipitation but also on the characteristics of the precipitation regime (such as duration and frequency of the precipitation events) and on the direction of the tracer main flow (determined by the species' average mixing ratio gradient). For this reason, averaged rainout lifetimes of tracers flowing downward from the stratosphere are found to differ substantially from those of tracers of surface origin flowing upward or tracers of a more ubiquitous tropospheric source. These results imply that the use of a first-order parameterization to simulate rainout in a photochemical model that does not explicitly calculate precipitation can be inadequate in representing this process. A computationally efficient parameterization that includes the effects of intermittence and asymmetry of rainout is proposed, and it is shown how this parameterization can be used to estimate rainout-determined tropospheric residence times from observational data sets. A review of published estimates of submicron aerosol tropospheric residence times based on observations shows that these are consistent with our model results.