The mass transfer to and from drops is of interest to a number of different fields, including spray and atmospheric systems. For drops falling in a gas the externally controlled mass transfer has been studied by a number of researchers and can be characterized by experimental correlations of Frossling (1 938) and Beard and Pruppacher (1971) or numerical modeling by Woo and Hamielec (I97 1) and Ramachandran (1985). These experimental correlations and models agree quite well. Internal mass transfer has been studied quite extensively, and a number of models have been developed. However, here models and experimental data conflict. That is the focus of this work.Models that have been developed can be divided into two types: stagnant or steady internal flow, and unsteady or turbulent internal flow. For the former case, a maximum rate of mass transfer can be predicted using the Kronig and Brink (1950) model. The circulation rate within drops is assumed to be much faster than the mass transfer rate, so lines of constant concentration become parallel to the streamlines predicted by a Hill's vortex. Higher mass transfer rates can be predicted if unsteady conditions within the drop are assumed. Handlos and Baron ( 1 957) developed a model for internal mass transfer assuming turbulent conditions within a drop. In terms of k,, the liquid-side mass transfer coefficient, their model can be expressed as Ruckenstein (1967) and Ruckenstein et al. (1971) postulated a model in which the drop interior was assumed to be well mixed and the entire resistance to mass transfer restricted to a thin liquid boundary layer. A Hill's vortex solution was linearized near the liquid surface, and the final expression for k, was found to be Angelo et al. (1966) proposed a model for oscillating drops. The authors postulated that during drop oscillation fresh area is formed and returned to the bulk, which is assumed to be well Experimental work has been performed on drops where both types of mass transfer mechanisms might be expected, steady internal circulation and unsteady or turbulent internal flow. Walcek et al. (1984) found that for drops smaller than 1.0 mm dia. falling a t terminal velocity, drops exhibited steady circulation patterns and followed the absorption characteristics of the Kronig and Brink model. For drops larger than 1.8 mm dia. the internal flow became unsteady, and the Kronig and Brink model was modified by using an effective diffusivity of 18 times the molecular diffusivity to explain the mass transfer rate. Between these drop sizes the effective diffusivity was a function of drop size. Garner and Lane (1959) measured the absorption rate of two large drop sizes, 4.22 and 5.85 mm. Absorption rates much greater than those predicted by Kronig and Brink were found. The drop oscillation frequency was observed and measured; it was close to that predicted by Lamb (Clift et al., 1978). Recently Kaji et al. (1985) measured mass transfer coefficients for drops of 2.20 mm dia. formed in an unpolluted atmosphere. The drops then accelerated...