The effect of charge on the sedimentation of macromolecules has been studied by Tiselius,' by Svedberg and Pedersen,2 and, subsequently and in greater detail, by I'eder~en.~ The basic concepts of their treatment may be formulated as follows. The macromolecules in solution are considered to be dissociated into ions, each macromolecule yielding Z + 1 free moving charged particles, vie, one (2-valent) macroion and Z (monovalent) small counterions. Additional positive and negative small ions may be provided through the inclusion in the system of a dissociating low molecular weight salt. When an external centrifugal field is applied, the ions will tend to move with unequal velocities, each kind according to its proper buoyant weight and friction coefficient. The unequal displacement of the ions will create a macroscopic electrostatic field in the solution and, if the direct interactions of the ions one with another and with the solvent are disregarded, the resultant motion of any ion may be described as an algebraic sum of two virtual motions : A sedimentation in the (externally applied) centrifugal field and an electrophoretic migration in the (internally created) electrostatic field. This additional electrophoretic motion gives rise to the so-called charge effect in sedimentation. A relatively simple expression may then be derived which describes the charge effect in terms of concentrations, valencies, buoyant weights and mobilities of all the ionic species in solution. Several detailed studies of charge effect in sedimentation have been rep~rted.~" The results were found to be in a qualitative agreement with the aforementioned elementary theory of Svedberg and Pedersen but the observed charge effect turned out to be much larger, by a factor of two or more. Furthermore, a charge effect is expected to occur in diffusion in much the same way as in sedimentation, so that measurement under the same conditions of both diffusion and sedimentation should greatly facilitate the critical interpretation of the charge effect. However very few diffusion studies of the charge effect are a~a i l a b l e .~-~ The interrelation between sedimentation and diffusion of electrolytes has been studied recently but mainly from the point of view of molecular weight determination.l0> 1 1~~5The elementary theory of the charge effect of Svedberg-Pedersen has thus found no quantitative confirmation in the sedimentation results, nor has it been supplemented by an allied treatment of the diffusion process. The