The role of charge on aerosol evolution and hence the nuclear source term has been an issue of interest, and there is a need for both experimental techniques and modeling for quantifying this role. Our focus here is on further exploration of a tandem differential mobility analyzer (TDMA) technique to simultaneously measure both the size and charge (positive, negative, and neutral) dependent aerosol distributions. We have generated graphite, gold, silver, and palladium nanoparticles (aerosol) using a spark generator. We measure the electrical mobility-size distributions for these aerosols using a TDMA, and from these data we deduce the full charge-size distributions. We observe asymmetry in the particle size distributions for negative and positive charges. This asymmetry could have a bearing on the dynamics of charged aerosols, indicating that the assumption of symmetry for size distributions of negatively and positively charged particles in source term simulations may not always be appropriate. Also, the experimental technique should find applications in measurements of aerosol rate processes that are affected by both particle charge and size (e.g., coagulation, deposition, and resuspension), and hence in modeling and simulation of the nuclear source term.