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We present an improved quantitative mobility spectrum analysis (i-QMSA) procedure for determining free electron and hole densities and mobilities from magnetic-field-dependent Hall and resistivity measurements on bulk or layered semiconductor samples. The i-QMSA technique is based on a fundamentally new approach, which optimizes the fit to the conductivity tensor components and their slopes by making those adjustments in the mobility spectra that result in the greatest error reduction. Empirical procedures for manipulating the mobility spectra are also introduced, with the dual purpose of reducing the error of the fit and simplifying the shape of the spectra to minimize the presence of unphysical artifacts. A fully automated computer implementation of the improved QMSA is applied to representative synthetic and real data sets involving various semiconductor material systems. These results show that, as compared with previous approaches, the presented algorithm maximizes the information that may be extracted from a given data set, and is suitable for use as a standard tool in the characterization of semiconductor material and device transport properties. © 1998 American Institute of Physics.