In novel photovoltaic absorbers, it is often difficult to assess the root causes of low open-circuit voltages, which may be due to bulk recombination or sub-optimal contacts. In the present work, we discuss the role of temperature- and illumination-dependent device electrical measurements in quantifying and distinguishing these per form ance losses - in particular, for determining bounds on interface recombination velocities, band alignment, and minority carrier lifetime. We assess the accuracy of this approach by direct comparison to photoelectron spectroscopy. Then, we demonstrate how more computationally intensive model parameter fitting approaches can draw more insights from this broad measurement space. We apply this measurement and modeling approach to high- performance III-V and thin-film chalcogenide devices.