Highly accurate multi-angle polarimeters are essential for taking the next step in global characterization of atmospheric aerosol. Spectral polarization modulation enables highly accurate snapshot polarimetry and is very suitable for ground-, air- and space-based instrumentation. In this paper we present two instruments that employ this technology, the SPEX prototype and groundSPEX. We have performed ground-based measurements at the CESAR Observatory in the Netherlands with these two instruments. We compare the measured degree of linear polarization of co- located measurements, which show an rms difference of 0.005. Aerosol microphysical properties that have been retrieved from these measurements agree well with similar retrievals from AERONET measurements. Finally, we discuss the current efforts to upgrade the SPEX prototype to an autonomous instrument suitable for flying on NASA’s ER-2 high altitude aircraft.