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The Airborne Multiangle SpectroPolarimetric Imager (AirMSPI) is an eight-band (355, 380, 445, 470, 555, 660, 865, 935 nm) pushbroom camera, measuring polarization in the 470, 660, and 865 nm bands, mounted on a gimbal to acquire multiangular observations over a ±67° along-track range. The instrument has been flying aboard the NASA ER-2 high altitude aircraft since October 2010. AirMSPI employs a photoelastic modulator-based polarimetric imaging technique to enable accurate measurements of the degree and angle of linear polarization in addition to spectral intensity. A description of the AirMSPI instrument and ground data processing approach is presented. Example images of clear, hazy, and cloudy scenes over the Pacific Ocean and California land targets obtained during flights between 2010 and 2012 are shown, and quantitative interpretations of the data using vector radiative transfer theory and scene models are provided to highlight the instrument's capabilities for determining aerosol and cloud microphysical properties and cloud 3-D spatial distributions. Sensitivity to parameters such as aerosol particle size distribution, ocean surface wind speed and direction, cloud-top and cloud-base height, and cloud droplet size is discussed. AirMSPI represents a major step toward realization of the type of imaging polarimeter envisioned to fly on NASA's Aerosol-Cloud-Ecosystem (ACE) mission in the next decade.