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Observations from the Ground-based Multiangle SpectroPolarimetric Imager (GroundMSPI) are used to relate angle of linear polarization (AoLP) measurements to material properties and illumination conditions in sunlit outdoor environments. GroundMSPI is a push-broom spectropolarimetric camera with an uncertainty in degree of linear polarization (DoLP) of ±0.005. This polarimetric accuracy yields useful AoLP images even when the DoLP is less than 0.02. AoLP images are reported with respect to dependency on surface texture, surface orientation, albedo, and illumination conditions. Agreement with well-known principles of polarized light scattering is illustrated, and several special cases are described. Expected observations of AoLP tangential to surface orientation and AoLP perpendicular to the scattering plane are reported. Significant changes in the AoLP are observed from common variations in outdoor …