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Optimal Estimation (OE) methods can simultaneously estimate surface and atmospheric properties from remote Visible/Shortwave imaging spectroscopy. Simultaneous solutions can improve retrieval accuracy with principled uncertainty quantification for hypothesis testing. While OE has been validated under benign atmospheric conditions, future global missions will observe environments with high aerosol and water vapor loadings. This work addresses the gap with diverse scenes from NASA’s Next Generation Airborne Visible Infrared Imaging Spectrometer (AVIRIS-NG) India campaign. We refine atmospheric models to capture varied aerosol optical depths and optical properties. We quantify retrieval accuracy and information content for both reflectance and aerosols over different surface types, comparing results to in situ and remote references. Additionally, we assess uncertainty of maximum a posteriori solutions using linearized estimates as well as new sampling-based inversions that more completely characterize posterior uncertainties. Principled uncertainty quantification can combine multiple spacecraft data products while preventing local environmental biases in future global investigations.