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As computational tools for X-ray computed tomography (CT) become more quantitatively accurate, knowledge of the source-detector spectral response is critical for quantitative system-independent reconstruction and material characterization capabilities. Directly measuring the spectral response of a CT system is hard, which motivates spectral estimation using transmission data obtained from a collection of known homogeneous objects. However, the associated inverse problem is ill-conditioned, making accurate estimation of the spectrum challenging, particularly in the absence of a close initial guess.In this paper, we describe a dictionary-based spectral estimation method that yields accurate results without the need for any initial estimate of the spectral response. Our method utilizes a MAP estimation framework that combines a physics-based forward model along with an L ₀ sparsity constraint and a simplex …