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 talk, 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 constraint on the dictionary coefficients. Our method uses a greedy support selection method and a new pair-wise iterated coordinate descent method to compute the above estimate. We demonstrate that our dictionary-based method outperforms a state-of-the-art method as shown in a cross-validation experiment on simulated datasets and some real datasets collected at beamline 8.3.2 of the Advanced Light Source (ALS) and Zeiss Xradia 510 Versa.