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Objectives: The aim of this study was to evaluate the feasibility and accuracy of cardiac late enhancement (LE) scanning for extracellular volume (ECV) quantification with dual-source photon-counting detector computed tomography (PCD-CT). Materials and Methods: In this institutional review board-approved study, 30 patients (mean age, 79 years; 12 women; mean body mass index, 28 kg/m 2 ) with severe aortic stenosis undergoing PCD-CT as part of their preprocedural workup for transcatheter aortic valve replacement were included. The scan protocol consisted of a nonenhanced calcium-scoring scan, coronary CT angiography (CTA) followed by CTA of the thoracoabdominal aorta, and a low-dose LE scan 5 minutes after the administration of 100 mL contrast media (all scans electrocardiogram-gated). Virtual monoenergetic (65 keV) and dual-energy (DE) iodine images were reconstructed from the LE scan. Extracellular volume was calculated using the iodine ratios of myocardium and blood-pool of the LE scan, and additionally based on single-energy (SE) subtraction of the nonenhanced scan from the LE scan. Three-dimensional analysis was performed automatically for the whole-heart myocardial volume by matching a heart model generated from the respective coronary CTA data. Bland-Altman and correlation analysis were used to compare the ECV values determined by both methods. Results: The median dose length product for the LE scan was 84 mGy•cm (interquartile range, 69; 125 mGy•cm). Extracellular volume quantification was feasible in all patients. The median ECV value was 30.5% (interquartile range, 28.4%-33.6%). Two focal ECV elevations matched known prior myocardial infarction. The DE-and SE-based ECV quantification correlated well (r = 0.87, P < 0.001). Bland-Altman analysis showed small mean errors between DE-and SE-based ECV quantification (0.9%; 95% confidence interval, 0.1%-1.6%) with narrow limits of agreement (−3.3% to 5.0%). Conclusions: Dual-source PCD-CT enables accurate ECV quantification using an LE cardiac DE scan at low radiation dose. Extracellular volume calculation from iodine ratios of the LE scan obviates the need for acquisition of a true nonenhanced scan and is not affected by potential misregistration between 2 separate scans.