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Systems and methods that utilize bremsstrahlung radiation may be used to facilitate the setting of a settable composition. For example, a method may include providing a settable composition in a portion of a wellbore penetrating a subterranean formation, a portion of the subterranean formation, or both; conveying an electron accelerator tool along the wellbore proximal to the settable composition; producing an electron beam in the electron accelerator tool with a trajectory that impinges a converter material, thereby converting the electron beam to bremsstrahlung photons; and irradiating the settable composition with the bremsstrahlung photons.