Kinetic modeling of laser-ion beam generation from the “break-out afterburner” (BOA) has been modeled for several deuteron-rich solid-density target foils. Modeling the transport of these beams in a beryllium converter shows as much as a fourfold increase in neutron yield over the present state of the art through the use of alternative target materials. Additionally, species-separation dynamics during the BOA can be exploited to control the hardness of the neutron spectra, of interest for, for example, enhancing penetrability in shielded material in active neutron interrogation settings.