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We have studied the formation and properties of two-species ion Coulomb crystals in the Penning trap of the SpecTrap experiment. These crystals have been formed by injection of admixture ions from an external source into a previously confined and laser-cooled cloud of magnesium ions. This kind of study, performed over a range of the admixture ions’ charge-to-mass ratios, indicates the conditions for their sympathetic cooling and the formation of two-species ion crystals. This mechanism allows efficient cooling of the admixed species such as highly charged ions which do not feature suitable laser-cooling transitions, and thus make them accessible to high-resolution laser spectroscopy. [ABSTRACT FROM AUTHOR]