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Al—Fe—Si alloys having optimized properties through the use of additives are disclosed. In some aspects, an alloy includes aluminum in a first amount, iron in a second amount, silicon in a third amount, and an additive in a fourth amount. The additive is selected from the group consisting of a non-metal additive, a transition-metal additive, a rare-metal additive, and combinations thereof. The first amount, the second amount, the third amount, and the fourth amount produce an alloy with a stoichiometric formula (Al1-xAx)3Fe2Si where A is the additive.