A method of synthesizing rubidium uranium fluoride crystals. The method includes combining uranium-based feedstock with a mineralizer solution that includes a rubidium fluoride. The feedstock and mineralizer solution are pressurized and a thermal gradient applied thereto such that a first portion of the feedstock and the mineralizer solution is heated to a temperature that is greater than a temperature of a second portion of the feedstock and the mineralizer solution. Uranium nutrient enters the mineralizer solution from the feedstock in the first portion and uranium nutrient precipitates to spontaneously form crystals in the second portion.
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