A method of synthesizing uranium dioxide crystals. The method of synthesizing includes combining a uranium-based feedstock with a mineralizer solution. The uranium-based feedstock is selected from uranium dioxide, uranium tetrafluoride, uranium tetrachloride, triuranium octoxide, and uranium trioxide. The feedstock and mineralizer solution are pressurized, and then a thermal gradient is 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. The 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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