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5 meV. Our results deepen the fundamental understanding of organic compounds with magnetic ground states, featuring perspectives in carbon-based spintronic devices.The complex structures and electronic properties of alkali metals and their alloys provide a natural laboratory for studying the interelectronic interactions of metals under compression. A recent theoretical study (J. Phys. Chem. Lett.2019, 10, 3006) predicted an interesting pressure-induced decomposition-recombination behavior of the Na2K compound over a pressure range of