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The magnetic properties of dilute Li_2(Li_1-xFe_x)N with x ∼ 0.001 are dominated by the spin of single, isolated Fe atoms. Below T = 10 K the spin-relaxation times become temperature-independent indicating a crossover from thermal excitations to the quantum tunneling regime. We report on a strong increase of the spin-flip probability in transverse magnetic fields that proves the resonant character of this tunneling process. Longitudinal fields, on the other hand, lift the ground-statedoi:10.1103/physrevlett.120.147202 pmid:29694147 fatcat:hh6ggzqjnbfnlabbu27jxahaeq