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In order to study a change in electrochemical, structural, and magnetic properties for lithium manganese oxide spinels Li[LixMn2−x]O4 (LMO) with 0 ≤ x ≤ 1/3, muon-spin rotation and relaxation (μSR) spectra were recorded under pressure (P) up to 2.1 GPa. At ambient P, P = 0.1 MPa, the antiferromagnetic or spin-glass-like transition temperature (Tm) at P = 0.1 MPa monotonically decreases with increasing x. On the contrary, the slope of the Tm vs. P (dTm/dP) rapidly increases from 0.9(1) K/GPa at x = 0 to 1.4 K/GPa at x = 0.1, then drops to 0.7(1) K/GPa at x = 0.15, and finally keeps constant (∼0.4 K/GPa) with further increasing x. Considering the structural change of LMO with x, the decrease in the distance between Mn ions (dMn-Mn) is likely to play an essential role for determining Tm under P. According to cyclic voltammetry on LMO, the peak current at both anodic and cathodic directions shows the maximum at x = 0.1, indicating the highest diffusivity of Li+ ions (DLi) at x = 0.1.

Pressure dependence of magnetic transition temperature in Li[LixMn2−x]O4 (0 ≤ x ≤ 1/3) studied by muon-spin rotation and relaxation