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We report 7Li-NMR studies on LiInCr4O8 and LiGaCr4O8, in which Cr3+ ions withspin 3/2 form a breathing pyrochlore lattice, a network of tetrahedra withalternating sizes. In LiInCr4O8 with large alternation, the nuclear relaxationrate 1/T1 shows an activated temperature (T) dependence down to 18 K,indicating a singlet ground state with a spin gap. This behavior, however, isdisrupted by an antiferromagnetic (AF) transition at 13 K, which is preceded byanother, most likely structural, transition at 16 K. In contrast, LiGaCr4O8with small alternation shows no spin gap but exhibits a first-order AFtransition over a distributed T-range 13-20 K. Nevertheless, 1/T1 of theparamagnetic phase diverges toward 13 K, indicating proximity to a second-ordertransition. The results indicate that LiGaCr4O8 is located in the vicinity of atricritical point in the phase diagram.

Novel Phase Transitions in the Breathing Pyrochlore Lattice: 7Li-NMR on LiInCr4O8 and LiGaCr4O8