A detailed investigation of ZnCr2Se4 is presented which is dominated by strong ferromagnetic exchange but orders antiferromagnetically at TN=21 K. Specific heat and thermal expansion exhibit sharp first-order anomalies at the antiferromagnetic transition. TN is shifted to lower temperatures by external magnetic fields and finally is fully suppressed by a field of 65 kOe. The relative length change DeltaL/L(T) is unusually large and exhibits negative thermal expansion alpha below 75 K down to TN indicating strong frustration of the lattice. Magnetostriction DeltaL/L(H) reveals large values comparable to giant magnetostrictive materials. These results point to a spin-driven origin of the structural instability at TN explained in terms of competing ferromagnetic and antiferromagnetic exchange interactions.
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