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The n-type HgCr2Se4 exhibits a sharp semiconductor-to-metal transition (SMT)in resistivity accompanying the ferromagnetic order at TC = 106 K. Here, weinvestigate the effects of pressure and magnetic field on the concomitant SMTand ferromagnetic order by measuring resistivity, dc and ac magneticsusceptibility, as well as single-crystal neutron diffraction under variouspressures up to 8 GPa and magnetic fields up to 8 T. Our results demonstratethat the ferromagnetic metallic ground state of n-type HgCr2Se4 is destabilizedand gradually replaced by an antiferromagnetic, most likely a spiral magnetic,and insulating ground state upon the application of high pressure. On the otherhand, the application of external magnetic fields can restore the ferromagneticmetallic state again at high pressures, resulting in a colossalmagnetoresistance (CMR) as high as ~ 3 * 10^11 % under 5 T and 2 K at 4 GPa.The present study demonstrates that n-type HgCr2Se4 is located at a peculiarcritical point where the balance of competion between ferromagnetic andantiferromagnetic interactions can be easily tipped by the external stimuli,providing a new platform for achieving CMR in a single-valent system.

Magnetic competition induced colossal magnetoresistance in n-type HgCr2Se4 under high pressures