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Most unconventional superconductors, including cuprates and iron-basedsuperconductors, are derived from chemical doping or application of pressure ontheir collinearly magnetic-ordered parent compounds[1-5]. The recentlydiscovered pressure-induced superconductor CrAs, as a rare example of anon-collinear helimagnetic superconductor, has therefore generated greatinterest in understanding microscopic magnetic properties and their interplaywith superconductivity [6-8]. Unlike cuprates and iron based superconductorswhere the magnetic moment direction barely changes upon doping, here we showthat CrAs exhibits a spin reorientation from the ab plane to the ac plane,along with an abrupt drop of the magnetic propagation vector at a criticalpressure (Pc~0.6 GPa). This magnetic phase transition coincides with theemergence of bulk superconductivity, indicating a direct connection betweenmagnetism and superconductivity. With further increasing pressure, the magneticorder completely disappears near the optimal Tc regime (P~0.94 GPa). Moreover,the Cr magnetic moments between nearest neighbors tend to be alignedantiparallel with increasing pressure toward the optimal superconductivityregime. Our findings suggest that the non-collinear helimagnetic order isstrongly coupled to structural and electronic degrees of freedom, and thatantiferromagnetic correlations associated with the low magnetic vector phaseare crucial for superconductivity.

Structural and Magnetic Phase Diagram of CrAs and its Relationship with Pressure-induced Superconductivity