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Report No.

Two-step Mott transition in Ni(S,Se)$$_2$$; $$mu$$SR studies and charge-spin percolation model

Sheng, Q.*; Kaneko, Tatsuya*; Yamakawa, Kohtaro*; Guguchia, Z.*; Gong, Z.*; Zhao, G.*; Dai, G.*; Jin, C.*; Guo, S.*; Fu, L.*; Gu, Y.*; Ning, F.*; Cai, Y.*; Kojima, Kenji*; Beare, J.*; Luke, G. M.*; Miyasaka, Shigeki*; Matsuura, Masato*; Shamoto, Shinichi*; Ito, Takashi   ; Higemoto, Wataru  ; Gauzzi, A.*; Klein, Y.*; Uemura, Yasutomo*

A pyrite system NiS$$_{2-x}$$Se$$_x$$ exhibits a bandwidth controlled Mott transition via (S,Se) substitutions in a two-step process: the antiferromagnetic insulator (AFI) to antiferromagnetic metal (AFM) transition at $$xsim$$0.45 followed by the AFM to paramagnetic metal (PMM) transition at $$xsim$$1.0. Among a few other Mott systems which exhibit similar two-step transitions, Ni(S,Se)$$_2$$ is of particular interest because a large intermediate AFM region in the phase diagram would provide unique opportunities to study the interplay between the spin and charge order. By comparing and combining our muon spin relaxation studies and previous neutron scattering studies, here we propose a picture where the spin order is maintained by the percolation of "nonmetallic" localized and dangling Ni moments surrounded by S, while the charge transition from AFI to AFM is caused by the percolation of the conducting paths generated by the Ni-Se-Ni bonds.



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