Title: A muSR Investigation of the Two-step Mott Transition in NiS₂ with Se Doping
Description: Mott insulators are a family of materials in which strong electron-electron interactions induce an unconventional insulating state in the system that would otherwise behave as an electrical conductor according to the non-interacting band theory. In particular, the nature of the Mott metal-insulator transition (MIT) has been the subject of intense research interest because it can involve a complicated interplay between magnetic and electronic properties. In some Mott systems, Mott transitions occur in the one-step process, from an antiferromagnetic insulator (AFI) to a paramagnetic metal phase (PMM), while in other Mott systems a two-step transition with an intermediate antiferromagnetic metal (AFM) phase can be observed. Since 2015, the muon spin relaxation (𝜇SR) group at Columbia University started systematic 𝜇SR studies on a series of Mott systems, including one-step transition Mott systems 𝑅𝐸NiO₃ and V₂O₃, as well as two-step transition Mott systems Ba(Co, Ni)S₂, Ni(S, Se)₂ and (La, Sr)VO₃.

This dissertation first introduces the comprehensive 𝜇SR research on multiple families of Mott systems conducted by our 𝜇SR group, including 𝑅𝐸NiO₃, V₂O₃, and BaCoS₂. Then the 𝜇SR experimental findings on the Mott system NiS₂₋ₓSeₓ will be presented, which is the most extensively studied material in this thesis. The NiS₂₋ₓSeₓ system is of particular interest because there is a large region of intermediate AFM state emerging between AFI and PMM states with Se doping, making it an ideal platform to provide information on static magnetism in the AFM state and thus can help us better understand the evolution of magnetic NiS₂₋ₓSeₓ, with our key findings being: (1) The AFM state of the NiS₂₋ₓSeₓ system shows significantly random spin correlations, and the magnetic order is suppressed by a gradual reduction of the ordered moment size, with a nearly full ordered volume fraction until very close to the AFM-PMM boundary. (2) No signature of dynamic critical behavior was observed in the thermal phase transition, indicating a first-order thermal phase transition.

The next part of this dissertation presents our computational simulations on the NiS₂₋ₓSeₓ system. Dipolar field simulations have shown that only the combination of easy axis randomization and Ni moment dilution in NiS₂ can lead to the internal field distribution corresponding to the observed 𝜇SR spectrum in the AFM region. Also, this picture could qualitatively explain the neutron and muon results consistently, thus reconciling the seemingly contradicting experimental results by 𝜇SR and the previous neutron scattering studies shown in the AFM region. Furthermore, we propose a percolation model that can capture both the charge and spin connections of the interpenetrating percolating spin and charge networks in the NiS₂₋ₓSeₓsystem, which raises the possibility of "compromising metallicity and magnetic order" in the two-step Mott transition evolving AFI to AFM to PMM states in NiS₂₋ₓSeₓ.