Volume-wise destruction of the antiferromagnetic Mott insulating state through quantum tuning

Metal-to-insulator transitions (MITs) are a dramatic manifestation of strong electron correlations in solids1. The insulating phase can often be suppressed by quantum tuning, i.e. varying a nonthermal parameter such as chemical composi- tion or pressure, resulting in a zero-temperature quantum phase transition (QPT) to a metallic state driven by quantum fluctuations, in contrast to conventional phase transitions driven by thermal fluctuations. Theories of exotic phenomena known to occur near the Mott QPT such as quantum criticality and high-temperature superconductivity often assume a second-order QPT, but direct experimental evidence for either first- or second-order behavior at the magnetic QPT associated with the Mott transition has been scarce and further masked by the superconducting phase in unconventional superconductors. Most measurements of QPTs have been performed by volume-integrated probes, such as neutron scattering, magnetization, and transport, in which discontinuous behavior, phase separation, and spatially inhomogeneous responses are averaged and smeared out, leading at times to misidentification as continuous second-order transitions. Here, we demonstrate through muon spin relaxation/rotation (MuSR) experiments on two archetypal Mott insulating systems, composition-tuned RENiO3 (RE=rare earth element) and pressured-tuned V2O3, that the QPT from antiferromagnetic insulator to paramagnetic metal is first-order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value across the phase diagram until it is suddenly destroyed at the QPT. These findings call for further investigation into the role of inelastic soft modes and the nature of dynamic spin and charge fluctuations underlying the transition.