Nonmagnetic Ground State in RuO$_2$ Revealed by Muon Spin Rotation

The magnetic ground state of single crystalline RuO$_2$ was investigated by the muon spin rotation/relaxation ($μ$SR) experiment. The spin precession signal due to the spontaneous internal magnetic field $B_{\rm loc}$, which is expected in the magnetically ordered phase, was not observed in the temperature range 5--400~K. Muon sites were evaluated by first-principles calculations using dilute hydrogen simulating muon as pseudo-hydrogen, and $B_{\rm loc}$ was simulated for the antiferromagnetic (AFM) structures with a Ru magnetic moment $|{\bf m}_{\rm Ru}|\approx0.05μ_\mathrm{B}$ suggested from diffraction experiments. As a result, the possibility was ruled out that muons are localized at sites where $B_{\rm loc}$ accidentally cancels. Conversely, assuming that the slow relaxation observed in $μ$SR spectra was part of the precession signal, the upper limit for the magnitude of $|{\bf m}_{\rm Ru}|$ was estimated to be $4.8(2)\times10^{-4}μ_{\rm B}$, which is significantly less than $0.05μ_\mathrm{B}$. These results indicate that the AFM order, as reported, is unlikely to exist in the bulk crystal.