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

Abstract

The magnetic ground state of single crystalline RuO${}_2$ was investigated by the muon spin rotation/relaxation ($\mu$SR) experiment. The spin precession signal due to the spontaneous internal magnetic field $B_{\mathrm{loc}}$, 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 $B_{\mathrm{loc}}$ was simulated for the antiferromagnetic (AFM) structures with a Ru magnetic moment $|{\mathbf{m}}_{\mathrm{Ru}}|\approx 0.05{\mu }_{\mathrm{B}}$ suggested from diffraction experiments. As a result, the possibility was ruled out that muons are localized at sites where $B_{\mathrm{loc}}$ accidentally cancels. Conversely, assuming that the slow relaxation observed in $\mu$SR spectra was part of the precession signal, the upper limit for the magnitude of $|{\mathbf{m}}_{\mathrm{Ru}}|$ was estimated to be $4.8(2)\times 10^{-4}{\mu }_{\mathrm{B}}$, which is significantly less than $0.05{\mu }_{\mathrm{B}}$. These results indicate that the AFM order, as reported, is unlikely to exist in the bulk crystal.

6 pages, 4 figures

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