Competing4f-electron dynamics in Ce(Ru1−xFex)2Al10(0≤x≤1.0): Magnetic ordering emerging from the Kondo semiconducting state

Abstract

We have carried out muon spin relaxation (\ensuremath{\mu}SR), neutron diffraction, and inelastic neutron scattering (INS) investigations on polycrystalline samples of Ce(Ru${}_{1\ensuremath{-}x}$Fe${}_{x}$)${}_{2}$Al${}_{10}$ ($x=0$, 0.3, 0.5, 0.8, and 1) to investigate the nature of the ground state (magnetic ordered versus paramagnetic) and the origin of the spin-gap formation as evident from the bulk measurements in the end members. Our zero-field \ensuremath{\mu}SR spectra clearly reveal coherent two-frequency oscillations at low temperature in $x=0$, 0.3, and 0.5 samples, which confirm the long-range magnetic ordering of the Ce moment with N\`eel temperature T${}_{\mathrm{N}}=27$, 26, and 21 K, respectively. On the other hand, the \ensuremath{\mu}SR spectra of $x=0.8$ and $x=1$ down to 1.4 K and 0.045 K, respectively, exhibit a temperature-independent Kubo-Toyabe term, confirming a paramagnetic ground state. The long-range magnetic ordering in $x=0.5$ below 21 K has been confirmed through the neutron diffraction study. INS measurements of $x=0$ clearly reveal the presence of a sharp inelastic excitation near 8 meV between 5 K and 26 K, due to an opening of a gap in the spin excitation spectrum, which transforms into a broad response at and above 30 K. Interestingly, at 4.5 K, the spin-gap excitation broadens in $x=0.3$ and exhibits two clear peaks at 8.4(3) and 12.0(5) meV in $x=0.5$. In the $x=0.8$ sample, which remains paramagnetic down to 1.2 K, there is a clear signature of a spin gap of 10--12 meV at 7 K, with a strong wave-vector--dependent intensity. Evidence of a spin gap of 12.5(5) meV has also been found in $x=1$. The observation of a spin gap in the paramagnetic samples ($x=0.8$ and 1) is an interesting finding in this study, and it challenges our understanding of the origin of the semiconducting gap in Ce${T}_{2}$Al${}_{10}$ ($T$ = Ru and Os) compounds in terms of a hybridization gap opening only a small part of the Fermi surface, gapped spin waves, or a spin-dimer gap.