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Register a new userScattering Continuum and Possible Fractionalized Excitations in $alpha$-RuCl$_3$
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The combination of electronic correlation and spin-orbit coupling is thought to precipitate a variety of highly unusual electronic phases in solids, including topological and quantum spin liquid states. We report a Raman scattering study that provides evidence for unconventional excitations in $alpha$-RuCl$_3$, a spin-orbit coupled Mott insulator on the honeycomb lattice. In particular, our measurements reveal unusual magnetic scattering, typified by a broad continuum. The temperature dependence of this continuum is evident over a large scale compared to the magnetic ordering temperature, suggestive of frustrated magnetic interactions. This is confirmed through an analysis of the phonon linewidths, which show a related anomaly due to spin-phonon coupling. These observations are in line with theoretical expectations for the Heisenberg-Kitaev model and suggest that $alpha$-RuCl$_3$ may be close to a quantum spin liquid ground state.
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We report on THz, infrared reflectivity and transmission experiments for wave numbers from 10 to 8000 cm$^{-1}$ ($sim$ 1 meV - 1 eV) and for temperatures from 5 to 295 K on the Kitaev candidate material {alpha}-RuCl$_3$. As reported earlier, the compound under investigation passes through a first-order structural phase transition, from a monoclinic high-temperature to a rhombohedral low-temperature phase. The phase transition shows an extreme and unusual hysteretic behavior, which extends from 60 to 166 K. In passing this phase transition, in the complete frequency range investigated we found a significant reflectance change, which amounts almost a factor of two. We provide a broadband spectrum of dielectric constant, dielectric loss and optical conductivity from the THz to the mid infrared regime and study in detail the phonon response and the low-lying electronic density of states. We provide evidence for the onset of an optical energy gap, which is of order 200 meV, in good agreement with the gap derived from measurements of the DC electrical resistivity. Remarkably, the onset of the gap exhibits a strong blue shift on increasing temperatures.
We report measurements of optical absorption in the zig-zag antiferromagnet $alpha$-RuCl$_3$ as a function of temperature, $T$, magnetic field, $B$, and photon energy, $hbaromega$ in the range $sim$ 0.3 to 8.3 meV, using time-domain terahertz spectroscopy. Polarized measurements show that 3-fold rotational symmetry is broken in the honeycomb plane from 2 K to 300 K. We find a sharp absorption peak at 2.56 meV upon cooling below the Neel temperature of 7 K at $B=0$ that we identify as magnetic-dipole excitation of a zero-wavevector magnon, or antiferromagnetic resonance (AFMR). With application of $B$, the AFMR broadens and shifts to lower frequency as long-range magnetic order is lost in a manner consistent with transitioning to a spin-disordered phase. From direct, internally calibrated measurement of the AFMR spectral weight, we place an upper bound on the contribution to the $dc$ susceptibility from a magnetic excitation continuum.
We present initial Raman spectroscopy experiments on exfoliated flakes of $alpha$-RuCl$_3$, from tens of nm thick down to single layers. Besides unexpectedly finding this material to be air stable, in the thinnest layers we observe the appearance with decreasing temperature of a symmetry-forbidden mode in crossed polarization, along with an anomalous broadening of a mode at 164 cm$^{-1}$ that is known to couple to a continuum of magnetic excitations. This may be due to an enhancement of magnetic fluctuations and evidence for a distorted honeycomb lattice in single- and bi-layer samples.
Fractionalized excitations are of considerable interest in recent condensed-matter physics. Fractionalization of the spin degrees of freedom into localized and itinerant Majorana fermions are predicted for the Kitaev spin liquid, an exactly solvable model with bond-dependent interactions on a two-dimensional honeycomb lattice. As function of temperature, theory predicts a characteristic two-peak structure of the heat capacity as fingerprint of these excitations. Here we report on detailed heat-capacity experiments as function of temperature and magnetic field in high-quality single crystals of {alpha}-RuCl3 and undertook considerable efforts to determine the exact phonon background. We measured single-crystalline RhCl3 as non-magnetic reference and performed ab-initio calculations of the phonon density of states for both compounds. These ab-initio calculations document that the intrinsic phonon contribution to the heat capacity cannot be obtained by a simple rescaling of the nonmagnetic reference using differences in the atomic masses. Sizable renormalization is required even for non-magnetic RhCl3 with its minute difference from the title compound. In {alpha}-RuCl3 in zero magnetic field, excess heat capacity exists at temperatures well above the onset of magnetic order. In external magnetic fields far beyond quantum criticality, when long-range magnetic order is fully suppressed, the excess heat capacity exhibits the characteristic two-peak structure. In zero field, the lower peak just appears at temperatures around the onset of magnetic order and seems to be connected with canonical spin degrees of freedom. At higher fields, beyond the critical field, this peak is shifted to 10 K. The high-temperature peak located around 50 K is hardly influenced by external magnetic fields, carries the predicted amount of entropy, R/2 ln2, and may resemble remnants of Kitaev physics.
Kitaev interactions underlying a quantum spin liquid have been long sought, but experimental data from which their strengths can be determined directly is still lacking. Here, by carrying out inelastic neutron scattering measurements on high-quality single crystals of $alpha$-RuCl$_3$, we observe spin-wave spectra with a gap of $sim$2 meV around the M point of the two-dimensional Brillouin zone. We derive an effective-spin model in the strong-coupling limit based on energy bands obtained from first-principle calculations, and find that the anisotropic Kitaev interaction $K$ term and the isotropic antiferromagentic off-diagonal exchange interaction $Gamma$ term are significantly larger than the Heisenberg exchange coupling $J$ term. Our experimental data can be well fit using an effective-spin model with $K=-6.8$ meV and $Gamma=9.5$ meV. These results demonstrate explicitly that Kitaev physics is realized in real materials.
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