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Register a new userMagnetic field-dependent low-energy magnon dynamics in $alpha$-RuCl3
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Revealing the spin excitations of complex quantum magnets is key to developing a minimal model that explains the underlying magnetic correlations in the ground state. We investigate the low-energy magnons in $alpha$-RuCl$_3$ by combining time-domain terahertz spectroscopy under an external magnetic field and model Hamiltonian calculations. We observe two absorption peaks around 2.0 and 2.4 meV, which we attribute to zone-center spin waves. Using linear spin-wave theory with only nearest-neighbor terms of the exchange couplings, we calculate the antiferromagnetic resonance frequencies and reveal their dependence on an external field applied parallel to the nearest-neighbor Ru-Ru bonds. We find that the magnon behavior in an applied magnetic field can be understood only by including an off-diagonal $Gamma$ exchange term to the minimal Heisenberg-Kitaev model. Such an anisotropic exchange interaction that manifests itself as a result of strong spin-orbit coupling can naturally account for the observed mixing of the modes at higher fields strengths.
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Single crystals of the Kitaev spin-liquid candidate $alpha$-RuCl$_3$ have been studied to determine low-temperature bulk properties, structure and the magnetic ground state. Refinements of x-ray diffraction data show that the low temperature crystal structure is described by space group $C2/m$ with a nearly-perfect honeycomb lattice exhibiting less than 0.2 % in-plane distortion. The as-grown single crystals exhibit only one sharp magnetic transition at $T_{N}$ = 7~K. The magnetic order below this temperature exhibits a propagation vector of $k$ = (0, 1, 1/3), which coincides with a 3-layer stacking of the $C2/m$ unit cells. Magnetic transitions at higher temperatures up to 14~K can be introduced by deformations of the crystal that result in regions in the crystal with a 2-layer stacking sequence. The best fit symmetry allowed magnetic structure of the as-grown crystals shows that the spins lie in the $ac$-plane, with a zigzag configuration in each honeycomb layer. The three layer repeat out-of-plane structure can be refined as a 120$^o$ spiral order or a collinear structure with spin direction 35$^o$ away from the $a$-axis. The collinear spin configuration yields a slightly better fit and also is physically preferred. The average ordered moment in either structure is less than 0.45(5) $mu_B$ per Ru$^{3+}$ ion.
We use time-domain terahertz spectroscopy to measure the low energy conductivity and magnons in RuCl$_3$ under external magnetic field. At zero field, an oscillation with a frequency of 0.62 THz is clearly observed in time-domain spectrum below T$_N$, which is identified as a magnon excitation in the magnetic order state. The magnon excitation is not affected by the external magnetic field $textbf{H}_{DC}$ when it is applied along the c-axis, but is clearly suppressed when $textbf{H}_{DC}$ is applied within ab plane. More interestingly, when the magnetic component of THz wave $textbf{h}(t)$ is perpendicular to the applied in-plane magnetic field, we observe another coherent oscillation at slightly higher energy scale at the field above 2 T, which is eventually suppressed for $H_{DC}>$5 T. The measurement seems to indicate that the in-plane magnetic field can lift the degeneracy of two branches of low energy magnons at $Gamma$ point. The low energy optical conductivity calculated from the measured transmission spectrum is dominated by a broad continuum contribution, which is not affected by changing either temperature or external magnetic field. The continuum is likely to be related to the fractional spin excitation due to dominated Kitaev interaction in the material.
Kitaev-type interactions between neighbouring magnetic moments emerge in the honeycomb material ${alpha}$-RuCl3. It is debated however whether these Kitaev interactions are ferromagnetic or antiferromagnetic. With electron energy loss spectroscopy (EELS) we study the lowest excitation across the Mott-Hubbard gap, which involves a d4 triplet in the final state and therefore is sensitive to nearest-neighbor spin-spin correlations. At low temperature the spectral weight of these triplets is strongly enhanced, in accordance with optical data. We show that the magnetic correlation function that determines this EELS spectral weight is directly related to a Kitaev-type spin-spin correlator and that the temperature dependence agrees very well with the results of a microscopic magnetic Hamiltonian for ${alpha}$-RuCl3 with ferromagnetic Kitaev coupling.
We investigate the phononic in-plane longitudinal low-temperature thermal conductivity kappa_ab of the Kitaev quantum magnet alpha-RuCl3 for large in-plane magnetic fields up to 33 T. Our data reveal for fields larger than the critical field Bc ~ 8 T, at which the magnetic order is suppressed, a dramatic increase of kappa_ab at all temperatures investigated. The analysis of our data shows that the phonons are not only strongly scattered by a magnetic mode at relatively large energy which scales roughly linearly with the magnetic field, but also by a small-energy mode which emerges near Bc with a square-root-like field dependence. While the former is in striking agreement with recent spin wave theory (SWT) results of the magnetic excitation spectrum at the Gamma point, the energy of the latter is too small to be compatible with the SWT-expected magnon gap at the M point, despite the matching field dependence. Therefore, an alternative scenario based on phonon scattering off the thermal excitation of random-singlet states is proposed.
The light-induced femtosecond dynamics of the sublattice magnetizations in the antiferromagnetically ordered phase of the semiconductor $alpha$-MnTe is investigated theoretically as function of an external driving field. The electromagnetic field is coupled to optical modes and the concomitant atomic displacements modulate the Heisenberg exchange couplings. We derive the equations of motion for the time-dependent sublattice magnetization in spin wave theory and analyze the contributions from the driven magnon modes. The antiferromagnetic order parameter exhibits coherent longitudinal oscillations determined by the external driving frequency which decay due to dephasing. Including a phenomenological dissipative term to mimic spin-lattice relaxation processes leads to relaxation back to thermal equilibrium. We provide approximate analytic solutions of the resulting differential equations which allow us to understand the effect of the driving light pulse on the amplitude, frequency, and lifetime of the coherent spin dynamics.
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