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Register a new userOptical conductivity in multiferroic GaV$_4$S$_8$ and GeV$_4$S$_8$: Phonons and electronic transitions
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We report on optical spectroscopy on the lacunar spinels GaV$_4$S$_8$ and GeV$_4$S$_8$ in the spectral range from 100 to 23000 cm$^{-1}$ and for temperatures from 5 to 300 K. These multiferroic spinel systems reveal Jahn-Teller driven ferroelectricity and complex magnetic order at low temperatures. We study the infrared-active phonon modes and the low-lying electronic excitations in the cubic high-temperature phase, as well as in the orbitally and in the magnetically ordered low-temperature phases. We compare the phonon modes in these two compounds, which undergo different symmetry-lowering Jahn-Teller transitions into ferroelectric and orbitally ordered phases, and exhibit different magnetic ground states. We follow the splitting of the phonon modes at the structural phase transition and detect additional splittings at the onset of antiferromagnetic order in GeV$_4$S$_8$. We observe electronic transitions within the $d$-derived bands of the V$_4$ clusters and document a significant influence of the structural and magnetic phase transitions on the narrow electronic band gaps.
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The orientation of Neel-type skyrmions in the lacunar spinels GaV$_4$S$_8$ and GaV$_4$Se$_8$ is tied to the polar axes of their underlying crystal structure through the Dzyaloshinskii-Moriya interaction. In these crystals, the skyrmion lattice phase exists for externally applied magnetic fields parallel to these axes and withstands oblique magnetic fields up to some critical angle. Here, we map out the stability of the skyrmion lattice phase in both crystals as a function of field angle and magnitude using dynamic cantilever magnetometry. The measured phase diagrams reproduce the major features predicted by a recent theoretical model, including a reentrant cycloidal phase in GaV$_4$Se$_8$. Nonetheless, we observe a greater robustness of the skyrmion phase to oblique fields, suggesting possible refinements to the model. Besides identifying transitions between the cycloidal, skyrmion lattice, and ferromagnetic states in the bulk, we measure additional anomalies in GaV$_4$Se$_8$ and assign them to magnetic states confined to polar structural domain walls.
We report the feasibility of using magnetoentropic mapping for the rapid identification of magnetic cycloid and skyrmion phases in uniaxial systems, based on the GaV4S8 and GaV4Se8 model skyrmion hosts with easy-axis and easy-plane anisotropies respectively. We show that these measurements can be interpreted with the help of a simple numerical model for the spin Hamiltonian to yield unambiguous assignments for both single phase regions and phase boundaries. In the two lacunar spinel chemistries, we obtain excellent agreement between the measured magnetoentropic features and a minimal spin Hamiltonian built on Heisenberg exchange, single-ion anisotropy, and anisotropic Dzyaloshinskii-Moriya interactions. In particular, we identify characteristic high-entropy behavior in the cycloid phase that serves as a precursor to the formation of skyrmions at elevated temperatures and is a readily-measurable signature of this phase transition. Our results demonstrate that rapid magnetoentropic mapping guided by numerical modeling is an effective means of understanding the complex magnetic phase diagrams innate to skyrmion hosts. One notable exception is the observation of an anomalous, low-temperature high-entropy state in the easy-plane system GaV$_4$Se$_8$, which is not captured in the numerical model. Possible origins of this state are discussed.
We present the results of broadband dielectric spectroscopy of GaMo$_4$S$_8$, a lacunar spinel system that recently was shown to exhibit non-canonical, orbitally-driven ferroelectricity. Our study reveals complex relaxation dynamics of this multiferroic material, both above and below its Jahn-Teller transition at T$_{textrm{JT}}=47$ K. Above T$_{textrm{JT}}$, two types of coupled dipolar-orbital dynamics seem to compete: relaxations within cluster-like regions with short-range polar order like in relaxor ferroelectrics and critical fluctuations of only weakly interacting dipoles, the latter resembling the typical dynamics of order-disorder type ferroelectrics. Below the Jahn-Teller transition, the onset of orbital order drives the system into long-range ferroelectric order and dipolar dynamics within the ferroelectric domains is observed. The coupled dipolar and orbital relaxation behavior of GaMo$_4$S$_8$ above the Jahn-Teller transition markedly differs from that of the skyrmion host GaV$_4$S$_8$, which seems to be linked to differences in the structural distortions of the two systems on the unit-cell level.
We have investigated the directional dichroism of magnetic resonance spectra in the polar ferromagnet GaV$_4$S$_8$. While four types of structural domains are energetically degenerated under zero field, the magnetic resonance for each domain is well separated by applying magnetic fields due to uniaxial magnetic anisotropy. Consequently, the directional dichroism as large as 20 % is clearly observed without domain cancellation. The present observation therefore demonstrates that not only magnetoelectric mono-domain crystals but also magnetoelectric multi-domain specimens can be used to realize microwave (optical) diodes owing to the lack of inversion domains.
The magnetic ground state of polycrystalline Neel skyrmion hosting material GaV$_4$S$_8$ has been investigated using ac susceptibility and powder neutron diffraction. In the absence of an applied magnetic field GaV$_4$S$_8$ undergoes a transition from a paramagnetic to a cycloidal state below 13~K and then to a ferromagnetic-like state below 6~K. With evidence from ac susceptibility and powder neutron diffraction, we have identified the commensurate magnetic structure at 1.5 K, with ordered magnetic moments of $0.23(2)~mu_{mathrm{B}}$ on the V1 sites and $0.22(1)~mu_{mathrm{B}}$ on the V2 sites. These moments have ferromagnetic-like alignment but with a 39(8)$^{circ}$ canting of the magnetic moments on the V2 sites away from the V$_4$ cluster. In the incommensurate magnetic phase that exists between 6 and 13 K, we provide a thorough and careful analysis of the cycloidal magnetic structure exhibited by this material using powder neutron diffraction.
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