No Arabic abstract
We present an investigation of the influence of low-levels of chemical substitution on the magnetic ground state and N{ e}el skyrmion lattice (SkL) state in GaV$_4$S$_{8-y}$Se$_y$, where $y =0, 0.1, 7.9$, and $8$. Muon-spin spectroscopy ($mu$SR) measurements on $y=0$ and 0.1 materials reveal the magnetic ground state consists of microscopically coexisting incommensurate cycloidal and ferromagnetic environments, while chemical substitution leads to the growth of localized regions of increased spin density. $mu$SR measurements of emergent low-frequency skyrmion dynamics show that the SkL exists under low-levels of substitution at both ends of the series. Skyrmionic excitations persist to temperatures below the equilibrium SkL in substituted samples, suggesting the presence of skyrmion precursors over a wide range of temperatures.
Polycrystalline members of the GaV$_4$S$_{8-y}$Se$_y$ family of materials with small levels of substitution between $0 leq y leq 0.5$ and $7.5 leq yleq 8$ have been synthesized in order to investigate their magnetic and structural properties. Substitutions to the skyrmion hosting parent compounds GaV$_4$S$_8$ and GaV$_4$Se$_8$, are found to suppress the temperature of the cubic to rhombohedral structural phase transition that occurs in both end compounds and to create a temperature region around the transition where there is a coexistence of these two phases. Similarly, the magnitude of the magnetization and temperature of the magnetic transition are both suppressed in all substituted compounds until a glassy-like magnetic state is realized. There is evidence from the $ac$ susceptibility data that skyrmion lattices with similar dynamics to those in GaV$_4$S$_8$ and GaV$_4$Se$_8$ are present in compounds with very low levels of substitution, $0 < y< 0.2$ and $7.8 < y < 8$, however, these states vanish at higher levels of substitution. The magnetic properties of these substituted materials are affected by the substitution altering exchange pathways and resulting in the creation of increasingly disordered magnetic states.
We report small-angle neutron scattering studies of the lacunar spinel GaV$_4$S$_8$, which reveal the long-wavelength magnetic states to be cycloidally modulated. This provides direct support for the formation of Neel-type skyrmions recently claimed to exist in this compound. In striking contrast with all other bulk skyrmion host materials, upon cooling the modulated magnetic states transform into a ferromagnetic state. These results indicate all of the modulated states in GaV$_4$S$_8$, including the skyrmion state, gain their stability from thermal fluctuations, while at lower temperature the ferromagnetic state emerges in accord with the strong easy-axis magnetic anisotropy. In the vicinity of the transition between the ferromagnetic and modulated states, both a phase coexistence and a soliton-like state are also evidenced by our study.
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 on the anomalous magnetization dynamics of the cycloidally-modulated spin textures under the influence of uniaxial anisotropy in multiferroic $mathrm{GaV_4S_8}$. The temperature and field dependence of the linear ac susceptibility [$chi_{1omega}^{prime}(T,H)$], ac magnetic loss [$chi_{1omega}^{primeprime}(T,H)$], and nonlinear ac magnetic response [$M_{3omega}(T,H)$] are examined across the magnetic phase diagram in the frequency range $f = 10-10000$ Hz. According to recent theory, skyrmion vortices under axial crystal symmetry are confined along specific orientations, resulting in enhanced robustness against oblique magnetic fields and altered spin dynamics. We characterize the magnetic response of each spin texture and find that the dynamic rigidity of the Neel skyrmion lattice appears enhanced compared to Bloch-type skyrmions in cubic systems, even in the multidomain state. Anomalous $M_{3omega}$ and strong dissipation emerge over the same phase regime where strong variations in the cycloid pitch were observed on lowering temperature in recent small-angle neutron scattering experiments [White et al., Phys. Rev. B 97, 020401(R) (2018)]. Here, we show that strong anisotropy also drives an extended crossover of the zero-field cycloid texture in $mathrm{GaV_4S_8}$. The frequency dependence of these dynamic signatures is consistent with that of a robust anharmonic spin texture exhibiting a correlated domain arrangement. The results underpin the essential role of magnetic anisotropy in enhancing the rigidity of topological spin textures for diverse applications.
ZrSiS is a nodal-line semimetal, whose electronic band structure contains a diamond-shaped line of Dirac nodes. We carried out a comparative study on the optical conductivity of ZrSiS and related compounds ZrSiSe, ZrSiTe, ZrGeS, and ZrGeTe by reflectivity measurements over a broad frequency range combined with density functional theory calculations. The optical conductivity exhibits a distinct U shape, ending at a sharp peak at around 10000~cm$^{-1}$ for all studied compounds, except for ZrSiTe. The U shape of the optical conductivity is due to transitions between the linearly dispersing bands crossing each other along the nodal line. The sharp high-energy peak is related to transitions between almost parallel bands, and its energy position depends on the interlayer bonding correlated with the $c$/$a$ ratio, which can be tuned by either chemical or external pressure. For ZrSiTe, another pair of crossing bands appears in the vicinity of the Fermi level, corrugating the nodal-line electronic structure and leading to the observed difference in optical conductivity. The findings suggest that the Dirac physics in Zr$XY$ compounds with $X$=Si, Ge and $Y$=S, Se, Te is closely connected to the interlayer bonding.