We present first-principles results on the magnetoelastic coupling in $α$-RuCl$_3$ and uncover a striking dependence of the magnetic coupling constants on strain effects. Different magnetic interactions are found to respond very unequally to variations in the lattice, with the Kitaev interaction being the most sensitive. Exact diagonalization results on our magnetoelastic model reproduce recent measurements of the structural Grüneisen parameter and explain the origin of the negative magnetostriction of $α$-RuCl$_3$, disentangling contributions related to different anisotropic interactions and g factors. Uniaxial strain perpendicular to the honeycomb planes is predicted to reorganize the relative coupling strengths, strongly enhancing the Kitaev interaction while simultaneously weakening the other anisotropic exchanges under compression. Uniaxial strain may therefore pose a fruitful route to experimentally tune $α$-RuCl$_3$ nearer to the Kitaev limit.
The Kitaev material $α$-RuCl$_3$ is among the most prominent candidates to host a quantum spin-liquid state endowed with fractionalized excitations. Recent experimental and theoretical investigations have separately revealed the importance of both the magnetoelastic coupling and the magnetic anisotropy, in dependence of the applied magnetic field direction. In this combined theoretical and experimental research, we investigate the anisotropic magnetic and magnetoelastic properties for magnetic fields applied along the main crystallographic axes as well as for fields canted out of the honeycomb…
We present high-resolution thermal-expansion and specific-heat measurements of single crystalline alpha-RuCl3. An extremely hysteretic structural transition expanding over 100 K is observed by thermal- expansion along both crystallographic axes, which we attribute to a change of stacking sequence of the RuCl3 layers. Three magnetic transitions are observed, which we link to the different stacking sequences. Using our data and thermodynamic relations, we derive the uniaxial and hydrostatic pressure derivatives of all three magnetic transitions. Our results demonstrate that magnetic order should…
We present high-resolution measurements of the thermal expansion and the magnetostriction of TlCuCl$_{3}$ which shows field-induced antiferromagnetic order. We find pronounced anomalies in the field and temperature dependence of different directions of the lattice signaling a large magnetoelastic coupling. The phase boundary is extremely sensitive to pressure, e.g. the transition field would change by about +/- 185$%/GPa under uniaxial pressure applied along certain directions. This drastic effect can unambiguously be traced back to changes of the intradimer coupling under uniaxial pressure. T…
Single crystals of Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl were investigated using high-resolution capacitance dilatometry in magnetic fields up to 15 T. Pronounced magnetoelastic coupling is found upon evolution of long-range antiferromagnetic order at T$_{\mathrm{N}} = 26.4(3)$ K. Grüneisen analysis reveals moderate effects of uniaxial pressure on T$_{\mathrm{N}}$, of $1.8(4)$ K/GPa, $-0.62(15)$ K/GPa and $0.33(10)$ K/GPa for $p \parallel a$, $b$, and $c$, respectively. Below 22 K, Grüneisen scaling fails which implies the presence of competing interactions. The structural phase transition at T$_{\math…
We report detailed thermodynamic studies on high-quality single crystals of the centrosymmetric skyrmion-hosting intermetallic Gd2PdSi3 by means of high-resolution capacitance dilatometry in fields up to 15 T which are complemented by specific heat and magnetization studies. Our dilatometric measurements show magnetoelastic effects associated with antiferromagnetic order at TN1 = 22.3 K and TN2 = 19.7 K, as well as strong field effects in an applied magnetic field of 15 Tup to 200 K (150 K) for B||c (B||a*, i.e. B perp c). The data allow us to complete the magneticphase diagram, including a ne…
We report high-resolution capacitance dilatometry studies on the uniaxial length changes in a NdB$_4$ single crystal. The evolution of magnetically ordered phases below $T_{\rm N}$= 17.2~K (commensurate antiferromagnetic phase, cAFM), $T_{\rm IT}$= 6.8~K (intermediate incommensurate phase, IT), and $T_{\rm LT}$= 4.8~K (low-temperature phase, LT) is associated with pronounced anomalies in the thermal expansion coefficients. The data imply significant magneto-elastic coupling and evidence of a structural phase transition at $T_{\rm LT}$ . While both cAFM and LT favor structural anisotropy $δ$ be…
Magnetoelastic coupling and uniaxial pressure dependencies of the ferromagnetic ordering temperature in the quasi-two-dimensional layered van-der-Waals material CrI$_3$ are experimentally studied and quantified by high-resolution dilatometry. Clear anomalies in the thermal expansion coefficients at $T_{\rm C}$ imply positive (negative) pressure dependencies $\partial T_{\rm C}/\partial p_{\rm i}$ for pressure applied along (perpendicular to) the $c$ axis. The experimental results are backed up by numerical studies showing that the dominant, intra-layer magnetic coupling increases upon compress…
We report magnetic and inter-plane transport properties of Ca3Ru2O7 at high magnetic fields and low temperatures. Ca3Ru2O7 with a bilayered orthorhombic structure is a Mott-like system with a narrow charge gap of 0.1eV. Of a host of unusual physical phenomena revealed in this study, a few are particularly intriguing: (1) a collapse of the c-axis lattice parameter at a metal-nonmetal transition, TMI (=48 K), and a rapid increase of TMI with low uniaxial pressure applied along the c-axis; (2) quantum oscillations in the gapped, nonmetallic state for 20 mK<T<6.5 K; (3) tunneling colossal magnetor…
Magnetoelastic interaction couples spin and lattice degrees of freedom and plays a key role in thermal transport properties of magnetic insulators. In the Kitaev quantum spin liquid, the low energy excitations are charge neutral Majorana fermions, which transform the magnetoelasctic interaction into Majorana-phonon scattering. Motivated by anomalous thermal properties of the Kitaev quantum spin liquid candidate RuCl$_3$, in this letter, we combine meV resolution inelastic x-ray scattering and theoretical calculation to examine the Majorana-phonon scattering. We analytically derive the velocity…
In this work, we study magnetoelastic interactions by means of ultrasound experiments in $α$-RuCl$_3$ -- a prototypical material for the Kitaev spin model on the honeycomb lattice, with a possible spin-liquid state featuring Majorana fermions and $\mathbb{Z}_{2}$-flux excitations. We present results of the temperature and in-plane magnetic-field dependence of the sound velocity and sound attenuation for several longitudinal and transverse phonon modes propagating along high-symmetry crystallographic directions. A comprehensive data analysis above the ordered state provides strong evidence of p…
Considerable research interest has been attracted to noncollinear magnetic structures for their intriguing physics and promising applications. In this work, based on relativistic density functional theory, we reveal the interesting magnetic order and relevant properties in monolayer RuF$_4$, which can be exfoliated from its bulk phase. Although the spins on Ru ions are almost antiferromagnetically aligned between nearest-neighbors, weak ferromagnetism is generated because of the antisymmetric Dzyaloshinskii-Moriya interaction as well as the single-ion anisotropy. A prominent magneto-optical Ke…
We report a method for determining the spatial dependence of the magnetic exchange coupling, $dJ/dr$, from magnetostriction measurements of a quantum magnet. The organic Ni $S = 1$ system NiCl$_2$-4SC(NH$_2$)$_2$ exhibits lattice distortions in response to field-induced canted antiferromagnetism between $H_{c1} = 2.1$ T and $H_{c2} = 12.6$ T. We are able to model the magnetostriction in terms of uniaxial stress on the sample created by magnetic interactions between neighboring Ni atoms along the c-axis. The uniaxial strain is equal to $(1/E)dJ_c/dx_c < S_{\bf r} \cdot S_{{\bf r}+ {\bf e}_c} >$…
We report a detailed experimental and theoretical study on the effect of hydrostatic pressure on the structural and magnetic aspects of the layered honeycomb antiferromagent $α$-RuCl$_{3}$. Magnetic susceptibility measurements performed under almost ideal hydrostatic-pressure conditions yield that the phase transition to zigzag-type antiferromagnetic order at $T_N$ = 7.3 K can be rapidly suppressed to about 6.1 K. A further suppression with increasing pressure is impeded due to the occurrence of a pressure-induced structural transition at $p \geq$ 104 MPa, accompanied by a strong dimerization …
We report the thermodynamic properties studied by thermal expansion, magnetostriction, magnetisation, and specific heat measurements as well as the low-energy magnetic excitations of \mto\ and investigate how magneto-elastic coupling and magnetic anisotropy affect the evolution of long-range order and the magnetic phase diagram. Specifically, we utilise high-resolution capacitance dilatometry and antiferromagnetic resonance (AFMR) studies by means of high-frequency electron spin resonance (HF-ESR) spectroscopy. The role of anisotropy is reflected by spin-reorientation at $B_{\rm{SF}}$~$\simeq …
Cr$_2$Ge$_2$Te$_6$ is a quasi-2D semiconducting van der Waals ferromagnet down to the bilayer with great potential for technological applications. Engineering the critical temperature to achieve room temperature applications is one of the critical next steps on this path. Here, we report high-resolution capacitance dilatometry studies on Cr$_2$Ge$_2$Te$_6$ single crystals which directly prove significant magnetoelastic coupling and provide quantitative values of the large uniaxial pressure effects on long-range magnetic order (${\partial}T_{\mathrm{C}}/{\partial}p_{\mathrm{c}}$ = 24.7 K/GPa an…
High-quality single crystals of CoTiO$_3$ are grown and used to elucidate in detail structural and magnetostructural effects by means of high-resolution capacitance dilatometry studies in fields up to 15 T which are complemented by specific heat and magnetization measurements. In addition, we refine the single-crystal structure of the ilmenite ($R\bar{3}$) phase. At the antiferromagnetic ordering temperature $T_\mathrm{N}$, pronounced $λ$-shaped anomaly in the thermal expansion coefficients signals shrinking of both the $c$ and $b$ axes, indicating strong magnetoelastic coupling with uniaxial …
Competing Interactions and the Effects of Uniaxial Out-of-plane Perturbations in the Honeycomb Antiferromagnet Na$_2$Co$_2$TeO$_6$
Kirchhoff Institute for Physics, Heidelberg University（海德堡大学基尔霍夫物理研究所）；Institute of Physics, Academia Sinica（中央研究院物理学研究所）；Department of Physics, Sungkyunkwan University（成均馆大学物理系）
The magnetic, thermodynamic, and pyroelectric properties of LiFeP$_2$O$_7$ single crystals are investigated with emphasis on the magnetoelectric interaction of the electrical polarization with the magnetic order parameter. The magnetic order below T$_N\simeq$ 27 K is found to be a canted antiferromagnet with a weak ferromagnetic component along the $b-$axis. A sharp peak of the pyroelectric current at T$_N$ proves the strong internal magnetoelectric interaction resulting in a sizable polarization decrease at the onset of magnetic order. The magnetoelectric effect in external magnetic fields co…
