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D. A. S. Kaib

Publications and source records attributed to D. A. S. Kaib.

5 recordsLinked to original sources

Accessing Few-Layer CrI$_3$ Magnetoelasticity Through Bulk Single Crystals

The persistence of ferromagnetic long-range order in monolayers of the van der Waals semiconductor CrI$_3$ opens new routes for spintronic applications based on two-dimensional quantum magnets. In the fabrication of such devices, the constituent materials inevitably experience anisotropic strain, which modifies their intrinsic electronic properties. At the same time, strain can serve as a powerful tuning parameter, driving the material to desired regimes. While several theoretical studies have investigated the effect of biaxial in-plane strain on CrI$_3$ numerically, experiments are widely limited to the application of hydrostatic pressure. Here, we perform high-resolution magnetostriction experiments on bulk CrI$_3$ samples, and \textit{ab-initio}-based magnetoelastic calculations, to elucidate the role of uniaxial lattice strain on the magnetic properties. Our data show that magnetostriction in CrI$_3$ is unexpectedly sensitive to surface effects, which enables us to investigate the influence of in-plane and out-of-plane strain separately, in both the bulk ferromagnetic (BFM) phase emerging at $T_{\rm C}=61\,\mathrm{K}$ and the surface antiferromagnetic (SAFM) phase below $T^* \simeq 50\,\mathrm{K}$. In particular, we quantify the uniaxial strain dependence of the surface interlayer coupling $J^{\rm SAFM}_{\perp}$ and the surface spin-flip field $B^*$, which drastically exceed the strain effects in the BFM phase by a factor of $\sim 30$. The large magnetostrictive response allows us to study the magnetoelastic coupling in few-layer CrI$_3$ through experiments on bulk single crystals, without requiring exfoliation.

cond-mat.str-el↗

Combined experimental and theoretical study of hydrostatic (He-gas) pressure effects in $α$-RuCl$_3$

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 of Ru-Ru bonds, which gives rise to a collapse of the magnetic susceptibility. Whereas the dimerization transition is strongly first order, as reflected by large discontinuous changes in $χ$ and pronounced hysteresis effects, the magnetic transition under varying pressure and magnetic field also reveals indications for a weakly first-order transition. We assign this observation to a strong magnetoelastic coupling in this system. Measurements of $χ$ under varying pressure in the paramagnetic regime ($T > T_N$) and before dimerization ($p <$ 100 MPa) reveal a considerable increase of $χ$ with pressure. These experimental observations are consistent with the results of ab-initio Density Functional Theory (DFT) calculations on the pressure-dependent structure and the corresponding pressure-dependent magnetic model. Comparative susceptibility measurements on a second crystal showing two consecutive magnetic transitions instead of one, indicating the influence of stacking faults. Using different temperature-pressure protocols the effect of these stacking faults can be temporarily overcome, transforming the magnetic state from a multiple-$T_N$ into a single-$T_N$ state.

cond-mat.str-el↗

Angle-dependent thermodynamics of $α$-RuCl$_3$

Thermodynamics of the Kitaev honeycomb magnet $α$-RuCl$_3$ is studied for different directions of in-plane magnetic field using measurements of the magnetic Grüneisen parameter $Γ_B$ and specific heat $C$. We identify two critical fields $B_c^{\rm AF1}$ and $B_c^{\rm AF2}$ corresponding, respectively, to a transition between two magnetically ordered states and the loss of magnetic order toward a quantum paramagnetic state. The $B_c^{AF2}$ phase boundary reveals a narrow region of magnetic fields where inverse melting of the ordered phase may occur. No additional transitions are detected above $B_c^{\rm AF2}$ for any direction of the in-plane field, although a shoulder anomaly in $Γ_B$ is observed systematically at $8-10$ T. Large field-induced entropy effects imply additional low-energy excitations at low fields and/or strongly field-dependent phonon entropies. Our results establish universal features of $α$-RuCl$_3$ in high magnetic fields and challenge the presence of a field-induced Kitaev spin liquid in this material.

cond-mat.str-el↗

Thermodynamic perspective on the field-induced behavior of $α$-RuCl$_3$

Measurements of the magnetic Grüneisen parameter ($Γ_B$) and specific heat on the Kitaev material candidate $α$-RuCl$_3$ are used to access in-plane field- and temperature-dependence of the entropy up to 12 T and down to 1 K. No signatures corresponding to phase transitions are detected beyond the boundary of the magnetically ordered region, but only a shoulder-like anomaly in $Γ_B$, involving an entropy increment as small as $10^{-5} R\log 2$. These observations put into question the presence of a thermodynamic phase transition between the purported quantum spin liquid and the field-polarized state of $α$-RuCl$_3$. We show theoretically that at low temperatures $Γ_B$ is sensitive to crossings in the lowest excitations within gapped phases, and identify the measured shoulder-like anomaly as being of such origin. Exact diagonalization calculations demonstrate that the shoulder-like anomaly can be reproduced in extended Kitaev models that gain proximity to an additional phase at finite field without entering it. We discuss manifestations of this proximity in other measurements.

cond-mat.str-el↗

High-Field Quantum Disordered State in $α$-RuCl3: Spin Flips, Bound States, and a Multi-Particle Continuum

Layered $α$-RuCl3 has been discussed as a proximate Kitaev spin liquid compound. Raman and THz spectroscopy of magnetic excitations confirm that the low-temperature antiferromagnetic ordered phase features a broad Raman continuum, together with two magnon-like excitations at 2.7 and 3.6 meV, respectively. The continuum strength is maximized as long-range order is suppressed by an external magnetic field. The state above the field-induced quantum phase transition around 7.5 T is characterized by a gapped multi-particle continuum out of which a two-particle bound state emerges, together with a well-defined single-particle excitation at lower energy. Exact diagonalization calculations demonstrate that Kitaev and off-diagonal exchange terms in the Fleury-Loudon operator are crucial for the occurrence of these features in the Raman spectra. Our study firmly establishes the partially-polarized quantum disordered character of the high-field phase.

cond-mat.str-el↗