arXiv subjects

Th. Doert

Publications and source records attributed to Th. Doert.

At least 19 recordsLinked to original sources

arXiv2025

Anisotropic magnetism and spin fluctuations in the triangular-lattice spin-liquid candidate NaYbSe$_2$: a single-crystal $^{23}$Na and $^{77}$Se NMR study

The ytterbium-based delafossite NaYbSe$_2$ is discussed as a prototype for a spin-orbit entangled, effective spin-1/2 triangular spin lattice with emerging antiferromagnetic correlations and a quantum-spin-liquid (QSL) ground state. We report on a comprehensive study of the static and dynamic anisotropic magnetism in single-crystalline samples of NaYbSe$_2$, using NMR spectroscopy as a local-probe technique. We performed $^{23}$Na and $^{77}$Se NMR measurements in magnetic fields up to 16 T, applied along the in-plane and out-of-plane crystallographic directions and at temperatures from 300 down to 0.3 K. We could determine the anisotropic hyperfine contributions from the angular dependence of the $^{23}$Na and $^{77}$Se NMR spectra. In the paramagnetic regime, we probed the temperature dependence of the $^{23}$Na and $^{77}$Se spectral shift and the hyperfine coupling constants for fields applied along the principal crystal axes. The spin-lattice relaxation-rate data indicate critical spin fluctuations and the absence of long-range magnetic order at low magnetic fields and temperatures down to 0.3 K, evidenced by a monotonic increase of $1/T_1$ and associated spectral broadening. This is a clear proof of the evolution of a critical QSL ground state with residual fluctuations down to lowest temperatures. At elevated fields, we observe the emergence of long-range order, as the temperature-dependent $1/T_1$ rate passes through a pronounced maximum at $T_N$ at given field, followed by a decrease at lower temperatures. Further, we find an inhomogeneous broadening of the $^{23}$Na spectra below $T_N$, probing the histogram of the local-field distribution in the presence of the field-induced order.

cond-mat.str-el↗

arXiv2022

Dilution of the magnetic lattice in the Kitaev candidate $\alpha$-RuCl$_3$ by Rh$^{3+}$ doping

Magnetic dilution of a well-established Kitaev candidate system is realized in the substitutional Ru$_{1-x}$Rh$_x$Cl$_3$ series ($x = 0.02-0.6$). Optimized syntheses protocols yield uniformly-doped single crystals and polycrystalline powders that are isostructural to the parental $\alpha$-RuCl$_3$ as per X-ray diffraction. The Rh content $x$ is accurately determined by the quantitative energy-dispersive X-ray spectroscopy technique with standards. We determine the magnetic phase diagram of Ru$_{1-x}$Rh$_x$Cl$_3$ for in-plane magnetic fields from magnetization and specific-heat measurements as a function of $x$ and stacking periodicity, and identify the suppression of the magnetic order at $x \approx 0.2$ towards a disordered phase, which does not show any clear signature of freezing into a spin glass. Comparing with previous studies on the substitution series Ru$_{1-x}$Ir$_x$Cl$_3$, we propose that chemical pressure would contribute to the suppression of magnetic order especially in Ru$_{1-x}$Ir$_x$Cl$_3$ and that the zigzag magnetic ground state appears to be relatively robust with respect to the dilution of the Kitaev--$\Gamma$--Heisenberg magnetic lattice. We also discovered a slight dependence of the magnetic properties on thermal cycling, which would be due to an incomplete structural transition.

cond-mat.str-el↗

arXiv2022

Spin-wave dynamics in the KCeS2 delafossite: A theoretical description of powder inelastic neutron-scattering data

Layered rare-earth delafossites $ARX_2$ with $R$ = Yb(III) or Ce(III) have received a lot of interest as potential hosts for a quantum spin-liquid ground state. Some systems of this family that show no long-range order down to the lowest measured temperatures, such as NaYbO$_2$, NaYbS$_2$, and NaYbSe$_2$, are presumed to be in a quantum spin-liquid state. However, other isostructural compounds are known to order antiferromagnetically at subkelvin temperatures. Among them, KCeS$_2$ exhibits stripe-$yz$ magnetic order in the triangular-lattice planes that sets in below 400 mK. Here we investigate the spin-wave spectrum of this ordered phase with powder inelastic neutron scattering and describe it using a model Hamiltonian obtained from first-principles calculations based on the complete $|J,m_J\rangle$ multiplet description of the Ce sites with an anisotropic nearest-neighbor exchange interaction. Combing the current understanding of the exchange interaction in the systems with the effects of texturing in the powder, we have been able to model the inelastic neutron scattering spectrum with high fidelity.

cond-mat.str-el↗

arXiv2021

Yb delafossites: unique exchange frustration of 4f spin 1/2 moments on a perfect triangular lattice

While the Heisenberg model for magnetic Mott insulators on planar lattice structures is comparatively well understood in the case of transition metal ions, the intrinsic spin-orbit entanglement of 4f magnetic ions on such lattices shows fascinating new physics largely due to corresponding strong anisotropies both in their single-ion and their exchange properties. We show here that the Yb delafossites, containing perfect magnetic Yb$^{3+}$ triangular lattice planes with pseudospin $s=1/2$ at low temperatures, are an ideal platform to study these new phenomena. Competing frustrated interactions may lead to an absence of magnetic order associated to a gapless spin liquid ground state with a huge linear specific heat exceeding that of many heavy fermions, whereas the application of a magnetic field induces anisotropic magnetic order with successive transitions into different long ranged ordered structures. In this comparative study, we discuss our experimental findings in terms of a unified crystal-field and exchange model. We combine electron paramagnetic resonance (EPR) experiments and results from neutron scattering with measurements of the magnetic susceptibility, isothermal magnetization up to full polarization, and specific heat to determine the relevant model parameters. The impact of the crystal field is discussed as well as the symmetry-compatible form of the exchange tensor, and we give explicit expressions for the anisotropic g factor, the temperature dependence of the susceptibility, the exchange-narrowed EPR linewidth and the saturation field.

cond-mat.str-el↗

arXiv2020

Magnetic Properties of an Effective Spin-$\frac{1}{2}$ Triangular-Lattice Compound LiYbS$_2$

Here, we report the synthesis and magnetic properties of a Yb-based triangular-lattice compound LiYbS$_2$. At low temperatures, it features an effective spin-$\frac{1}{2}$ state due to the combined effect of crystal electric field and spin orbit coupling. Magnetic susceptibility measurements and $^7$Li nuclear magnetic resonance experiments reveal the absence of magnetic long range ordering down to 2~K, which suggests a possible quantum spin liquid ground state. A dominant antiferromagnetic nearest neighbour exchange interaction $J/k_{\rm B}\simeq$ 5.3~K could be extracted form the magnetic susceptibility. The NMR linewidth analysis yields the coupling constant between the Li nuclei and Yb$^{3+}$ ions which was found to be purely dipolar in nature.

cond-mat.str-el↗

arXiv2019

Anisotropic field-induced ordering in the triangular-lattice quantum spin liquid NaYbSe$_2$

High-quality single crystals of NaYbSe$_2$, which resembles a perfect triangular-lattice antiferromagnet without the intrinsic disorder, are investigated by magnetization and specific heat, as well as the local probe techniques nuclear magnetic resonance (NMR) and electron spin resonance (ESR). The low-field measurements confirm the absence of any spin freezing or long-range magnetic order down to 50~mK, which suggests a quantum spin liquid ground (QSL) state with gapless excitations. The instability of the QSL state is observed upon applying magnetic fields. For the $H\bot c$ direction, a field-induced magnetic phase transition is observed above 2~T from the $C_{\rm p}(T)$ data, agreeing with a clear $\frac{M_s}{3}$ plateau of $M(H)$, which is associated with an up-up-down (uud) spin arrangement. For the $H\|c$ direction, a field-induced transition could be evidenced at a much higher field range (9 - 21~T). The $^{23}$Na NMR measurements provide microscopic evidence for field-induced ordering for both directions. A reentrant behavior of $T_{\rm N}$, originating from the thermal and quantum spin fluctuations, is observed for both directions. The anisotropic exchange interactions $J_{\perp}\simeq$ 4.7~K and $J_z\simeq$2.33~K are extracted from the modified bond-dependent XXZ model for the spin-$\frac{1}{2}$ triangular-lattice antiferromagnet. The absence of magnetic long-range order at zero fields is assigned to the effect of strong bond-frustration, arising from the complex spin-orbit entangled $4f$ ground state. Finally, we derive the highly anisotropic magnetic phase diagram, which is discussed in comparison with the existing theoretical models for spin-$\frac{1}{2}$ triangular-lattice antiferromagnets.

cond-mat.str-el↗

arXiv2019

Quantum spin liquid ground state in the disorder free triangular lattice NaYbS$_2$

Rare-earth delafossites were recently proposed as promising candidates for the realization of an effective $S$=1/2 quantum spin liquid (QSL) on the triangular lattice. In contrast to the most actively studied triangular-lattice antiferromagnet YbMgGaO$_4$, which is known for considerable structural disorder due to site intermixing, NaYbS$_2$ delafossite realizes structurally ideal triangular layers. We present detailed $\mu$SR studies on this regular (undistorted) triangular Yb sublattice based system with effective spin $J_{\mathrm{eff}}=1/2$ in the temperature range 0.05 - 40 K. Zero-field (ZF) and longitudinal field (LF) $\mu$SR studies confirm the absence of any long range magnetic order state down to 0.05K ($\sim J$/80). Current $\mu$SR results together with the so far available bulk characterization data suggest that NaYbS$_2$ is an ideal candidate to identify QSL ground state.

cond-mat.str-el↗

arXiv2018

NaYbS$_2$ - a new planar spin-$\frac{1}{2}$ triangular-lattice magnet and putative spin liquid

Platelike high-quality NaYbS$_{2}$ rhombohedral single crystals with lateral dimensions of a few mm have been grown and investigated in great detail by bulk methods like magnetization and specific heat, but also by local probes like nuclear magnetic resonance (NMR), electron-spin resonance (ESR), muon-spin relaxation ($\mu$SR), and inelastic neutron scattering (INS) over a wide field and temperature range. Our single-crystal studies clearly evidence a strongly anisotropic quasi-2D magnetism and an emerging spin-orbit entangled $S=1/2$ state of Yb towards low temperatures together with an absence of long-range magnetic order down to 260~mK. In particular, the clear and narrow Yb ESR lines together with narrow $^{23}$Na NMR lines evidence an absence of inherent structural distortions in the system, which is in strong contrast to the related spin-liquid candidate YbMgGaO$_{4}$ falling within the same space group $R\overline{3}m$. This identifies NaYbS$_{2}$ as a rather pure spin-1/2 triangular lattice magnet and a new putative quantum spin liquid.

cond-mat.str-el↗

arXiv2017

Nearest-neighbor Kitaev exchange blocked by charge order in electron doped $\alpha$-RuCl$_{3}$

A quantum spin-liquid might be realized in $\alpha$-RuCl$_{3}$, a honeycomb-lattice magnetic material with substantial spin-orbit coupling. Moreover, $\alpha$-RuCl$_{3}$ is a Mott insulator, which implies the possibility that novel exotic phases occur upon doping. Here, we study the electronic structure of this material when intercalated with potassium by photoemission spectroscopy, electron energy loss spectroscopy, and density functional theory calculations. We obtain a stable stoichiometry at K$_{0.5}$RuCl$_3$. This gives rise to a peculiar charge disproportionation into formally Ru$^{2+}$ (4$d^6$) and Ru$^{3+}$ (4$d^5$). Every Ru 4$d^5$ site with one hole in the $t_{2g}$ shell is surrounded by nearest neighbors of 4$d^6$ character, where the $t_{2g}$ level is full and magnetically inert. Thus, each type of Ru sites forms a triangular lattice and nearest-neighbor interactions of the original honeycomb are blocked.

cond-mat.str-el↗

arXiv2016

J$_{eff}$ description of the honeycomb Mott insulator ${\alpha}$-RuCl$_3$

Novel ground states might be realized in honeycomb lattices with strong spin-orbit coupling. Here we study the electronic structure of ${\alpha}$-RuCl$_3$, in which the Ru ions are in a d5 configuration and form a honeycomb lattice, by angle-resolved photoemission, x-ray photoemission and electron energy loss spectroscopy supported by density functional theory and multiplet calculations. We find that ${\alpha}$-RuCl$_3$ is a Mott insulator with significant spin-orbit coupling, whose low energy electronic structure is naturally mapped onto Jeff states. This makes ${\alpha}$-RuCl$_3$ a promising candidate for the realization of Kitaev physics. Relevant electronic parameters such as the Hubbard energy U, the crystal field splitting 10Dq and the charge transfer energy are evaluated. Furthermore, we observe significant Cl photodesorption with time, which must be taken into account when interpreting photoemission and other surface sensitive experiments.

cond-mat.str-el↗

arXiv2012

Anisotropic electrical resistivity of LaFeAsO: evidence for electronic nematicity

Single crystals of LaFeAsO were successfully grown out of KI flux. Temperature dependent electrical resistivity was measured with current flow along the basal plane, ρ_perpend(T), as well as with current flow along the crystallographic c-axis, ρ_parallel(T), the latter one utilizing electron beam lithography and argon ion beam milling. The anisotropy ratio was found to lie between ρ_parallel/ρ_perpend = 20 - 200. The measurement of ρ_perpend(T) was performed with current flow along the tetragonal [1 0 0] direction and along the [1 1 0] direction and revealed a clear in-plane anisotropy already at T \leq 175 K. This is significantly above the orthorhombic distortion at T_0 = 147 K and indicates the formation of an electron nematic phase. Magnetic susceptibility and electrical resistivity give evidence for a change of the magnetic structure of the iron atoms from antiferromagnetic to ferromagnetic arrangement along the c-axis at T^\ast = 11 K.

cond-mat.supr-con↗

arXiv2012

Tetragonal to Orthorhombic Transition of GdFeAsO Studied by Single-Crystal Synchrotron X-Ray Diffraction

A study of the tetragonal to orthorhombic phase transition of GdFeAsO is presented. Planes of the reciprocal space were reconstructed form single-crystal synchrotron X-ray diffraction data. By cooling below the structural transition temperature splitting of the Bragg reflections was observed corresponding to four different twin domain orientations. A model was developed to quantify the distortion of the lattice from the position of the splitted reflections relative to each other. Constrained 2D-Cauchy fits of several splitted reflections provided positions of the reflections. The influence of the structural distortion was detectable already above the structural transition temperature hinting at fluctuations in the tetragonal phase.

cond-mat.supr-con↗

arXiv2010

Structural trends from a consistent set of single-crystal data of REFeAsO (RE = La, Ce, Pr, Nd, Sm, Gd, and Tb)

A new crystal growth technique for single-crystals of REFeAsO (RE = La, Ce, Pr, Nd, Sm, Gd, and Tb) using NaI/KI as flux is presented. Crystals with a size up to 300 $μ$m were isolated for single-crystal X-ray diffraction measurements. Lattice parameters were determined by LeBail fits of X-ray powder data against LaB6 standard. A consistent set of structural data is obtained and interpreted in a hard-sphere model. Effective radii for the rare-earth metal atoms for REFeAsO are deduced. The relation of the intra- and inter-plane distances of the arsenic atoms is identified as limiter of the phase formation, and its influence on Tc is discussed.

cond-mat.supr-con↗

arXiv2009

Magnetic and electrical transport anomalies in RMAs2 (R= Pr and Sm, M= Ag and Au)

The results of magnetization, heat-capacity, and electrical resistivity (rho) studies of the compounds, RMAs2 (R= Pr and Sm; M= Ag, Au), crystallizing in HfCuSi2-derived structure are reported. PrAgAs2 orders antiferromagnetically at T_N= 5 K. The Au analogue, however, does not exhibit long range magnetic order down to 1.8 K. We infer that this is due to subtle differences in their crystallographic features, particularly noting that both the Sm compounds with identical crystal structure as that of former order magnetically nearly at the same temperature (about 17 K). It appears that, in PrAgAs2, SmAgAs2, and SmAuAs2, there is an additional magnetic transition at a lower temperature, as though the similarity in the crystal structure results in similarities in magnetism as well. The rho for PrAgAs2 and PrAuAs2 exhibits negative temperature coefficient in some temperature range in the paramagnetic state. SmAuAs2 exhibits magnetic Brillouin-zone gap effect in rho at T_N, while SmAgAs2 shows a well-defined broad minimum well above T_N around 45 K. Thus, these compounds reveal interesting magnetic and transport properties.

cond-mat.str-el↗

arXiv2005

Magnetic behavior of EuCu2As2: Delicate balance between antiferromagnetic and ferromagnetic order

The Eu-based compound, EuCu2As2, crystallizing in the ThCr2Si2-type tetragonal structure, has been synthesized and its magnetic behavior has been investigated by magnetization (M), heat-capacity (C) and electrical resistivity (rho) measurements as a function of temperature (T) and magnetic field (H) as well as by 151Eu Moessbauer measurements. The results reveal that Eu is divalent ordering antiferromagnetically below 15 K in the absence of magnetic field, apparently with the formation of magnetic Brillouin-zone boundary gaps. A fascinating observation is made in a narrow temperature range before antiferromagnetism sets in: That is, there is a remarkable upturn just below 20 K in the plot of magnetic susceptibility versus T even at low fields, as though the compound actually tends to order ferromagnetically. There are corresponding anomalies in the magnetocaloric effect data as well. In addition, a small application of magnetic field (around 1 kOe at 1.8 K) in the antiferromagnetic state causes spin-reorientation effect. These results suggest that there is a close balance between antiferromagnetism and ferromagnetism in this compound

cond-mat.str-el↗

arXiv2004

Electrical resistivity and tunneling anomalies in CeCuAs2

The compound CeCuAs2 is found to exhibit negative temperature (T) coefficient of electrical resistivity (rho) under ambient pressure conditions in the entire T-range of investigation (45 mK to 300 K), even in the presence of high magnetic fields. Preliminary tunneling spectroscopic measurements indicate the existence of a psuedo-gap at least at low temperatures, thereby implying that this compound could be classified as a Kondo semi-conductor, though rho(T) interestingly is not found to be of an activated type.

cond-mat.str-el↗

arXiv2004

Magnetic, electrical resistivity, heat-capacity and thermopower anomalies in CeCuAs2

The results of magnetic susceptibility, electrical resistivity ($ρ$), heat-capacity (C) and thermopower (S) measurements on CeCuAs2, forming in ZrCuSi2-type tetragonal structure, are reported. Our investigations reveal that Ce is trivalent and there is no clear evidence for long range magnetic ordering down to 45 mK. The $ρ$ behavior is notable in the sense that (i) the temperature (T)-coefficient of $ρ$ is negative in the entire range of measurement (45 mK to 300 K) with large values of $ρ$, while S behavior is typical of metallic Kondo lattices, and (ii) $ρ$ is proportional to T-0.6 at low temperatures, without any influence on the exponent by the application of a magnetic field, which does not seem to classify this compound into hither-to-known non-Fermi liquid (NFL) systems. In contrast to the logarithmic increase known for NFL systems, C/T measured down to 0.5 K exhibits a fall below 2 K. The observed properties of this compound are unusual among Ce systems.

cond-mat.str-el↗

arXiv2004

Magnetic and transport anomalies in the compounds, RCuAs2 (R= Pr, Nd, Sm, Gd, Tb, Dy, Ho, and Er)

The results of dc magnetization, heat capacity, electrical resistivity (rho) and magnetoresistance measurements are reported in detail for the compounds, RCuAs2 for R= Pr, Nd, Sm, Gd, Tb, Dy, Ho, and Er, crystallizing in HfCuSi2-type tetragonal structure, with the aim of bringing out anomalies among 'normal' (that is, other than Ce and Yb) rare-earths. The results establish that all these compounds order antiferromagnetically at low temperatures with deviations from de Gennes scaling. Isothermal magnetization (M) data below respective Neel temperatures (TN) reveal the existence of field-induced metamagnetic-like transitions for most of the compounds (except R= Sm and Gd), whereas in Sm and Gd compounds M varies essentially linearly with magnetic field. With respect to the rho behavior, there appears to be a subtle difference in the temperature dependence beyond 50 K between Sm on the one hand and the rest on the other. In addition, the unexpected rho(T) minimum reported recently for R = Sm, Gd, Tb and Dy in the paramagnetic state (around 20 to 30 K) is essentially absent for R = Ho and Er. The results overall reveal that the normal rare-earths in this series present an interesting situation in magnetism, warranting a new theoretical approach to describe the transport behavior in the paramagnetic state particularly in the vicinity of TN.

cond-mat.mtrl-sci↗