arXiv subjects

B. Büchner

Publications and source records attributed to B. Büchner.

At least 91 records · Page 5Linked to original sources

arXiv2019

Spin-glass state and reversed magnetic anisotropy induced by Cr doping in the Kitaev magnet $α$-RuCl$_3$

Magnetic properties of the substitution series Ru$_{1-x}$Cr$_x$Cl$_3$ were investigated to determine the evolution from the anisotropic Kitaev magnet $α$-RuCl$_3$ with $J_{\rm eff} = 1/2$ magnetic Ru$^{3+}$ ions to the isotropic Heisenberg magnet CrCl$_3$ with $S = 3/2$ magnetic Cr$^{3+}$ ions. Magnetization measurements on single crystals revealed a reversal of the magnetic anisotropy under doping, which we argue to arise from the competition between anisotropic Kitaev and off-diagonal interactions on the Ru-Ru links and approximately isotropic Cr-Ru and isotropic Cr-Cr interactions. In addition, combined magnetization, ac susceptibility and specific-heat measurements clearly show the destabilization of the long-range magnetic order of $α$-RuCl$_3$ in favor of a spin-glass state of Ru$_{1-x}$Cr$_x$Cl$_3$ for a low doping of $x\backsimeq0.1$. The corresponding freezing temperature as a function of Cr content shows a broad maximum around $x\backsimeq0.45$.

cond-mat.str-el↗

arXiv2019

Magnetic anisotropy and spin-polarized two-dimensional electron gas in the van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$

We report a comprehensive experimental investigation on the magnetic anisotropy in bulk single crystals of Cr$_2$Ge$_2$Te$_6$, a quasi-two-dimensional ferromagnet belonging to the family of magnetic layered transition metal trichalcogenides that have attracted recently a big deal of interest with regard to the fundamental and applied aspects of two-dimensional magnetism. For this purpose electron spin resonance (ESR) and ferromagnetic resonance (FMR) measurements have been carried out over a wide frequency and temperature range. A gradual change in the angular dependence of the ESR linewidth at temperatures above the ferromagnetic transition temperature $T_{\rm c}$ reveals the development of two-dimensional spin correlations in the vicinity of $T_{\rm c}$ thereby proving the intrinsically low-dimensional character of spin dynamics in Cr$_2$Ge$_2$Te$_6$. Angular and frequency dependent measurements in the ferromagnetic phase clearly show an easy-axis type anisotropy of this compound. Furthermore, these experiments are compared with simulations based on a phenomenological approach, which takes into account results of static magnetization measurements as well as high temperature $g$ factors obtained from ESR spectroscopy in the paramagnetic phase. As a result the determined magnetocrystalline anisotropy energy density (MAE) $K_U$ is $(0.48 \pm 0.02) \times10^6$ erg/cm$^3$. This analysis is complemented by density functional calculations which yield the experimental MAE value for a particular value of the electronic correlation strength $U$. The analysis of the electronic structure reveals that the low-lying conduction band carries almost completely spin-polarized, quasi-homogeneous, two-dimensional states.

cond-mat.str-el↗

arXiv2019

Emerging superconductivity with broken time reversal symmetry inside a superconducting $s$-wave state

In general, magnetism and superconductivity are antagonistic to each other. However, there are several families of superconductors, in which superconductivity may coexist with magnetism, and only a few examples are known, when superconductivity itself induces spontaneous magnetism. The most known compounds are Sr$_2$RuO$_4$ and some noncentrosymmetric superconductors. Here, we report the finding of a narrow dome of a novel $s+is'$ superconducting (SC) phase with broken time-reversal symmetry (BTRS) inside the broad $s$-wave SC region of the centrosymmetric multiband superconductor Ba$_{\rm 1-x}$K$_{\rm x}$Fe$_2$As$_2$ ($0.7 \lesssim x \lesssim 0.85$). We observe spontaneous magnetic fields inside this dome using the muon spin relaxation ($μ$SR) technique. Furthermore, our detailed specific heat study reveals that the BTRS dome appears very close to a change in the topology of the Fermi surface (Lifshitz transition). With this, we experimentally demonstrate the emergence of a novel quantum state due to topological changes of the electronic system.

cond-mat.supr-con↗

arXiv2019

Magnetic interactions and spin dynamics in the bond-disordered pyrochlore fluoride NaCaCo$_2$F$_7$

We report high-frequency/high-field electron spin resonance (ESR) and high-field magnetization studies on single crystals of the bond-disordered pyrochlore NaCaCo$_2$F$_7$. Frequency- and temperature-dependent ESR investigations above the freezing temperature $T_f \sim 2.4$ K reveal the coexistence of two distinct magnetic phases. A cooperative paramagnetic phase, evidenced by a gapless excitation mode, is found as well as a spin-glass phase developing below 20 K which is associated with a gapped low-energy excitation. Effective $g$-factors close to 2 are obtained for both modes in line with pulsed high-field magnetization measurements which show an unsaturated isotropic behavior up to 58 T at 2 K. In order to describe the field-dependent magnetization in high magnetic fields, we propose an empirical model accounting for highly anisotropic ionic $g$-tensors expected for this material and taking into account the strongly competing interactions between the spins which lead to a frustrated ground state. As a detailed quantitative relation between effective $g$-factors as determined from ESR and the local $g$-tensors obtained by neutron scattering [Ross et al., Phys. Rev. B 93, 014433 (2016)] is still sought after, our work motivates further theoretical investigations of the low-energy excitations in bond-disordered pyrochlores.

cond-mat.str-el↗

arXiv2019

Charge and nematic orders in AFe$_2$As$_2$ (A= Rb,Cs) superconductors

We discuss the results of $^{75}$As Nuclear Quadrupole Resonance (NQR) and muon spin relaxation measurements in AFe$_2$As$_2$ (A= Cs, Rb) iron-based superconductors. We demonstrate that the crossover detected in the nuclear spin-lattice relaxation rate $1/T_1$ (around 150 K in RbFe$_2$As$_2$ and around 75 K in CsFe$_2$As$_2$), from a high temperature nearly localized to a low temperature delocalized behaviour, is associated with the onset of an inhomogeneous local charge distribution causing the broadening or even the splitting of the NQR spectra as well as an increase in the muon spin relaxation rate. We argue that this crossover, occurring at temperatures well above the phase transition to the nematic long-range order, is associated with a charge disproportionation at the Fe sites induced by competing Hund's and Coulomb couplings. In RbFe$_2$As$_2$ around 35 K, far below that crossover temperature, we observe a peak in the NQR $1/T_1$ which is possibly associated with the critical slowing down of electronic nematic fluctuations on approaching the transition to the nematic long-range order.

cond-mat.str-el↗

arXiv2019

Yanson point-contact spectroscopy of Weyl semimetal WTe2

We carried out point contact (PC) investigation of WTe2 single crystals. We measured Yanson d2V/dI2 PC spectra of the electron-phonon interaction (EPI) in WTe2. The spectra demonstrate a main phonon peak around 8 meV and a shallow second maximum near 16 meV. Their position is in line with the calculation of the EPI spectra of WTe2 in the literature, albeit phonons with higher energy are not resolved in our PC spectra. An additional contribution to the spectra is present above the phonon energy, what may be connected with the peculiar electronic band structure and need to be clarified. We detected tiny superconducting features in d2V/dI2 close to zero bias, which broadens by increasing temperature and blurs above 6K. Thus, (surface) superconductivity may exist in WTe2 with a topologically nontrivial state. We found a broad maximum in dV/dI at large voltages (>200 mV) indicating change of conductivity from metallic to semiconducting type. The latter might be induced by the high current density (~10^8 A/cm^2) in the PC and/or local heating, thus enabling the manipulation of the quantum electronic states at the interface in the PC core.

cond-mat.mes-hall↗

arXiv2019

The magnetic phase diagram of the frustrated spin chain compound linarite, PbCuSO$_4$(OH)$_2$, as seen by neutron diffraction and $^1$H-NMR

We report on a detailed neutron diffraction and $^1$H-NMR study on the frustrated spin-1/2 chain material linarite, PbCuSO$_4$(OH)$_2$, where competing ferromagnetic nearest neighbor and antiferromagnetic next-nearest neighbor interactions lead to frustration. From the magnetic Bragg peak intensity studied down to 60 mK, the magnetic moment per Cu atom is obtained within the whole magnetic phase diagram for $H \parallel b$ axis. Further, we establish the detailed configurations of the shift of the SDW propagation vector in phase V with field and temperature. Finally, combining our neutron diffraction results with those from a low-temperature/high-field NMR study we find an even more complex phase diagram close to the quasi-saturation field suggesting that bound two-magnon excitations are the lowest energy excitations close to and in the quasi-saturation regime. Qualitatively and semi-quantitatively, we relate such behavior to $XYZ$ exchange anisotropy and contributions from the Dzyaloshinsky-Moriya interaction to affect the magnetic properties of linarite.

cond-mat.str-el↗

arXiv2018

Signatures of low-energy fractionalized excitations in $α$-RuCl$_3$ from field-dependent microwave absorption

Topologically ordered states of matter are generically characterized by excitations with quantum number fractionalization. A prime example is the spin liquid realized in Kitaev's honeycomb-lattice compass model where spin-flip excitations fractionalize into Majorana fermions and Ising gauge fluxes. While numerous compounds have been proposed to be proximate to such a spin-liquid phase, clear-cut evidence for fractionalized excitations is lacking. Here we employ microwave absorption measurements to study the low-energy excitations in $α$-RuCl$_3$ over a wide range of frequencies, magnetic fields, and temperatures, covering in particular the vicinity of the field-driven quantum phase transition where long-range magnetic order disappears. In addition to conventional gapped magnon modes we find a highly unusual broad continuum characteristic of fractionalization which -- most remarkably -- extends to energies below the lowest sharp mode and to temperatures significantly higher than the ordering temperature, and develops a gap of a nontrivial origin in strong magnetic fields. Our results unravel the signatures of fractionalized excitations in $α$-RuCl$_3$ and pave the way to a more complete understanding of the Kitaev spin liquid and its instabilities.

cond-mat.str-el↗

arXiv2018

Spectral field mapping in plasmonic nanostructures with nanometer resolution

Plasmonic nanostructures and devices are rapidly transforming light manipulation technology by allowing to modify and enhance optical fields on sub-wavelength scales. Advances in this field rely heavily on the development of new characterization methods for the fundamental nanoscale interactions. However, the direct and quantitative mapping of transient electric and magnetic fields characterizing the plasmonic coupling has been proven elusive to date. Here we demonstrate how to directly measure the inelastic momentum transfer of surface plasmon modes via the energy-loss filtered deflection of a focused electron beam in a transmission electron microscope. By scanning the beam over the sample we obtain a spatially and spectrally resolved deflection map and we further show how this deflection is related quantitatively to the spectral component of the induced electric and magnetic fields pertaining to the mode. In some regards this technique is an extension to the established differential phase contrast into the dynamic regime.

physics.optics↗

arXiv2018

Orbiton-Phonon coupling in Ir5+(5d4) double perovskite Ba2YIrO6

Ba2YIrO6, a Mott insulator, with four valence electrons in Ir5+ d-shell (5d4) is supposed to be non-magnetic, with Jeff = 0, within the atomic physics picture. However, recent suggestions of non-zero magnetism have raised some fundamental questions about its origin. Focussing on the phonon dynamics, probed via Raman scattering, as a function of temperature and different incident photon energies, as an external perturbation. Our studies reveal strong renormalization of the phonon self-energy parameters and integrated intensity for first-order modes, especially redshift of the few first-order modes with decreasing temperature and anomalous softening of modes associated with IrO6 octahedra, as well as high energy Raman bands attributed to the strong anharmonic phonons and coupling with orbital excitations. The distinct renormalization of second-order Raman bands with respect to their first-order counterpart suggest that higher energy Raman bands have significant contribution from orbital excitations. Our observation indicates that strong anharmonic phonons coupled with electronic/orbital degrees of freedom provides a knob for tuning the conventional electronic levels for 5d-orbitals, and this may give rise to non-zero magnetism as postulated in recent theoretical calculations with rich magnetic phases.

cond-mat.str-el↗

arXiv2018

Increasing the performance of the superconducting spin valve using a Heusler alloy

We have studied superconducting properties of the spin-valve thin layer heterostructures CoO$_x$/F1/Cu/F2/Cu/Pb where the ferromagnetic F1 layer was standardly made of Permalloy whereas for the F2 layer we have taken a specially prepared film of the Heusler alloy Co$_2$Cr$_{1-x}$Fe$_x$Al with a small degree of spin polarization of the conduction band. The heterostructures demonstrate a significant superconducting spin-valve effect, i.e. a complete switching on and off of the superconducting current flowing through the system by manipulating the mutual orientations of the magnetization of the F1 and F2 layers. The magnitude of the effect is doubled in comparison with the previously studied analogous multilayers with the F2 layer made of the strong ferromagnet Fe. Theoretical analysis shows that a drastic enhancement of the switching effect is due to a smaller exchange field in the heterostructure coming from the Heusler film as compared to Fe. This enables to approach almost ideal theoretical magnitude of the switching in the Heusler-based multilayer with the F2 layer thickness of $\sim 1$\,nm.

cond-mat.supr-con↗

arXiv2018

Massive Dirac fermions in layered BaZnBi$_2$

Using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) we study the electronic structure of layered BaZnBi$_2$. Our experimental results show no evidence of Dirac states in BaZnBi$_2$ originated either from the bulk or the surface. The calculated band structure without spin-orbit interaction shows several linear dispersive band crossing points throughout the Brillouin zone. However, as soon as the spin-orbit interaction is turned on, the band crossing points are significantly gapped out. The experimental observations are in good agreement with our DFT calculations. These observations suggest that the Dirac fermions in BaZnBi$_2$ are trivial and massive. We also observe experimentally that the electronic structure of BaZnBi$_2$ comprises of several linear dispersive bands in the vicinity of Fermi level dispersing to a wider range of binding energy.

cond-mat.mtrl-sci↗

arXiv2018

Surface superconductivity in the Weyl semimetal MoTe2 detected by point contact spectroscopy

MoTe2 is a Weyl semimetal, which exhibits unique non-saturating magnetoresistance and strongly reinforced superconductivity under pressure. Here, we demonstrate that a novel mesoscopic superconductivity at ambient pressure arises on the surface of MoTe2 with a critical temperature up to 5 K significantly exceeding the bulk Tc=0.1K. We measured the derivatives of I-V curves for metallic hetero-contacts of MoTe2 with Ag or Cu, homo-contacts of MoTe2 as well as "soft" point contacts (PCs). Large number of these hetero-contacts exhibit a dV/dI dependence, which is characteristic for Andreev reflection. It allows to determine the superconducting gap Δ. The average gap values are 2Δ=1.30+/-0.15 meV with a 2Δ/kBTc ratio of 3.7+/-0.4, which slightly exceeds the standard BCS value of 3.52. Furthermore, the temperature dependence of the gap follows a BCS-like behavior, which points to a nodeless superconducting order parameter with some strong-coupling renormalization. Remarkably, the observation of a "gapless-like" single minimum in the dV/dI of "soft" PCs may indicate a topological superconducting state of the MoTe2 surface as these contacts probe mainly the interface and avoid additional pressure effect. Therefore, MoTe2 might be a suitable material to study new forms of topological superconductivity.

cond-mat.supr-con↗

arXiv2018

Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet alpha-RuCl3

Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material alpha-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p=0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin liquid phase in alpha-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.

cond-mat.str-el↗

arXiv2018

Unraveling the nature of magnetism of the 5$\boldsymbol{d^4}$ double perovskite Ba$_2$YIrO$_6$

We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba$_2$YIrO$_6$. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir$^{5+}$ (5$d^4$) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5$d^4$ iridates and the emergence of a novel exotic magnetic state. Our data evidence that the magnetism of the studied material is solely due to a few percent of Ir$^{4+}$ and Ir$^{6+}$ magnetic defects while the regular Ir$^{5+}$ sites remain nonmagnetic. Remarkably, the defect Ir$^{6+}$ species manifest magnetic correlations in the ESR spectra at $T\lesssim 20$ K suggesting a long-range character of superexchange in the double prevoskites as proposed by recent theories.

cond-mat.str-el↗

arXiv2018

Tuning the interplay between nematicity and spin fluctuations in Na$_{1-x}$Li$_x$FeAs superconductors

Strong interplay of spin and charge/orbital degrees of freedom is the fundamental characteristic of the iron-based superconductors (FeSCs), which leads to the emergence of a nematic state as a rule in the vicinity of the antiferromagnetic state. Despite intense debate for many years, however, whether nematicity is driven by spin or orbital fluctuations remains unsettled. Here, by use of transport, magnetization, and $^{75}$As nuclear magnetic resonance (NMR) measurements, we show a striking transformation of the relationship between nematicity and spin fluctuations (SFs) in Na$_{1-x}$Li$_x$FeAs; For $x\leq 0.02$, the nematic transition promotes SFs. In contrast, for $x\geq 0.03$, the system undergoes a non-magnetic phase transition at a temperature $T_0$ into a distinct nematic state that suppresses SFs. Such a drastic change of the spin fluctuation spectrum associated with nematicity by small doping is highly unusual, and provides insights into the origin and nature of nematicity in FeSCs.

cond-mat.str-el↗

arXiv2018

Nematicity and magnetism in LaFeAsO single crystals probed by $^{75}$As nuclear magnetic resonance

We report a $^{75}$As nuclear magnetic resonance study in LaFeAsO single crystals, which undergoes nematic and antiferromagnetic transitions at $T_\text{nem}\sim 156$ K and $T_N \sim 138$ K, respectively. Below $T_\text{nem}$, the $^{75}$As spectrum splits sharply into two for an external magnetic field parallel to the orthorhombic $a$ or $b$ axis in the FeAs planes. Our analysis of the data demonstrates that the NMR line splitting arises from an electronically driven rotational symmetry breaking. The $^{75}$As spin-lattice relaxation rate as a function of temperature shows that spin fluctuations are strongly enhanced just below $T_\text{nem}$. These NMR findings indicate that nematic order promotes spin fluctuations in magnetically ordered LaFeAsO, as observed in non-magnetic and superconducting FeSe. We conclude that the origin of nematicity is identical in both FeSe and LaFeAsO regardless of whether or not a long range magnetic order develops in the nematic state.

cond-mat.str-el↗

arXiv2018

An ultra-high vacuum scanning tunneling microscope operating at sub-Kelvin temperatures and high magnetic fields for spin-resolved measurements

We present the construction and performance of an ultra-low temperature scanning tunneling microscope (STM), working in ultra-high vacuum conditions (UHV) and in high magnetic fields up to 9 T. The cryogenic environment of the STM is generated by a single shot $^3$He magnet cryostat in combination with a $^4$He dewar system. At base temperature (300~mK), the cryostat has an operation time of approximately 80 hours. The special design of the microscope allows the transfer of the STM head from the cryostat to a UHV-chamber system, where samples and STM-tips can be easily exchanged. The UHV chambers are equipped with specific surface science treatment tools for the functionalization of samples and tips, including high-temperature treatments and thin film deposition. This, particularly, enables spin-resolved tunneling measurements. We present test measurements using well known samples and tips based on superconductor and metallic materials such as LiFeAs, Nb, Fe and W, respectively. The measurements demonstrate the outstanding performance of the STM with high spatial and energy resolution as well as the spin-resolved capability.

cond-mat.str-el↗