arXiv subjects

P. Gegenwart

Publications and source records attributed to P. Gegenwart.

At least 37 records · Page 2Linked to original sources

arXiv2021

Frustrated magnet for adiabatic demagnetization cooling to milli-Kelvin temperatures

Generation of very low temperatures has been crucially important for applications and fundamental research, as low-temperature quantum coherence enables operation of quantum computers and formation of exotic quantum states, such as superfluidity and superconductivity. One of the major techniques to reach milli-Kelvin temperatures is adiabatic demagnetization refrigeration (ADR). This method uses almost non-interacting magnetic moments of paramagnetic salts where large distances suppress interactions between the magnetic ions. The large spatial separations are facilitated by water molecules, with a drawback of reduced stability of the material. Here, we show that an H$_2$O-free frustrated magnet KBaYb(BO$_3$)$_2$ can be ideal refrigerant for ADR, achieving at least 22\,mK upon demagnetization under adiabatic conditions. Compared to conventional refrigerants, KBaYb(BO$_3)_2$ does not degrade even under high temperatures and ultra-high vacuum conditions. Further, its frustrated magnetic network and structural randomness enable cooling to temperatures several times lower than the energy scale of magnetic interactions, which is the main limiting factor for the base temperature of conventional refrigerants.

cond-mat.str-el↗

arXiv2021

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↗

arXiv2020

Topological magnetic order and superconductivity in EuRbFe$_4$As$_4$

We study single crystals of the magnetic superconductor EuRbFe$_4$As$_4$ by magnetization, electron spin resonance (ESR), angle-resolved photoemission spectroscopy (ARPES) and electrical resistance in pulsed magnetic fields up to 630 kOe. The superconducting state below 36.5 K is almost isotropic and only weakly affected by the development of Eu$^{2+}$ magnetic order at 15 K. On the other hand, for the external magnetic field applied along the c-axis the temperature dependence of the ESR linewidth reveals a Berezinskii-Kosterlitz-Thouless topological transition below 15 K. This indicates that Eu$^{2+}$-planes are a good realization of a two-dimensional XY-magnet, which reflects the decoupling of the Eu$^{2+}$ magnetic moments from superconducting FeAs-layers.

cond-mat.supr-con↗

arXiv2020

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↗

arXiv2020

Field evolution of low-energy excitations in the hyperhoneycomb magnet $β$-Li$_2$IrO$_3$

$^7$Li nuclear magnetic resonance (NMR) and terahertz (THz) spectroscopies are used to probe magnetic excitations and their field dependence in the hyperhoneycomb Kitaev magnet $β$-Li$_2$IrO$_3$. Spin-lattice relaxation rate ($1/T_1$) measured down to 100\,mK indicates gapless nature of the excitations at low fields (below $H_c\simeq 2.8$\,T), in contrast to the gapped magnon excitations found in the honeycomb Kitaev magnet $α$-RuCl$_3$ at zero applied magnetic field. At higher temperatures in $β$-Li$_2$IrO$_3$, $1/T_1$ passes through a broad maximum without any clear anomaly at the Néel temperature $T_N\simeq 38$\,K, suggesting the abundance of low-energy excitations that are indeed observed as two peaks in the THz spectra, both correspond to zone-center magnon excitations. At higher fields (above $H_c$), an excitation gap opens, and a re-distribution of the THz spectral weight is observed without any indication of an excitation continuum, in contrast to $α$-RuCl$_3$ where an excitation continuum was reported.

cond-mat.str-el↗

arXiv2020

Reply to the Comment by S. Wirth et al. on "Tuning low-energy scales in YbRh$_2$Si$_2$ by non-isoelectronic substitution and pressure"

Previously, we reported that the doping and pressure dependence of the $T^\ast(B)$ crossover in YbRh$_2$Si$_2$ is incompatible with its interpretation as signature of a Kondo breakdown [M.-H. Schubert et al., Phys. Rev. Research 1, 032004(R) (2019)]. The comment by S. Wirth et al. [arXiv:1910.04108] refers to Hall measurements on undoped YbRh$_2$Si$_2$ and criticizes our study as incomplete and inconclusive. We thoroughly inspect these data and rebut the arguments of the comment.

cond-mat.str-el↗

arXiv2020

Epitaxial growth and orientation-dependent anomalous Hall effect of noncollinear antiferromagnetic Mn$_3$Ni$_{0.35}$Cu$_{0.65}$N films

We report the growth of noncollinear antiferromagnetic (AFM) Mn$_3$Ni$_{0.35}$Cu$_{0.65}$N films and the orientation-dependent anomalous Hall effect (AHE) of (001) and (111) films due to nonzero Berry curvature. We found that post-annealing at 500$^\circ$C can significantly improve the AHE signals, though using the appropriate post-annealing conditions is important. The AHE and magnetization loops show sharp flipping at the coercive field in (111) films, while (001) films are hard to saturate by a magnetic field. The anomalous Hall conductivity of (111) films is an order of magnitude larger than that of (001) films. The present results provide not only a better understanding of the AHE in Mn$_3X$N systems but also further opportunities to study the unique phenomena related to noncollinear AFM.

cond-mat.mtrl-sci↗

arXiv2019

High-resolution resonant inelastic x-ray scattering study of the electron-phonon coupling in honeycomb $α$-Li$_2$IrO$_3$

The excitations in honeycomb $α$-Li$_2$IrO$_3$ have been investigated with high-resolution resonant inelastic x-ray scattering (RIXS) at the O K edge. The low-energy response is dominated by a fully resolved ladder of excitations, which we interpret as being due to multi-phonon processes in the presence of strong electron-phonon coupling (EPC). At higher energies, the orbital excitations are shown to be dressed by phonons. The high quality of the data permits a quantitative test of the analytical model for the RIXS cross-section, which has been proposed to describe EPC in transition metal oxides (TMOs). We find that the magnitude of the EPC is comparable to that found for a range of 3d TMOs. This indicates that EPC may be of equal importance in determining the phenomenology displayed by corresponding 5d based systems.

cond-mat.str-el↗

arXiv2019

Tuning low-energy scales in YbRh$_2$Si$_2$ by non-isoelectronic substitution and pressure

The heavy-fermion metal YbRh$_2$Si$_2$ realizes a field-induced quantum critical point with multiple vanishing energy scales $T_{\rm N}(B)$ and $T^\ast(B)$. We investigate their change with partial non-isoelectronic substitutions, chemical and hydrostatic pressure. Low-temperature electrical resistivity, specific heat and magnetic susceptibility of Yb(Rh$_{1-x}$T$_x$)$_2$Si$_2$ with T=Fe or Ni for $x\leq 0.1$, magnetic fields $B\leq 0.3$~T (applied perpendicular to the c-axis) and hydrostatic pressure $p\leq 1.5$~GPa are reported. The data allow to disentangle the combined influences of hydrostatic and chemical pressure, as well as non-isoelectronic substitution. In contrast to Ni- and Co-substitution, which enhance magnetic order, Fe-substitution acts oppositely. For $x=0.1$ it also completely suppresses the $T^\ast$ crossover and eliminates ferromagnetic fluctuations. The pressure, magnetic field and temperature dependences of $T^\ast$ are incompatible with its interpretation as Kondo breakdown signature.

cond-mat.str-el↗

arXiv2019

Anisotropic temperature-field phase diagram of single-crystalline $β$-Li$_2$IrO$_3$: magnetization, specific heat, and $^7$Li NMR study

Detailed magnetization, specific heat, and $^7$Li nuclear magnetic resonance (NMR) measurements on single crystals of the hyperhoneycomb Kitaev magnet $β$-Li$_2$IrO$_3$ are reported. At high temperatures, {\cred anisotropy of the magnetization is reflected by the different Curie-Weiss temperatures for different field directions}, in agreement with the combination of a ferromagnetic Kitaev interaction ($K$) and a negative off-diagonal anisotropy ($Γ$) as two leading terms in the spin Hamiltonian. At low temperatures, magnetic fields applied along $a$ or $c$ have only a weak effect on the system and reduce the Néel temperature from 38 K at 0 T to about 35.5 K at 14 T, with no field-induced transitions observed up to 58 T on a powder sample. In contrast, the field applied along $b$ causes a drastic reduction in the $T_N$ that vanishes around $H_c=2.8$ T giving way to a crossover toward a quantum paramagnetic state. $^7$Li NMR measurements in this field-induced state reveal a gradual line broadening and a continuous evolution of the line shift with temperature, suggesting the development of local magnetic fields. The spin-lattice relaxation rate shows a peak around the crossover temperature 40 K and follows power-law behavior below this temperature.

cond-mat.str-el↗

arXiv2019

Fingerprints of Kitaev physics in the magnetic excitations of honeycomb iridates

In the quest for realizations of quantum spin liquids, the exploration of Kitaev materials - spin-orbit entangled Mott insulators with strong bond-directional exchanges - has taken center stage. However, in these materials the local spin-orbital j=1/2 moments typically show long-range magnetic order at low temperature, thus defying the formation of a spin-liquid ground state. Using resonant inelastic x-ray scattering (RIXS), we here report on a proximate spin liquid regime with clear fingerprints of Kitaev physics in the magnetic excitations of the honeycomb iridates alpha-Li2IrO3 and Na2IrO3. We observe a broad continuum of magnetic excitations that persists up to at least 300K, more than an order of magnitude larger than the magnetic ordering temperatures. We prove the magnetic character of this continuum by an analysis of the resonance behavior. RIXS measurements of the dynamical structure factor for energies within the continuum show that dynamical spin-spin correlations are restricted to nearest neighbors. Notably, these spectroscopic observations are also present in the magnetically ordered state for excitation energies above the conventional magnon excitations. Phenomenologically, our data agree with inelastic neutron scattering results on the related honeycomb compound RuCl3, establishing a common ground for a proximate Kitaev spin-liquid regime in these materials.

cond-mat.str-el↗

arXiv2019

Optical signature of the pressure-induced dimerization in the honeycomb iridate $α$-Li$_2$IrO$_3$

We studied the effect of external pressure on the electrodynamic properties of $α$-Li$_2$IrO$_3$ single crystals in the frequency range of the phonon modes and the Ir $d$-$d$ transitions. The abrupt hardening of several phonon modes under pressure supports the onset of the dimerized phase at the critical pressure $P_c$=3.8 GPa. With increasing pressure an overall decrease in spectral weight of the Ir $d$-$d$ transitions is found up to $P_c$. Above $P_c$, the local (on-site) $d$-$d$ excitations gain spectral weight with increasing pressure, which hints at a pressure-induced increase in the octahedral distortions. The non-local (intersite) Ir $d$-$d$ transitions show a monotonic blue-shift and decrease in spectral weight. The changes observed for the non-local excitations are most prominent well above $P_c$, namely for pressures $\geq$12 GPa, and only small changes occur for pressures close to $P_c$. The profile of the optical conductivity at high pressures ($\sim$20 GPa) appears to be indicative for the dimerized state in iridates.

cond-mat.str-el↗

arXiv2019

Pressure-induced formation of rhodium zigzag chains in the honeycomb rhodate Li$_2$RhO$_3$

We use powder x-ray diffraction to study the effect of pressure on the crystal structure of the honeycomb rhodate Li$_2$RhO$_3$. We observe low-pressure ($P$$<$$P_{c1}$ = 6.5 GPa) and high-pressure ($P$$>$$P_{c2}$ = 14 GPa) regions corresponding to the monoclinic $C2/m$ symmetry, while a phase mixture is observed at intermediate pressures. At $P$$>$$P_{c2}$, the honeycomb structure becomes distorted and features short Rh--Rh bonds forming zigzag chains stretched along the crystallographic $a$ direction. This is in contrast to dimerized patterns observed in triclinic high-pressure polymorphs of $α$-Li$_2$IrO$_3$ and $α$-RuCl$_3$. Density-functional theory calculations at various pressure conditions reveal that the observed rhodium zigzag-chain pattern is not expected under hydrostatic pressure but can be reproduced by assuming anisotropic pressure conditions.

cond-mat.str-el↗

arXiv2019

Anisotropic exchange Hamiltonian, magnetic phase diagram and domain inversion of Nd$_2$Zr$_2$O$_7$

We present thermodynamic and neutron scattering measurements on the quantum spin ice candidate Nd$_2$Zr$_2$O$_7$. The parameterization of the anisotropic exchange Hamiltonian is refined based on high-energy-resolution inelastic neutron scattering data together with thermodynamic data using linear spin wave theory and numerical linked cluster expansion. Magnetic phase diagrams are calculated using classical Monte Carlo simulations with fields along \mbox{[100]}, \mbox{[110]} and \mbox{[111]} crystallographic directions which agree qualitatively with the experiment. Large hysteresis and irreversibility for \mbox{[111]} is reproduced and the microscopic mechanism is revealed by mean field calculations to be the existence of metastable states and domain inversion. Our results shed light on the explanations of the recently observed dynamical kagome ice in Nd$_2$Zr$_2$O$_7$ in \mbox{[111]} fields.

cond-mat.mtrl-sci↗

arXiv2019

Structural, thermodynamic, and local probe investigations of a honeycomb material Ag$_{3}$LiMn$_{2}$O$_{6}$

The system Ag[Li$_{1/3}$Mn$_{2/3}$]O$_{2}$ belongs to a quaternary 3R-delafossite family and crystallizes in a monoclinic symmetry with space group $C\,2/m$ and the magnetic Mn$^{4+}$($S=3/2$) ions form a honeycomb network in the $ab$-plane. An anomaly around 50 K and the presence of antiferromagnetic (AFM) coupling (Curie-Weiss temperature $θ_{CW}\sim-51$ K) were inferred from our magnetic susceptibility data. The magnetic specific heat clearly manifests the onset of magnetic ordering in the vicinity of 48\,K and the recovered magnetic entropy, above the ordering temperature, falls short of the expected value, implying the presence of short-range magnetic correlations. The (ESR) line broadening on approaching the ordering temperature $T_{\rm N}$ could be described in terms of a Berezinski-Kosterlitz-Thouless (BKT) scenario with $T_{\rm KT}=40(1)$ K. $^{7}$Li NMR line-shift probed as a function of temperature tracks the static susceptibility (K$_{iso}$) of magnetically coupled Mn$^{4+}$ ions. The $^{7}$Li spin-lattice relaxation rate (1/$T$$_{1}$) exhibits a sharp decrease below about 50 K. Combining our bulk and local probe measurements, we establish the presence of an ordered ground state for the honeycomb system Ag$_{3}$LiMn$_{2}$O$_{6}$.Our ab-initio electronic structure calculations suggest that in the $ab$-plane, the nearest neighbor (NN) exchange interaction is strong and AFM, while the next NN and the third NN exchange interactions are FM and AFM respectively. In the absence of any frustration the system is expected to exhibit long-range, AFM order, in agreement with experiment.

cond-mat.str-el↗

arXiv2019

Anomalous Hall effect in non-collinear antiferromagnetic antiperovskite Mn$_{3}$Ni$_{1-x}$Cu$_{x}$N

We report the anomalous Hall effect (AHE) in antiperovskite Mn$_{3}$NiN with substantial doping of Cu on the Ni site (i.e. Mn$_{3}$Ni$_{1-x}$Cu$_{x}$N), which stabilizes a noncollinear antiferromagnetic (AFM) order compatible with the AHE. Observed on both sintered polycrystalline pieces and single crystalline films, the AHE does not scale with the net magnetization, contrary to the conventional ferromagnetic case. The existence of the AHE is explained through symmetry analysis based on the $Γ_{\rm 4g}$ AFM order in Cu doped Mn$_{3}$NiN. DFT calculations of the intrinsic contribution to the AHE reveal the non-vanishing Berry curvature in momentum space due to the noncollinear magnetic order. Combined with other attractive properties, antiperovskite Mn$_{3}$AN system offers great potential in AFM spintronics.

cond-mat.str-el↗

arXiv2019

Unconventional magnetism in the 4d$^{4}$ based ($S=1$) honeycomb system Ag$_{3}$LiRu$_{2}$O$_{6}$

We have investigated the thermodynamic and local magnetic properties of the Mott insulating system Ag$_{3}$LiRu$_{2}$O$_{6}$ containing Ru$^{4+}$ (4$d$$^{4}$) for novel magnetism. The material crystallizes in a monoclinic $C2/m$ structure with RuO$_{6}$ octahedra forming an edge-shared two-dimensional honeycomb lattice with limited stacking order along the $c$-direction. The large negative Curie-Weiss temperature ($θ_{CW}$ = -57 K) suggests antiferromagnetic interactions among Ru$^{4+}$ ions though magnetic susceptibility and heat capacity show no indication of magnetic long-range order down to 1.8 K and 0.4 K, respectively. $^{7}$Li nuclear magnetic resonance (NMR) shift follows the bulk susceptibility between 120-300 K and levels off below 120 K. Together with a power-law behavior in the temperature dependent spin-lattice relaxation rate between 0.2 and 2 K, it suggest dynamic spin correlations with gapless excitations. Electronic structure calculations suggest an $S = 1$ description of the Ru-moments and the possible importance of further neighbour interactions as also bi-quadratic and ring-exchange terms in determining the magnetic properties. Analysis of our $μ$SR data indicates spin freezing below 5 K but the spins remain on the borderline between static and dynamic magnetism even at 20 mK.

cond-mat.str-el↗

arXiv2019

Highly anisotropic strain dependencies in PrIr$_2$Zn$_{20}$

We report thermal expansion and magnetostriction of the cubic non-Kramers system PrIr$_2$Zn$_{20}$ with a non-magnetic $\varGamma_{3}$ ground state doublet. In previous experiments, antiferroquadrupolar order at \hbox{$T_{\mathrm{Q}}=0.11$\,K} and a Fermi liquid state around $B_{\mathrm{c}}\approx5$\,T for \hbox{$\boldsymbol{B}\parallel[001]$}, indicative of possible ferrohastatic order, were discovered. For magnetic fields \hbox{$\boldsymbol{B}\parallel[001]$}, the low temperature longitudinal and transverse thermal expansion and magnetostriction are highly anisotropic. The resulting volume strain is very small, indicating that the Pr valence remains nearly constant as a function of magnetic field. We conclude that the Fermi liquid state around $B_{\mathrm{c}}$ forms through a very little change in c-f hybridization. This result is in sharp contrast to Ce- and Yb-based Kramers Kondo lattices which show significantly larger volume strains due to the high sensitivity of the Kondo temperature to hydrostatic pressure.

cond-mat.str-el↗