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A. Jesche

Publications and source records attributed to A. Jesche.

At least 19 recordsLinked to original sources

Adiabatic demagnetization refrigeration with antiferromagnetically ordered NaGdP$_2$O$_7$

We present a comprehensive study of the structural, magnetic, and thermodynamic properties, as well as the adiabatic demagnetization refrigeration (ADR) performance of NaGdP$_2$O$_7$. Although NaGdP$_2$O$_7$ exhibits antiferromagnetic ordering at a N\'eel temperature of $T_{\rm N} = 570$ mK in zero field, ADR experiments achieved a minimum temperature of 220 mK starting from $T = 2$ K under an applied magnetic field of $\mu_0H = 5$ T. The warm-up time back to $T = 2$ K exceeds 60 hours, which is roughly 50 times longer than that of its Yb-based analogue, underscoring the potential of NaGdP$_2$O$_7$ as an efficient precooling stage in double-stage ADR systems. We show that NaGdP$_2$O$_7$ can be seen as a network of ferromagnetic spin chains with antiferromagnetic interchain couplings and also investigate the influence of antiferromagnetic ordering on the magnetic entropy. We find that the temperature dependence of the entropy plays a more dominant role than its magnetic field dependence in the magnetically ordered state.

cond-mat.str-el

Optical conductivity of the metallic pyrochlore iridate Pr$_2$Ir$_2$O$_7$: Influence of spin-orbit coupling and electronic correlations on the electronic structure

The synergy of strong spin-orbit coupling and electron-electron interactions gives rise to unconventional topological states, such as topological Mott insulator, Weyl semimetal, and quantum spin liquid. In this study, we have grown single crystals of the pyrochlore iridate Pr$_2$Ir$_2$O$_7$ and explored its magnetic, lattice dynamical, and electronic properties. While Raman spectroscopy data reveal six phonon modes confirming the cubic \textit{Fd$\bar{3}$m} crystal symmetry, dc magnetic susceptibility data show no anomalies and hence indicate the absence of magnetic phase transitions down to 2~K. Both temperature-dependent electric transport and optical conductivity data reveal the metallic character of Pr$_2$Ir$_2$O$_7$. The optical conductivity spectrum contains a mid-infrared absorption band, which becomes more pronounced with decreasing temperature due to spectral weight transfer from high to low energies. The presence of the mid-infrared band hints at the importance of correlation physics. The optical response furthermore suggests that Pr$_2$Ir$_2$O$_7$ is close to the Weyl semimetal phase.

cond-mat.str-el

Cooperative quantum tunneling of the magnetization in Fe-doped Li$_3$N

The spin-reversal in dilute Li$_2$(Li$_{1-x}$Fe$_{x}$)N with $x < 1$ % is dominated by resonant quantum tunneling of spatially well-separated states. We report on the effect of finite couplings between those states that give rise to cooperative, simultaneous quantum tunneling of two spins. This phenomenon, known as spin-spin cross relaxation, effectively elucidates the fine-structure observed in isothermal magnetization loops, a previously unresolved aspect. Temperature and field-dependent magnetization measurements were conducted over a range from T = 2 K to 300 K in applied fields of up to $\mu_0H$ = 7 T. Magnetic dipole fields are computed numerically. Our findings affirm the absence of stoichiometric defects in Li$_2$(Li$_{1-x}$Fe$_{x}$)N and underscore its exemplary suitability as a model system for investigating spin-reversal processes at the microscopic level. This is attributed to its comparatively simple crystal structure, the availability of large single crystals, elevated characteristic energies, and well-defined energy levels

cond-mat.str-el

Adiabatic demagnetization refrigeration to mK temperatures with the distorted square lattice magnet NaYbGeO$_{4}$

We report the synthesis, characterization, low-temperature magnetic, and thermodynamic measurements of the novel milli-Kelvin adiabatic demagnetization refrigeration (mK-ADR) candidate material NaYbGeO$_4$ which exhibits a distorted square lattice arrangement of YbO$_{6}$ magnetic units. Magnetization and specific heat indicate weakly interacting effective spin-1/2 moments below 10~K, with a Curie-Weiss temperature of only 15~mK, that can be polarized by magnetic fields of order 1~T. For the ADR performance test, we start the demagnetization from 5~T at a temperature of $\sim 2$~K and reach a minimum temperature of 150~mK at zero field. The warming curve indicates a sharp magnetic transition in the heat capacity at 210~mK, implying only weak magnetic frustration. The entropy density of $S_{\rm GS}\simeq 101$ mJ K$ ^{-1}$cm$^{-3}$ and hold time below 2~K of 220~min are competitive while the minimal temperature is higher compared to frustrated Ytterbium-oxide ADR materials studied under similar conditions.

cond-mat.str-el

Quantum disordered ground state in the spin-orbit coupled Jeff = 1/2 distorted honeycomb magnet BiYbGeO5

We delineate quantum magnetism in the strongly spin-orbit coupled, distorted honeycomb-lattice antiferromagnet BiYbGeO$_{5}$. Our magnetization and heat capacity measurements reveal that its low-temperature behavior is well described by an effective $J_{\rm eff}=1/2$ Kramers doublet of Yb$^{3+}$. The ground state is nonmagnetic with a tiny spin gap. Temperature-dependent magnetic susceptibility, magnetization isotherm, and heat capacity could be modeled well assuming isolated spin dimers with anisotropic exchange interactions $J_{\rm Z} \simeq 2.6$~K and $J_{\rm XY} \simeq 1.3$~K. Heat capacity measurements backed by muon spin relaxation suggest the absence of magnetic long-range order down to at least 80\,mK both in zero field and in applied fields. This sets BiYbGeO$_5$ apart from Yb$_2$Si$_2$O$_7$ with its unusual regime of magnon Bose-Einstein condensation and suggests negligible interdimer couplings, despite only a weak structural deformation of the honeycomb lattice.

cond-mat.str-el

Efficient adiabatic demagnetization refrigeration to below 50 mK with UHV compatible Ytterbium diphosphates $A$YbP$_2$O$_7$ ($A=$Na, K)

Attaining milli-Kelvin temperatures is often a prerequisite for the study of novel quantum phenomena and the operation of quantum devices. Adiabatic demagnetization refrigeration (ADR) is an effective, easy and sustainable alternative to evaporation or dilution cooling with the rare and super-expensive $^3$He. Paramagnetic salts, traditionally used for mK-ADR, suffer from chemical instability related to water of crystallization. We report synthesis, characterization as well as low-temperature magnetization and specific heat measurements of two new UHV compatible candidate materials NaYbP$_2$O$_7$ and KYbP$_2$O$_7$. Utilizing the PPMS at 2 K, the ADR of sintered pellets with Ag powder admixture starting at 5 T yields base temperatures (warm-up times) of 45 mK (55 min) and 37 mK (35 min) for NaYbP$_2$O$_7$ and KYbP$_2$O$_7$, respectively, slightly advantageous to KBaYb(BO$_3$)$_2$ (45 mK and 40 min) studied under similar conditions.

cond-mat.mtrl-sci

Adiabatic demagnetization cooling well below the magnetic ordering temperature in the triangular antiferromagnet KBaGd(BO3)2

Crystal structure, thermodynamic properties, and adiabatic demagnetization refrigeration (ADR) effect in the spin-7/2 triangular antiferromagnet KBaGd(BO3)2 are reported. With the average nearest-neighbor exchange coupling of 44 mK, this compound shows magnetic order below $T_N = 263$\,mK in zero field. The ADR tests reach the temperature of $T_{min} = 122$ mK, more than twice lower than $T_N$, along with the entropy storage capacity of 192 mJK$^{-1}$cm$^{-3}$ and the hold time of more than 8 hours in the PPMS setup, both significantly improved compared to the spin-1/2 Yb$^{3+}$ analog. We argue that KBaGd(BO3)2 shows a balanced interplay of exchange and dipolar couplings that together with structural randomness and geometrical frustration shift $T_{min}$ to well below the ordering temperature $T_N$, therefore facilitating the cooling.

cond-mat.str-el

Fluorite-related iridate Pr$_3$IrO$_7$: Crystal growth, structure, magnetism, thermodynamic, and optical properties

Spin-orbit coupling in heavy 5$d$ metal oxides, in particular, iridates have received tremendous interest in recent years due to the realization of exotic electronic and magnetic phases. Here, we report the synthesis, structural, magnetic, thermodynamic, and optical properties of the ternary iridate Pr$_3$IrO$_7$. Single crystals of Pr$_3$IrO$_7$ have been grown by the KF flux method. Structural analysis shows that Pr$_3$IrO$_7$ crystallizes in an orthorhombic phase with $Cmcm$ symmetry. The electron energy loss spectroscopy study indicates that Pr is in a 3+ valence state, which implies a 5+ oxidation state of Ir. Magnetization data measured at high and low magnetic fields do not exhibit any bifurcation between $M_{ZFC}$ and $M_{FC}$, however, a weak hump in $M(T)$ is observed at $T^*$$\sim$10.4~K. The specific heat data reveal two maxima at $\sim$253 K and $\sim$4.8 K. The optical conductivity $\sigma_1(\omega)$ spectrum shows 24 infrared-active phonon modes and reveals an insulating behavior with an optical gap $\Delta_{OP}$ of size $\sim$500~meV. During cooling down, the temperature-dependent reflectivity spectrum reveals eight extra phonon modes below the structural phase transition ($\sim$ 253 K). An anomaly is observed at around $T^*$ in the temperature evolution of infrared-active mode frequencies suggesting the presence of significant spin-phonon coupling in the system.

cond-mat.str-el

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

Li$_2$Sr[MnN]$_2$: a magnetically ordered, metallic nitride

Li$_2$Sr[MnN]$_2$ single crystals were successfully grown out of Li rich flux. The crystal structure was determined by single crystal X-ray diffraction and revealed almost linear $-$N$-$Mn$-$N$-$Mn$-$ chains as central structural motif. Tetragonal columns of this air and moisture sensitive nitridomanganate were employed for electrical transport, heat capacity, and anisotropic magnetization measurements. Both the electronic and magnetic properties are most remarkable, in particular the linear increase of the magnetic susceptibility with temperature that is reminiscent of underdoped cuprate and Fe-based superconductors. Clear indications for antiferromagnetic ordering at $T_{\rm N} = 290$ K were obtained. Metallic transport behavior is experimentally observed in accordance with electronic band structure calculations.

cond-mat.mtrl-sci

Angle-dependent thermodynamics of $\alpha$-RuCl$_3$

Thermodynamics of the Kitaev honeycomb magnet $\alpha$-RuCl$_3$ is studied for different directions of in-plane magnetic field using measurements of the magnetic Gr\"uneisen parameter $\Gamma_B$ 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 $\Gamma_B$ 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 $\alpha$-RuCl$_3$ in high magnetic fields and challenge the presence of a field-induced Kitaev spin liquid in this material.

cond-mat.str-el

Electron doping of the iron-arsenide superconductor CeFeAsO controlled by hydrostatic pressure

In the iron-pnictide material CeFeAsO not only the Fe moments, but also the local 4f moments of the Ce order antiferromagnetically at low temperatures. We elucidate on the peculiar role of the Ce on the emergence of superconductivity. While application of pressure suppresses the iron SDW ordering temperature monotonously up to 4 GPa, the Ce-4f magnetism is stabilized, until both types of magnetic orders disappear abruptly and a narrow SC dome develops. With further increasing pressure characteristics of a Kondo-lattice system become more and more apparent in the electrical resistivity. This suggests a connection of the emergence of superconductivity with the extinction of the magnetic order and the onset of Kondo-screening of the Ce-4f moments.

cond-mat.supr-con

Magnetic anisotropy and exchange paths for octa- and tetrahedrally coordinated Mn$^{2+}$ ions in the honeycomb multiferroic Mn$_2$Mo$_3$O$_8$

We investigated the static and dynamic magnetic properties of the polar ferrimagnet Mn$_2$Mo$_3$O$_8$ in three magnetically ordered phases via magnetization, magnetic torque, and THz absorption spectroscopy measurements. The observed magnetic field dependence of the spin-wave resonances, including Brillouin zone-center and zone-boundary excitations, magnetization, and torque, are well described by an extended two-sublattice antiferromagnetic classical mean-field model. In this orbitally quenched system, the competing weak easy-plane and easy-axis single-ion anisotropies of the two crystallographic sites are determined from the model and assigned to the tetra- and octahedral sites, respectively, by ab initio calculations.

cond-mat.str-el

Cooperative cluster-Jahn-Teller effect as a possible route to antiferroelectricity

We report the observation of an antipolar phase in cubic GaNb$_4$S$_8$ driven by an unconventional microscopic mechanism, the cooperative Jahn-Teller effect of Nb$_4$S$_4$ molecular clusters. The assignment of the antipolar nature is based on sudden changes in the crystal structure and a strong drop of the dielectric constant at $T_\mathrm{JT}=31$\,K, also indicating the first-order nature of the transition. In addition, we found that local symmetry lowering precedes long-range orbital ordering, implying the presence of a dynamic Jahn-Teller effect in the cubic phase above $T_\mathrm{JT}$. Based on the variety of structural polymorphs reported in lacunar spinels, also including ferroelectric phases, we argue that GaNb$_4$S$_8$ may be transformable to a ferroelectric state, which would further classify the observed antipolar phase as antiferrolectric.

cond-mat.str-el

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

Measurements of the magnetic Gr\"uneisen parameter ($\Gamma_B$) and specific heat on the Kitaev material candidate $\alpha$-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 $\Gamma_B$, 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 $\alpha$-RuCl$_3$. We show theoretically that at low temperatures $\Gamma_B$ 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-resolution resonant inelastic x-ray scattering study of the electron-phonon coupling in honeycomb $\alpha$-Li$_2$IrO$_3$

The excitations in honeycomb $\alpha$-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

Field evolution of low-energy excitations in the hyperhoneycomb magnet $\beta$-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 $\beta$-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 $\alpha$-RuCl$_3$ at zero applied magnetic field. At higher temperatures in $\beta$-Li$_2$IrO$_3$, $1/T_1$ passes through a broad maximum without any clear anomaly at the N\'eel 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 $\alpha$-RuCl$_3$ where an excitation continuum was reported.

cond-mat.str-el

Magnetic Field tuning of low energy spin dynamics in the single-atomic magnet Li$_2$(Li$_{1-x}$Fe$_x$)N

We present a systematic 57Fe-Moessbauer study on highly diluted Fe centers in Li2(Li1-xFex)N single-crystals as a function of temperature and magnetic field applied transverse and longitudinal with respect to the single-ion anisotropy axis. Below 30 K the Fe centers exhibit a giant magnetic hyperfine field of E_A = 70.25(2)T parallel to the axis of strongest electric field gradient Vzz = -154.0(1) V/A2. Fluctuations of the magnetic hyperfine field are observed between 50K and 300K and described by the Blume two-level relaxation model. From the temperature dependence of the uctuation rate an Orbach spin-lattice relaxation process is deduced. An Arrhenius analysis yields a single thermal activation barrier of E_A = 570(6)K and an attempt frequency nu_0 = 309(10) GHz. Moessbauer spectroscopy studies with applied transverse magnetic fields up to 5T reveal a large increase of the uctuation rate by more than one order of magnitude. In longitudinal magnetic fields a splitting of the uctuation rate into two branches is observed consistent with a Zeeman induced modifcation of the energy levels. The experimental observations are qualitatively reproduced by a single-ion effective spin Hamiltonian analysis assuming a Fe1+ d7 charge state with unquenched orbital moment and a J = 7=2 ground state. It is demonstrated that a weak axial single-ion anisotropy D of the order of a few Kelvin can cause a two orders of magnitude larger energy barrier for longitudinal spin fluctuations.

cond-mat.str-el