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M. Frontzek

Publications and source records attributed to M. Frontzek.

At least 19 recordsLinked to original sources
arXiv2022

Strongly-overdoped La$_{2-x}$Sr$_x$CuO$_4$: Evidence for Josephson-coupled grains of strongly-correlated superconductor

The interpretation of how superconductivity disappears in cuprates at large hole doping has been controversial. To address this issue, we present an experimental study of single-crystal and thin film samples of La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) with $x\ge0.25$. In particular, measurements of bulk susceptibility on LSCO crystals with $x=0.25$ indicate an onset of diamagnetism at $T_{c1}=38.5$ K, with a sharp transition to a phase with full bulk shielding at $T_{c2}=18$ K, independent of field direction. Strikingly, the in-plane resistivity only goes to zero at $T_{c2}$. Inelastic neutron scattering on $x=0.25$ crystals confirms the presence of low-energy incommensurate magnetic excitations with reduced strength compared to lower doping levels. The ratio of the spin gap to $T_{c2}$ is anomalously large. Our results are consistent with a theoretical prediction for strongly overdoped cuprates by Spivak, Oreto, and Kivelson, in which superconductivity initially develops within disconnected self-organized grains characterized by a reduced hole concentration, with bulk superconductivity occurring only after superconductivity is induced by proximity effect in the surrounding medium of higher hole concentration. Beyond the superconducting-to-metal transition, local differential conductance measurements on an LSCO thin film suggest that regions with pairing correlations survive, but are too dilute to support superconducting order. Future experiments will be needed to test the degree to which these results apply to overdoped cuprates in general.

cond-mat.supr-con↗
arXiv2021

Magnetoelastic Coupling and Phases in the Skyrmion Lattice Magnet Gd2PdSi3 Discovered by High-resolution Dilatometry

We report detailed thermodynamic studies on high-quality single crystals of the centrosymmetric skyrmion-hosting intermetallic Gd2PdSi3 by means of high-resolution capacitance dilatometry in fields up to 15 T which are complemented by specific heat and magnetization studies. Our dilatometric measurements show magnetoelastic effects associated with antiferromagnetic order at TN1 = 22.3 K and TN2 = 19.7 K, as well as strong field effects in an applied magnetic field of 15 Tup to 200 K (150 K) for B||c (B||a*, i.e. B perp c). The data allow us to complete the magneticphase diagram, including a new feature at T* approx 12 K below which a new degree of freedom becomesrelevant. For the first time, the magnetic B vs. T phase diagram for the a*-axis is also reported. Gr\"uneisen analysis shows the onset of magnetic contributions around 60 K, i.e., well above TN1. Uniaxial pressure dependencies of opposite sign, -1.3 K/GPa and 0.3 K/GPa, are extracted for the out-of-plane and in-plane directions at TN1. For T* we obtain dT*/dpc= 1.4 K/GPa. In particular we elucidate thermodynamic properties of the recently discovered skyrmion lattice phase and show that it is strongly enhanced by uniaxial pressure.

cond-mat.str-el↗
arXiv2019

Antiferromagnetic ordering and dipolar interactions of YbAlO$_3$

In this paper we report low-temperature magnetic properties of the rare-earth perovskite material YbAlO$_3$. Results of elastic and inelastic neutron scattering experiment, magnetization measurements along with the crystalline electrical field (CEF) calculations suggest that the ground state of Yb moments is a strongly anisotropic Kramers doublet, and the moments are confined in the $ab$-plane, pointing at an angle of $\varphi = \pm 23.5^{\circ}$ to the $a$-axis. With temperature decreasing below $T_{\rm N}=0.88$ K, Yb moments order into the coplanar, but non-collinear antiferromagnetic (AFM) structure $AxGy$, where the moments are pointed along their easy-axes. In addition, we highlight the importance of the dipole-dipole interaction, which selects the type of magnetic ordering and may be crucial for understanding magnetic properties of other rare-earth orthorhombic perovskites. Further analysis of the broad diffuse neutron scattering shows that one-dimensional interaction along the $c$-axis is dominant, and suggests YbAlO$_3$ as a new member of one dimensional quantum magnets.

cond-mat.str-el↗
arXiv2019

Tomonaga-Luttinger Liquid Behavior and Spinon Confinement in YbAlO$_3$

Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth based magnets because of the large effective spin anisotropy induced by the combination of strong spin-orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO$_3$ provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga-Luttinger liquid behavior and spinon confinement-deconfinement transitions in different regions of magnetic field-temperature phase diagram.

cond-mat.str-el↗
arXiv2018

Pauling entropy, metastability and equilibrium in Dy$_2$Ti$_2$O$_7$ spin ice

Determining the fate of the Pauling entropy in the classical spin ice material Dy$_2$Ti$_2$O$_7$ with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice - the dipolar spin ice model - predicts an ordering transition at $T\approx 0.15$ K, but recent experiments by Pomaranski $et\ al.$ suggest an entropy recovery over long time scales at temperatures as high as $0.5$ K, much too high to be compatible with theory. Using neutron scattering and specific heat measurements at low temperatures and with long time scales ($0.35$ K$/10^6$ s and $0.5$ K$/10^5$ s respectively) on several isotopically enriched samples we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Further, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez $et\ al.$ are, after all, essentially correct: the short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.

cond-mat.str-el↗
arXiv2018

Emergent spin-$1$ Haldane gap and ferroelectricity in a frustrated spin-$1/2$ ladder

We report experimental and theoretical evidence that Rb$_2$Cu$_2$Mo$_3$O$_{12}$ has a nonmagnetic tetramer ground state of a two-leg ladder comprising antiferromagnetically coupled frustrated spin-$1/2$ chains and exhibits a Haldane spin gap of emergent spin-1 pairs. Three spin excitations split from the spin-1 triplet by a Dzyaloshinskii-Moriya interaction are identified in inelastic neutron-scattering and electron spin resonance spectra. A tiny magnetic field generates ferroelectricity without closing the spin gap, indicating a novel class of ferroelectricity induced by a vector spin chirality order.

cond-mat.str-el↗
arXiv2017

Magnetic ground state of the Ising-like antiferromagnet DyScO$_3$

We report the low temperature magnetic properties of the DyScO$_3$ perovskite, which were characterized by means of single crystal and powder neutron scattering, and by magnetization measurements. Below $T_{\mathrm{N}}=3.15$ K, Dy$^{3+}$ moments form an antiferromagnetic structure with an easy axis of magnetization lying in the $ab$-plane. The magnetic moments are inclined at an angle of $\sim\pm{28}^{\circ}$ to the $b$-axis. We show that the ground state Kramers doublet of Dy$^{3+}$ is made up of primarily $|\pm 15/2\rangle$ eigenvectors and well separated by crystal field from the first excited state at $E_1=24.9$ meV. This leads to an extreme Ising single-ion anisotropy, $M_{\perp}/M_{\|}\sim{0.05}$. The transverse magnetic fluctuations, which are proportional to $M^{2}_{\perp}/M^{2}_{\|}$, are suppressed and only moment fluctuations along the local Ising direction are allowed. We also found that the Dy-Dy dipolar interactions along the crystallographic $c$-axis are 2-4 times larger than in-plane interactions.

cond-mat.str-el↗
arXiv2017

Field dependence of the magnetic correlations of the frustrated magnet SrDy$_2$O$_4$

The frustrated magnet SrDy$_2$O$_4$ exhibits a field-induced phase with a magnetization plateau at $1/3$ of the saturation value for magnetic fields applied along the $b$-axis. We report here a neutron scattering study of the nature and symmetry of the magnetic order in this field-induced phase. Below $T\approx 0.5$ K, there are strong hysteretic effects, and the order is short or long ranged for zero-field and field cooling, respectively. We find that the long-range ordered magnetic structure within the zig-zag chains is identical to that expected for the one-dimensional axial next-nearest neighbour Ising (ANNNI) model in longitudinal field. The long-range ordered structure in field contrasts with the short-range order found at zero field, and is probably reached through enhanced quantum fluctuations with increasing fields.

cond-mat.str-el↗
arXiv2016

Non-collinear antiferromagnetism of coupled spins and pseudospins in the double perovskite La2CuIrO6

We report the structural, magnetic and thermodynamic properties of the double perovskite compound La2CuIrO6 from X-ray, neutron diffraction, neutron depolarization, dc magnetization, ac susceptibility, specific heat, muon-spin-relaxation (uSR), electron-spin-resonance (ESR) and nuclear magnetic resonance (NMR) measurements. Below ~113 K, short-range spin-spin correlations occur within the Cu2+ sublattice. With decreasing temperature, the Ir4+ sublattice progressively involves in the correlation process. Below T = 74 K, the magnetic sublattices of Cu (spin s = 1/2) and Ir (pseudospin j = 1/2) in La2CuIrO6 are strongly coupled and exhibit an antiferromagnetic phase transition into a non-collinear magnetic structure accompanied by a small uncompensated transverse moment. A weak anomaly in ac-susceptibility as well as in the NMR and {\mu}SR spin lattice relaxation rates at 54 K is interpreted as a cooperative ordering of the transverse moments which is influenced by the strong spin-orbit coupled 5d ion Ir4+. We argue that the rich magnetic behaviour observed in La2CuIrO6 is related to complex magnetic interactions between the strongly correlated spin-only 3d ions with the strongly spin-orbit coupled 5d transition ions where a combination of the spin-orbit coupling and the low-symmetry of the crystal lattice plays a special role for the spin structure in the magnetically ordered state.

cond-mat.str-el↗
arXiv2015

Investigation of the magnetic structure and crystal field states of pyrochlore antiferromagnet Nd2Zr2O7

We present synchrotron x-ray diffraction, neutron powder diffraction and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd2Zr2O7 to study the ordered state magnetic structure and cystal field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long range all-in/all-out antiferromagnetic order below T_N ~ 0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) \mu_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65 \mu_B/Nd for the local <111> Ising ground state of Nd3+ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The strong Ising anisotropy is further confirmed by the inelastic neutron scattering data which reveals a well-isolated dipolar-octupolar type Kramers doublet ground state. The crystal field level scheme and ground state wavefunction have been determined.

cond-mat.str-el↗
arXiv2015

Complete decoupling of magnetic order and superconductivity in a conventional superconductor

Superconductivity and magnetic order strongly compete in many conventional superconductors, at least partly because both tend to gap the Fermi surface. In magnetically-ordered conventional superconductors, the competition between these cooperative phenomena leads to anomalies at magnetic and superconducting phase boundaries. Here we reveal that in Pr2Pt3Ge5 superconducting and multiple magnetic order are intertwined within the same HT-phase space, but remain completely decoupled. Our thermal conductivity measurements provide evidence for normal electrons in the superconducting phase from which magnetic order emerges with negligible coupling to electron bands that contribute to superconductivity.

cond-mat.str-el↗
arXiv2014

Pressure dependence of the magnetic order in CrAs: a neutron diffraction investigation

The suppression of magnetic order with pressure concomitant with the appearance of pressure- induced superconductivity was recently discovered in CrAs. Here we present a neutron diffraction study of the pressure evolution of the helimagnetic ground-state towards and in the vicinity of the superconducting phase. Neutron diffraction on polycrystalline CrAs was employed from zero pressure to 0.65 GPa and at various temperatures. The helimagnetic long-range order is sustained under pressure and the magnetic propagation vector does not show any considerable change. The average ordered magnetic moment is reduced from 1.73(2) {\mu}B at ambient pressure to 0.4(1) {\mu}B close to the critical pressure Pc=0.7 GPa, at which magnetic order is completely suppressed. The width of the magnetic Bragg peaks strongly depends on temperature and pressure, showing a maximum in the region of the onset of superconductivity. We interpret this as associated with competing ground-states in the vicinity of the superconducting phase.

cond-mat.str-el↗
arXiv2014

Crystal-field interaction and oxygen stoichiometry effects in strontium-doped rare-earth cobaltates

Inelastic neutron scattering was employed to study the crystal-field interaction in the strontium-doped rare-earth compounds R(x)Sr(1-x)CoO(3-z) (R=Pr, Nd, Ho, and Er). Particular emphasis is laid on the effect of oxygen deficiencies which naturally occur in the synthesis of these compounds. The observed energy spectra are found to be the result of a superposition of crystal fields with different nearest-neighbor oxygen coordination at the R sites. The experimental data are interpreted in terms of crystal-field parameters which behave in a consistent manner through the rare-earth series, thereby allowing a reliable extrapolation for rare-earth ions not considered in the present work.

cond-mat.mtrl-sci↗
arXiv2013

High magnetic field evolution of ferroelectricity in CuCrO2

CuCrO2 offers insights into the different types of spiral magnetic orderings that can form spontaneously due to frustration in triangular-lattice antiferromagnets. We explore the magnetic phase diagram up to 65 T along all the principle axes, and also use electric polarization to probe changes in the spiral order at high magnetic fields. It is known that at zero magnetic field a proper-screw spiral of the Cr S = 3/2 spins forms that in turn induces electric polarization with six possible orientations ab-plane. Applied magnetic fields in the (hard) ab-plane have been shown to induce a transition to cycloidal spiral magnetic order above 5.3 T in those domains that have spins perpendicular to the applied magnetic field. We show that the cycloidal order remains unchanged all the way up to 65 T, which is one quarter of the extrapolated saturation magnetization. On the other hand for magnetic fields along the (easy) c-axis, we observe a transition in the electric polarization near 45 T, and it is followed by a series of steps and/or oscillations in the electric polarization. The data is consistent with the a proper-screw-to-cycloidal transition that is pushed from 5.3 to 45 T by easy-axis anisotropy, and is in turn followed by stretching of the magnetic spiral through commensurate and incommensurate wave vectors. This work also highlights the ability of the magnetically-induced electric polarization to probe complex magnetic orders in regimes of phase space that are difficult to reach with neutron diffraction.

cond-mat.mtrl-sci↗
arXiv2013

Temperature-driven Phase Transformation in Y_3Co: Neutron Scattering and First-principles Studies

Contrary to previous studies that identified the ground state crystal structure of the entire R_3Co series (R is a rare earth) as orthorhombic Pnma, we show that Y_3Co undergoes a structural phase transition at T_t=160K. Single crystal neutron diffraction data reveal that at T_t the trigonal prisms formed by a cobalt atom and its six nearest-neighbor yttrium atoms experience distortions accompanied by notable changes of the Y-Co distances. The formation of the low-temperature phase is accompanied by a pronounced lattice distortion and anomalies seen in heat capacity and resistivity measurements. Density functional theory calculations reveal a dynamical instability of the Pnma structure of Y_3Co. In particular, a transversal acoustic phonon mode along the (00z) direction has imaginary frequencies at z<1/4. Employing inelastic neutron scattering measurements we find a strong damping of the (00z) phonon mode below a critical temperature T_t. The observed structural transformation causes the reduction of dimensionality of electronic bands and decreases the electronic density of states at the Fermi level that identifies Y_3Co as a system with the charge density wave instability.

cond-mat.mtrl-sci↗
arXiv2011

Magnetic structure of CuCrO2: a single crystal neutron diffraction study

This paper presents results of a recent study of multiferroic \CCO\ by means of single crystal neutron diffraction. This system has two close magnetic phase transitions at $T\nsub{N1}=24.2$ K and $T\nsub{N2}=23.6$ K. The low temperature magnetic structure below $T\nsub{N2}$ is unambiguously determined to be a fully 3-dimensional proper screw. Between $T\nsub{N1}$ and $T\nsub{N2}$ antiferromagnetic order is found that is essentially 2-dimensional. In this narrow temperature range, magnetic near neighbor correlations are still long range in the ($H,K$) plane, whereas nearest neighbors along the $L$-direction are uncorrelated. Thus, the multiferroic state is realized only in the low-temperature 3-dimensional state and not in the 2-dimensional state.

cond-mat.mtrl-sci↗
arXiv2011

Magnetic excitations in the geometric frustrated multiferroic CuCrO$_2$

In this paper detailed neutron scattering measurements of the magnetic excitation spectrum of CuCrO$_2$ in the ordered state below $T_{\rm{N1}}=24.2$ K are presented. The spectra are analyzed using a model Hamiltonian which includes intralayer-exchange up to the next-next-nearest neighbor and interlayer-exchange. We obtain a definite parameter set and show that exchange interaction terms beyond the next-nearest neighbor are important to describe the inelastic excitation spectrum. The magnetic ground state structure generated with our parameter set is in agreement with the structure proposed for CuCrO$_2$ from the results of single crystal diffraction experiments previously published. We argue that the role of the interlayer exchange is crucial to understand the incommensurability of the magnetic structure as well as the spin-charge coupling mechanism.

cond-mat.mtrl-sci↗