arXiv subjects

J. A. Mydosh

Publications and source records attributed to J. A. Mydosh.

At least 37 records · Page 2Linked to original sources

arXiv2011

Complex charge ordering in CeRuSn

At ambient temperatures, CeRuSn exhibits an extraordinary structure with a coexistence of two types of Ce ions in a metallic environment, namely trivalent Ce3+ and intermediate valent Ce(4-x)+. Charge ordering produces a doubling of the unit cell along the c-axis with respect to the basic monoclinic CeCoAl type structure. Below room temperature, a phase transition with very broad hysteresis has been observed in various bulk properties like electrical resistivity, magnetic susceptibility, and specific heat. The present x-ray diffraction results show that at low temperatures the doubling of the CeCoAl type structure is replaced by an ill-defined modulated ground state. In this state, at least three different modulation periods compete, with the dominant mode close to a tripling of the basic cell. The transition is accompanied by a significant contraction of the c axis. XANES data suggest that the average Ce valence remains constant, thus the observed c axis contraction is not due to any valence transition. We propose a qualitative structure model with modified stacking sequences of Ce3+ and Ce(4-x)+ layers in the various modulated phases. Surprisingly, far below 100 K the modulated state is sensitive to x-ray irradiation at photon fluxes available at a synchrotron. With photon fluxes of order 10E12/s, the modulated ground state can be destroyed on a timescale of minutes and the doubling of the CeCoAl cell observed at room temperature is recovered. The final state is metastable at 10 K. Heating the sample above 60 K again leads to a recovery of the modulated state. Thus, CeRuSn exhibits both thermally and x-ray induced reversible transformations of the Ce3+/Ce(4-x)+ charge ordering pattern. Such a behavior is unique among any know intermetallic compound.

cond-mat.str-el↗

arXiv2011

Colloquium: Hidden Order, Superconductivity, and Magnetism -- The Unsolved Case of URu2Si2

This Colloquium reviews the 25 year quest for understanding the continuous (second-order) mean-field-like phase transition occurring at 17.5 K in URu2Si2. About ten years ago, the term hidden order (HO) was coined and has since been utilized to describe the unknown ordered state, whose origin cannot be disclosed by conventional solid-state probes, such as x rays, neutrons, or muons. HO is able to support superconductivity at lower temperatures (Tc ~ 1.5 K), and when magnetism is developed with increasing pressure both the HO and the superconductivity are destroyed. Other ways of probing the HO are via Rh-doping and very large magnetic fields. During the last few years a variety of advanced techniques have been tested to probe the HO state and their attempts will be summarized. A digest of recent theoretical developments is also included. It is the objective of this Colloquium to shed additional light on the HO state and its associated phases in other materials.

cond-mat.str-el↗

arXiv2011

Hybridization gap and anisotropic far-infrared optical conductivity of URu2Si2

We performed far-infrared optical spectroscopy measurements on the heavy fermion compound URu 2 Si 2 as a function of temperature. The light's electric-field was applied along the a-axis or the c-axis of the tetragonal structure. We show that in addition to a pronounced anisotropy, the optical conductivity exhibits for both axis a partial suppression of spectral weight around 12 meV and below 30 K. We attribute these observations to a change in the bandstructure below 30 K. However, since these changes have no noticeable impact on the entropy nor on the DC transport properties, we suggest that this is a crossover phenomenon rather than a thermodynamic phase transition.

cond-mat.str-el↗

arXiv2010

Electronic structure theory of the hidden order material URu$_2$Si$_2$

We report a comprehensive electronic structure investigation of the paramagnetic (PM), the large moment antiferromagnetic (LMAF), and the hidden order (HO) phases of URu$_2$Si$_2$. We have performed relativistic full-potential calculations on the basis of the density functional theory (DFT), employing different exchange-correlation functionals to treat electron correlations within the open $5f$-shell of uranium. Specifically, we investigate---through a comparison between calculated and low-temperature experimental properties---whether the $5f$ electrons are localized or delocalized in URu$_2$Si$_2$. We also performed dynamical mean field theory calculations (LDA+DMFT) to investigate the temperature evolution of the quasi-particle states at 100~K and above, unveiling a progressive opening of a quasi-particle gap at the chemical potential when temperature is reduced. A detailed comparison of calculated properties with known experimental data demonstrates that the LSDA and GGA approaches, in which the uranium $5f$ electrons are treated as itinerant, provide an excellent explanation of the available low-temperature experimental data of the PM and LMAF phases. We show furthermore that due to a materials-specific Fermi surface instability a large, but partial, Fermi surface gapping of up to 750 K occurs upon antiferromagnetic symmetry breaking. The occurrence of the HO phase is explained through dynamical symmetry breaking induced by a mode of long-lived antiferromagnetic spin-fluctuations. This dynamical symmetry breaking model explains why the Fermi surface gapping in the HO phase is similar but smaller than that in the LMAF phase and it also explains why the HO and LMAF phases have the same Fermi surfaces yet different order parameters. Suitable derived order parameters for the HO are proposed to be the Fermi surface gap or the dynamic spin-spin correlation function.

cond-mat.str-el↗

arXiv2009

Spinon localization in the heat transport of the spin-1/2 ladder compound (C$_5$H$_{12}$N)$_2$CuBr$_4$

We present experiments on the magnetic field-dependent thermal transport in the spin-1/2 ladder system (C$_5$H$_{12}$N)$_2$CuBr$_4$. The thermal conductivity $κ(B)$ is only weakly affected by the field-induced transitions between the gapless Luttinger-liquid state realized for $B_{c1}< B < B_{c2}$ and the gapped states, suggesting the absence of a direct contribution of the spin excitations to the heat transport. We observe, however, that the thermal conductivity is strongly suppressed by the magnetic field deeply within the Luttinger-liquid state. These surprising observations are discussed in terms of localization of spinons within finite ladder segments and spinon-phonon umklapp scattering of the predominantly phononic heat transport.

cond-mat.str-el↗

arXiv2009

Epitaxy, stoichiometry, and magnetic properties of Gd-doped EuO films on YSZ (001)

We have succeeded in preparing high-quality Gd-doped single-crystalline EuO films. Using Eu-distillation-assisted molecular beam epitaxy and a systematic variation in the Gd and oxygen deposition rates, we have been able to observe sustained layer-by-layer epitaxial growth on yttria-stabilized cubic zirconia (001). The presence of Gd helps to stabilize the layer-by-layer growth mode. We used soft x-ray absorption spectroscopy at the Eu and Gd M4,5 edges to confirm the absence of Eu3+ contaminants and to determine the actual Gd concentration. The distillation process ensures the absence of oxygen vacancies in the films. From magnetization measurements we found the Curie temperature to increase smoothly as a function of doping from 70 K up to a maximum of 125 K. A threshold behavior was not observed for concentrations as low as 0.2%.

cond-mat.str-el↗

arXiv2009

Parasitic small-moment-antiferromagnetism and non-linear coupling of hidden order and antiferromagnetism in URu2Si2 observed by Larmor diffraction

We report simultaneous measurements of the distribution of lattice constants and the antiferromagnetic moment in high-purity URu2Si2, using both Larmor and conventional neutron diffraction, as a function of temperature and pressure up to 18 kbar. We establish that the tiny moment in the hidden order (HO) state is purely parasitic and quantitatively originates from the distribution of lattice constants. Moreover, the HO and large-moment antiferromagnetism (LMAF) at high pressure are separated by a line of first-order phase transitions, which ends in a bicritical point. Thus the HO and LMAF are coupled non-linearly and must have different symmetry, as expected of the HO being, e.g., incommensurate orbital currents, helicity order, or multipolar order.

cond-mat.str-el↗

arXiv2009

Evidence for strongly coupled charge-density-wave ordering in three-dimensional RE5Ir4Si10 compounds by optical measurements

We report optical spectra of Lu$_5$Ir$_4$Si$_{10}$ and Er$_5$Ir$_4$Si$_{10}$, exhibiting the phenomenon of coexisting superconductivity or antiferromagnetism and charge density wave (CDW) order. We measure the maximum value of the charge density wave gap present on part of the Fermi surface of Lu5Ir4Si10, corresponding to a ratio 2Δ/k_B T_CDW \approx 10, well above the value in the limit of weak electron-phonon coupling. Strong electron-phonon coupling was confirmed by analyzing the optical conductivity with the Holstein model describing the electron-phonon interactions, indicating the coupling to phonons centered at 30 meV, with a coupling constant λ\approx 2.6. Finally we provide evidence that approximately 16 % of the Fermi surface of Lu5Ir4Si10 becomes gapped in the CDW state.

cond-mat.str-el↗

arXiv2008

Uncovering the hidden order in URu2Si2: Identification of Fermi surface instability and gapping

Spontaneous, collective ordering of electronic degrees of freedom leads to second-order phase transitions that are characterized by an order parameter. The notion "hidden order" (HO) has recently been used for a variety of materials where a clear phase transition occurs to a phase without a known order parameter. The prototype example is the heavy-fermion compound URu2Si2 where a mysterious HO transition occurs at 17.5K. For more than twenty years this system has been studied theoretically and experimentally without a firm grasp of the underlying physics. Using state-of-the-art density-functional theory calculations, we provide here a microscopic explanation for the HO. We identify the Fermi surface "hot spots" where degeneracy induces a Fermi surface instability and quantify how symmetry breaking lifts the degeneracy, causing a surprisingly large Fermi surface gapping. As mechanism for the HO we propose spontaneous symmetry breaking through collective antiferromagnetic moment excitations.

cond-mat.str-el↗

arXiv2008

Mott-Hubbard exciton in the optical conductivity of YTiO3 and SmTiO3

In the Mott-Hubbard insulators YTiO3 and SmTiO3 we study optical excitations from the lower to the upper Hubbard band, d^1d^1 -> d^0d^2. The multi-peak structure observed in the optical conductivity reflects the multiplet structure of the upper Hubbard band in a multi-orbital system. Absorption bands at 2.55 and 4.15 eV in the ferromagnet YTiO3 correspond to final states with a triplet d^2 configuration, whereas a peak at 3.7 eV in the antiferromagnet SmTiO3 is attributed to a singlet d^2 final state. A strongly temperature-dependent peak at 1.95 eV in YTiO3 and 1.8 eV in SmTiO3 is interpreted in terms of a Hubbard exciton, i.e., a charge-neutral (quasi-)bound state of a hole in the lower Hubbard band and a double occupancy in the upper one. The binding to such a Hubbard exciton may arise both due to Coulomb attraction between nearest-neighbor sites and due to a lowering of the kinetic energy in a system with magnetic and/or orbital correlations. Furthermore, we observe anomalies of the spectral weight in the vicinity of the magnetic ordering transitions, both in YTiO3 and SmTiO3. In the G-type antiferromagnet SmTiO3, the sign of the change of the spectral weight at T_N depends on the polarization. This demonstrates that the temperature dependence of the spectral weight is not dominated by the spin-spin correlations, but rather reflects small changes of the orbital occupation.

cond-mat.str-el↗

arXiv2008

Magneto-thermal evidence of a partial gap at the Fermi surface of UPt_2Si_2

Motivated by the observation of a giant Nernst effect in URu_2Si_2, the thermoelectric response of the related system UPt_2Si_2 was investigated using thermal and electric transport properties such as the Nernst and Seebeck effects, thermal conductivity, Hall effect and electrical resitivity. Unlike URu_2Si_2, UPt_2Si_2 is neither superconducting nor exhibits a ``hidden-order'' state. Nevertheless a pronounced Nernst effect anomaly is found to coincide with the onset of the antiferromagnetic order in UPt_2Si_2. Although the absolute values are substantially lower, its appearance and characteristics can favorably be compared to the giant Nernst effect in URu_2Si_2 indicating the common feature of a partial Fermi surface gap.

cond-mat.str-el↗

arXiv2008

Field-dependent thermal transport in the Haldane chain compound NENP

We present a study of the magnetic field-dependent thermal transport in the spin S=1 chain material Ni(C2H8N2)2NO2(ClO4) (NENP). The measured thermal conductivity is found to be very sensitive to the field-induced changes in the spin excitation spectrum. The magnetic contribution to the total heat conductivity is analyzed in terms of a quasiparticle model, and we obtain a temperature and momentum independent mean free path. This implies that the motion of quasiparticles is effectively three dimensional despite the tiny interchain coupling.

cond-mat.str-el↗

arXiv2008

Mott-Hubbard versus charge-transfer behavior in LaSrMnO4 studied via optical conductivity

Using spectroscopic ellipsometry, we study the optical conductivity sigma(omega) of insulating LaSrMnO4 in the energy range of 0.75-5.8 eV from 15 to 330 K. The layered structure gives rise to a pronounced anisotropy. A multipeak structure is observed in sigma_1^a(omega) (2, 3.5, 4.5, 4.9, and 5.5 eV), while only one peak is present at 5.6 eV in sigma_1^c(omega). We employ a local multiplet calculation and obtain (i) an excellent description of the optical data, (ii) a detailed peak assignment in terms of the multiplet splitting of Mott-Hubbard and charge-transfer absorption bands, and (iii) effective parameters of the electronic structure, e.g., the on-site Coulomb repulsion U_eff=2.2 eV, the in-plane charge-transfer energy Delta_a=4.5 eV, and the crystal-field parameters for the d^4 configuration (10 Dq=1.2 eV, Delta_eg=1.4 eV, and Delta_t2g=0.2 eV). The spectral weight of the lowest absorption feature (at 1-2 eV) changes by a factor of 2 as a function of temperature, which can be attributed to the change of the nearest-neighbor spin-spin correlation function across the Neel temperature. Interpreting LaSrMnO4 effectively as a Mott-Hubbard insulator naturally explains this strong temperature dependence, the relative weight of the different absorption peaks, and the pronounced anisotropy. By means of transmittance measurements, we determine the onset of the optical gap Delta^a_opt=0.4-0.45 eV at 15 K and 0.1-0.2 eV at 300 K. Our data show that the crystal-field splitting is too large to explain the anomalous temperature dependence of the c-axis lattice parameter by thermal occupation of excited crystal-field levels. Alternatively, we propose that a thermal population of the upper Hubbard band gives rise to the shrinkage of the c-axis lattice parameter.

cond-mat.str-el↗

arXiv2007

Pyroxenes: A new class of multiferroics

Pyroxenes with the general formula $AM$Si$_2$O$_6$ ($A$ = mono- or divalent metal, $M$ = di- or trivalent metal) are shown to be a new class of multiferroic materials. In particular, we have found so far that NaFeSi$_2$O$_6$ becomes ferroelectric in a magnetically ordered state below $\simeq 6$ K. Similarly, magnetically driven ferroelectricity is also detected in the Li homologues, LiFeSi$_2$O$_6$ ($T_C \simeq 18$ K) and LiCrSi$_2$O$_6$ ($T_C \simeq 11$ K). In all these monoclinic systems the electric polarization can be strongly modified by magnetic fields. Measurements of magnetic susceptibility, pyroelectric current and dielectric constants (and their dependence on magnetic field) are performed using a natural crystal of aegirine (NaFeSi$_2$O$_6$) and synthetic crystals of LiFeSi$_2$O$_6$ and LiCrSi$_2$O$_6$ grown from melt solution. For NaFeSi$_2$O$_6$ a temperature versus magnetic field phase diagram for NaFeSi$_2$O$_6$ is proposed. Exchange constants are computed on the basis of {\it ab initio} band structure calculations. The possibility of a spiral magnetic structure caused by frustration as origin of the multiferroic behaviour is discussed. We propose that other pyroxenes may also be multiferroic, and that the versatility of this family offers an exceptional opportunity to study general conditions for and mechanisms of magnetically driven ferroelectricity.

cond-mat.str-el↗

arXiv2007

Thermal expansion of the magnetically ordering intermetallics RTMg (R = Eu, Gd and T = Ag, Au)

We report measurements of the thermal expansion for two Eu$^{+2}$- and two Gd$^{+3}$-based intermetallics which exhibit ferro- or antiferromagnetic phase transitions. These materials show sharp positive (EuAgMg and GdAuMg) and negative (EuAuMg and GdAgMg) peaks in the temperature dependence of the thermal expansion coefficient $α$ which become smeared and/or displaced in an external magnetic field. Together with specific heat data we determine the initial pressure dependences of the transition temperatures at ambient pressure using the Ehrenfest or Clausius-Clapeyron relation. We find large pressure dependences indicating strong spin-phonon coupling, in particular for GdAgMg and EuAuMg where a quantum phase transition might be reached at moderate pressures of a few GPa.

cond-mat.mtrl-sci↗

arXiv2007

Insulator to semiconductor transition and magnetic properties of the one-dimensional S = 1/2 system In_2VO_5

We report structural, magnetization, electrical resistivity and nuclear- and electron spin resonance data of the complex transition metal oxide In_2VO_5 in which structurally well-defined V-O chains are realized. An itinerant character of the vanadium d-electrons and ferromagnetic correlations, revealed at high temperatures, are contrasted with the insulating behavior and predominantly antiferromagnetic exchange between the localized V^{4+} S = 1/2-magnetic moments which develop below a certain characteristic temperature T* ~ 120 K. Eventually the compound exhibits short-range magnetic order at $T_SRO ~ 20 K. We attribute this crossover occurring around T* to the unusual anisotropic thermal contraction of the lattice which changes significantly the overlap integrals and the character of magnetic intra- and interchain interactions.

cond-mat.str-el↗

arXiv2007

Nernst Effect in NdBa_2[Cu_{1-y}Ni_y]_3O_{7-δ}

In NdBa_2[Cu_{1-y}Ni_y]_3O_{7-δ}, magnetic Ni-impurities suppress Tc but at the same time the pseudogap is strongly enhanced. This unique feature makes it an ideal system to study possible relations between the anomalous Nernst effect, superconductivity and the pseudogap. We present Nernst effect measurements on a series of optimally doped (O_7) and underdoped (O_{6.8}) samples with Ni contents ranging from y=0 to 0.12. In all samples an onset of the Nernst signal is found at T^ν> Tc. For the optimally doped samples T^νand Tc decrease simultaneously with increasing Ni content. The underdoped samples show a different behavior, i.e. the onset of the Nernst signal is hardly affected by increasing the Ni content from y=0 to 0.03. Irrespective of the oxygen content, T^νclearly does not track the enhanced pseudogap temperature T*.

cond-mat.supr-con↗

arXiv2007

Anomalous thermal expansion and strong damping of the thermal conductivity of NdMnO$_3$ and TbMnO$_3$ due to 4f crystal-field excitations

We present measurements of the thermal conductivity $κ$ and the thermal expansion $α$ of NdMnO$_3$ and TbMnO$_3$. In both compounds a splitting of the $4f$ multiplet of the $R^{3+}$ ion causes Schottky contributions to $α$. In TbMnO$_3$ this contribution arises from a crystal-field splitting, while in NdMnO$_3$ it is due to the Nd-Mn exchange coupling. Another consequence of this coupling is a strongly enhanced canting of the Mn moments. The thermal conductivity is greatly suppressed in both compounds. The main scattering process at low temperatures is resonant scattering of phonons between different energy levels of the $4f$ multiplets, whereas the complex 3d magnetism of the Mn ions is of minor importance.

cond-mat.str-el↗