arXiv subjects

V. S. Zapf

Publications and source records attributed to V. S. Zapf.

At least 19 recordsLinked to original sources

arXiv2021

Non-magnetic ion site disorder effects on the quantum magnetism of a spin-1/2 equilateral triangular lattice antiferromagnet

With the motivation to study how non-magnetic ion site disorder affects the quantum magnetism of Ba3CoSb2O9, a spin-1/2 equilateral triangular lattice antiferromagnet, we performed DC and AC susceptibility, specific heat, elastic and inelastic neutron scattering measurements on single crystalline samples of Ba2.87Sr0.13CoSb2O9 with Sr doping on non-magnetic Ba2+ ion sites. The results show that Ba2.87Sr0.13CoSb2O9 exhibits (i) a two-step magnetic transition at 2.7 K and 3.3 K, respectively; (ii) a possible canted 120-degree spin structure at zero field with reduced ordered moment as 1.24μB/Co; (iii) a series of spin state transitions for both H // ab-plane and H // c-axis. For H // ab-plane, the magnetization plateau feature related to the up-up-down phase is significantly suppressed; (iv) an inelastic neutron scattering spectrum with only one gapped mode at zero field, which splits to one gapless and one gapped mode at 9 T. All these features are distinctly different from those observed for the parent compound Ba3CoSb2O9, which demonstrates that the non-magnetic ion site disorder (the Sr doping) plays a complex role on the magnetic properties beyond the conventionally expected randomization of the exchange interactions. We propose the additional effects including the enhancement of quantum spin fluctuations and introduction of a possible spatial anisotropy through the local structural distortions.

cond-mat.str-el↗

arXiv2021

Magnetization process of atacamite: a case of weakly coupled $S = 1/2$ sawtooth chains

We present a combined experimental and theoretical study of the mineral atacamite Cu$_2$Cl(OH)$_3$. Density functional theory yields a Hamiltonian describing anisotropic sawtooth chains with weak 3D connections. Experimentally, we fully characterize the antiferromagnetically ordered state. Magnetic order shows a complex evolution with the magnetic field, while, starting at 31.5 T, we observe a plateau-like magnetization at about $M_{\rm sat}/2$. Based on complementary theoretical approaches, we show that the latter is unrelated to the known magnetization plateau of a sawtooth chain. Instead, we provide evidence that the magnetization process in atacamite is a field-driven canting of a 3D network of weakly coupled sawtooth chains that form giant moments.

cond-mat.str-el↗

arXiv2020

Domain wall patterning and giant response functions in ferrimagnetic spinels

The manipulation of mesoscale domain wall phenomena has emerged as a powerful strategy for designing ferroelectric responses in functional devices, but its full potential has not yet been realized in the field of magnetism. We show that mechanically strained samples of Mn$_3$O$_4$ and MnV$_2$O$_4$ exhibit a stripe-like patterning of the bulk magnetization below known magnetostructural transitions, similar to the structural domains reported in ferroelectric materials. Building off our previous magnetic force microscopy data, we use small angle neutron scattering to show that these patterns extend to the bulk, and demonstrate an ability to manipulate the domain walls via applied magnetic field and mechanical stress. We then connect these domains back to the anomalously large magnetoelastic and magnetodielectric response functions reported in these materials, directly correlating local and macroscopic measurements on the same crystals.

cond-mat.mtrl-sci↗

arXiv2017

Evolution of the Kondo lattice electronic structure above the transport coherence temperature

The temperature-dependent evolution of the Kondo lattice is a long-standing topic of theoretical and experimental investigation and yet it lacks a truly microscopic description of the relation of the basic $f$-$d$ hybridization processes to the fundamental temperature scales of Kondo screening and Fermi-liquid lattice coherence. Here, the temperature-dependence of $f$-$d$ hybridized band dispersions and Fermi-energy $f$ spectral weight in the Kondo lattice system CeCoIn$_5$ is investigated using $f$-resonant angle-resolved photoemission (ARPES) with sufficient detail to allow direct comparison to first principles dynamical mean field theory (DMFT) calculations containing full realism of crystalline electric field states. The ARPES results, for two orthogonal (001) and (100) cleaved surfaces and three different $f$-$d$ hybridization scenarios, with additional microscopic insight provided by DMFT, reveal $f$ participation in the Fermi surface at temperatures much higher than the lattice coherence temperature, $T^*\approx$ 45 K, commonly believed to be the onset for such behavior. The identification of a $T$-dependent crystalline electric field degeneracy crossover in the DMFT theory $below$ $T^*$ is specifically highlighted.

cond-mat.str-el↗

arXiv2016

Electric polarization observed in single crystals of multiferroic Lu2MnCoO6

We report electric polarization and magnetization measurements in single crystals of double perovskite Lu2MnCoO6 using pulsed magnetic fields and optical second harmonic generation (SHG) in DC magnetic fields. we observe well-resolved magnetic field-induced changes in the electric polarization in single crystals and thereby resolve the question about whether multiferroic behavior is intrinsic to these materials or an extrinsic feature of polycrystals. We find electric polarization along the crystalline b-axis, that is suppressed by applying a magnetic fields along c-axis and advance a model for the origin of magnetoelectric coupling. We furthermore map the phase diagram using both capacitance and electric polarization to identify regions of ordering and regions of magnetoelectric hysteresis. This compound is a rare example of coupled hysteretic behavior in the magnetic and electric properties. The ferromagnetic-like magnetic hysteresis loop that couples to hysteretic polarization can be attributed not to ordinary ferromagnetic domains, but to the rich physics of magnetic frustration of Ising-like spins in the axial next-nearest neighbor interaction model.

cond-mat.mtrl-sci↗

arXiv2015

Successive magnetic field-induced transitions and colossal magnetoelectric effect in Ni$_{3}$TeO$_{6}$

We report the discovery of a metamagnetic phase transition in a polar antiferromagnet Ni$_3$TeO$_6$ that occurs at 52 T. The new phase transition accompanies a colossal magnetoelectric effect, with a magnetic-field-induced polarization change of 0.3 $μ$C/cm$^2$, a value that is 4 times larger than for the spin-flop transition at 9 T in the same material, and also comparable to the largest magnetically-induced polarization changes observed to date. Via density-functional calculations we construct a full microscopic model that describes the data. We model the spin structures in all fields and clarify the physics behind the 52 T transition. The high-field transition involves a competition between multiple different exchange interactions which drives the polarization change through the exchange-striction mechanism. The resultant spin structure is rather counter-intuitive and complex, thus providing new insights on design principles for materials with strong magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2014

Multiferroicity with coexisting isotropic and anisotropic spins in Ca$_{3}$Co$_{2-x}$Mn$_{x}$O$_{6}$

We study magnetic and multiferroic behavior in Ca$_3$Co$_{2-x}$Mn$_{x}$O$_6$ ($x \sim$0.97) by high-field measurements of magnetization ($M$), magnetostriction ($L$($H$)/$L$), electric polarization ($P$), and magnetocaloric effect. This study also gives insight into the zero and low magnetic field magnetic structure and magnetoelectric coupling mechanisms. We measured $M$ and $Δ$$L$/$L$ up to pulsed magnetic fields of 92 T, and determined the saturation moment and field. On the controversial topic of the spin states of Co$^{2+}$ and Mn$^{4+}$ ions, we find evidence for $S$ = 3/2 spins for both ions with no magnetic field-induced spin-state crossovers. Our data also indicate that Mn$^{4+}$ spins are quasi-isotropic and develop components in the $ab$-plane in applied magnetic fields of 10 T. These spins cant until saturation at 85 T whereas the Ising Co$^{2+}$ spins saturate by 25 T. Furthermore, our results imply that mechanism for suppression of electric polarization with magnetic fields near 10 T is flopping of the Mn$^{4+}$ spins into the $ab$-plane, indicating that appropriate models must include the coexistence of Ising and quasi-isotropic spins.

cond-mat.str-el↗

arXiv2013

Magnetic Field Induced Transition in Vanadium Spinels

We study vanadium spinels $A$V$_2$O$_4$ ($A$ = Cd, Mg) in pulsed magnetic fields up to 65 T. A jump in magnetization at $μ_0 H \approx$ 40 T is observed in the single-crystal MgV$_2$O$_4$, indicating a field induced quantum phase transition between two distinct magnetic orders. In the multiferroic CdV$_2$O$_4$, the field-induced transition is accompanied by a suppression of the electric polarization. By modeling the magnetic properties in the presence of strong spin-orbit coupling characteristic of vanadium spinels, we show that both features of the field-induced transition can be successfully explained by including the effects of the local trigonal crystal field.

cond-mat.str-el↗

arXiv2013

Quantum oscillations and optical conductivity in Rashba spin-splitting BiTeI

We report the observation of Shubnikov-de Haas (SdH) oscillations in single crystals of the Rashba spin-splitting compound BiTeI, from both longitudinal ($R_{xx}(B)$) and Hall ($R_{xy}(B)$) magnetoresistance. Under magnetic field up to 65 T, we resolved unambiguously only one frequency $F = 284.3\pm 1.3$ T, corresponding to a Fermi momentum $k_{F} = 0.093\pm 0.002$Å$^{-1}$.The amplitude of oscillations is strongly suppressed by tilting magnetic field, suggesting a highly two-dimensional Fermi surface. Combining with optical spectroscopy, we show that quantum oscillations may be consistent with a bulk conduction band having a Rashba splitting momentum $k_{R}=0.046\pm$Å$^{-1}$.

cond-mat.mtrl-sci↗

arXiv2012

Synthesis and physical properties of the new potassium iron selenide superconductor K0.80Fe1.76Se2

In this article we review our studies of the K0.80Fe1.76Se2 superconductor, with an attempt to elucidate the crystal growth details and basic physical properties over a wide range of temperatures and applied magnetic field, including anisotropic magnetic and electrical transport properties, thermodynamic, London penetration depth, magneto-optical imaging and Mossbauer measurements. We find that: (i) Single crystals of similar stoichiometry can be grown both by furnace-cooled and decanted methods; (ii) Single crystalline K0.80Fe1.76Se2 shows moderate anisotropy in both magnetic susceptibility and electrical resistivity and a small modulation of stoichiometry of the crystal, which gives rise to broadened transitions; (iii) The upper critical field, Hc2(T) is ~ 55 T at 2 K for H||c, manifesting a temperature dependent anisotropy that peaks near 3.6 at 27 K and drops to 2.5 by 18 K; (iv) Mossbauer measurements reveal that the iron sublattice in K0.80Fe1.76Se2 clearly exhibits magnetic order, probably of the first order, from well below Tc to its Neel temperature of Tn = 532 +/- 2 K. It is very important to note that, although, at first glance there is an apparent dilemma posed by these data: high Tc superconductivity in a near insulating, large ordered moment material, analysis indicates that the sample may well consist of two phases with the minority superconducting phase (that does not exhibit magnetic order) being finely distributed, but connected with in an antiferromagnetic, poorly conducting, matrix, essentially making a superconducting aerogel.

cond-mat.supr-con↗

arXiv2011

Upper critical fields and two-band superconductivity in Sr1-xEux(Fe0.89Co0.11)2As2 (x=0.203 and 0.463)

The upper critical fields, Hc2 of single crystals of Sr1-xEux(Fe0.89Co0.11)2As2(x=0.203 and 0.463) were determined by radio frequency penetration depth measurements in pulsed magnetic fields. Hc2 approaches the Pauli limiting field but shows an upward curvature with an enhancement from the orbital limited field as inferred from Werthamer-Helfand-Hohenberg theory. We discuss the temperature dependence of the upper critical fields and the decreasing anisotropy using a two-band BCS model.

cond-mat.supr-con↗

arXiv2011

Multiferroic behavior in the new double-perovskite Lu$_2$MnCoO$_6$

We present a new member of the multiferroic oxides, Lu$_2$MnCoO$_6$, which we have investigated using X-ray diffraction, neutron diffraction, specific heat, magnetization, electric polarization, and dielectric constant measurements. This material possesses an electric polarization strongly coupled to a net magnetization below 35 K, despite the antiferromagnetic ordering of the $S = 3/2$ Mn$^{4+}$ and Co$^{2+}$ spins in an $\uparrow \uparrow \downarrow \downarrow$ configuration along the c-direction. We discuss the magnetic order in terms of a condensation of domain boundaries between $\uparrow \uparrow$ and $\downarrow \downarrow$ ferromagnetic domains, with each domain boundary producing a net electric polarization due to spatial inversion symmetry breaking. In an applied magnetic field the domain boundaries slide, controlling the size of the net magnetization, electric polarization, and magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2011

Anisotropic Hc2 of K0.8Fe1.76Se2 determined up to 60 T

The anisotropic upper critical field, Hc2(T), curves for K0.8Fe1.76Se2 are determined over a wide range of temperatures down to 1.5 K and magnetic fields up to 60 T. Anisotropic initial slopes of Hc2 ~ -1.4 T/K and -4.6 T/K for magnetic field applied along c-axis and ab-plane, respectively, were observed. Whereas the c-axis Hc2|c(T) increases quasi-linearly with decreasing temperature, the ab-plane Hc2|ab(T) shows a flattening, starting near 25 K above 30 T. This leads to a non-monotonic temperature dependence of the anisotropy parameter γ= Hc2|ab/Hc2|c. The anisotropy parameter is ~ 2 near Tc ~ 32 K and rises to a maximum γ~ 3.6 around 27 K. For lower temperatures, γdecreases with T in a linear fashion, dropping to γ~ 2.5 by T ~ 18 K. Despite the apparent differences between the K0.8Fe1.76Se2 and (Ba0.55K0.45)Fe2As2 or Ba(Fe0.926Co0.074)2As2, in terms of the magnetic state and proximity to an insulating state, the Hc2(T) curves are remarkably similar.

cond-mat.supr-con↗

arXiv2010

Quantum fluctuations and strong mass renormalization in NiCl2-4SC(NH2)2

In a number of quantum paramagnets, magnetic field can induce a quantum phase transition to an antiferromagnetic state which exists for a range of fields Hc1 < H < Hc2. Generally, these compounds exhibit a significant asymmetry in their properties at low- and high-field transitions. Here we present detailed specific heat and thermal conductivity measurements in NiCl2-4SC(NH2)2 together with analytical and numerical results. We show that the asymmetry is caused by a strong renormalization of the effective mass of spin excitations due to quantum fluctuations for H<Hc1 that are absent for H<Hc2.

cond-mat.str-el↗

arXiv2010

Magnetoelectric effects in an organo-metallic quantum magnet

We observe a bilinear magnetic field-induced electric polarization of 50 $μC/m^2$ in single crystals of NiCl$_2$-4SC(NH$_2$)$_2$ (DTN). DTN forms a tetragonal structure that breaks inversion symmetry, with the highly polar thiourea molecules all tilted in the same direction along the c-axis. Application of a magnetic field between 2 and 12 T induces canted antiferromagnetism of the Ni spins and the resulting magnetization closely tracks the electric polarization. We speculate that the Ni magnetic forces acting on the soft organic lattice can create significant distortions and modify the angles of the thiourea molecules, thereby creating a magnetoelectric effect. This is an example of how magnetoelectric effects can be constructed in organo-metallic single crystals by combining magnetic ions with electrically polar organic elements.

cond-mat.mtrl-sci↗

arXiv2009

Magnetically-induced electric polarization in an organo-metallic magnet

The coupling between magnetic order and ferroelectricity has been under intense investigation in a wide range of transition-metal oxides. The strongest coupling is obtained in so-called magnetically-induced multiferroics where ferroelectricity arises directly from magnetic order that breaks inversion symmetry. However, it has been difficult to find non-oxide based materials in which these effects occur. Here we present a study of copper dimethyl sulfoxide dichloride (CDC), an organo-metallic quantum magnet containing $S = 1/2$ Cu spins, in which electric polarization arises from non-collinear magnetic order. We show that the electric polarization can be switched in a stunning hysteretic fashion. Because the magnetic order in CDC is mediated by large organic molecules, our study shows that magnetoelectric interactions can exist in this important class of materials, opening the road to designing magnetoelectrics and multiferroics using large molecules as building blocks. Further, we demonstrate that CDC undergoes a magnetoelectric quantum phase transition where both ferroelectric and magnetic order emerge simultaneously as a function of magnetic field at very low temperatures.

cond-mat.mtrl-sci↗

arXiv2008

Character of magnetic excitations in a quasi-one-dimensional antiferromagnet near the quantum critical points: Impact on magneto-acoustic properties

We report results of magneto-acoustic studies in the quantum spin-chain magnet NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) having a field-induced ordered antiferromagnetic (AF) phase. In the vicinity of the quantum critical points (QCPs) the acoustic $c_{33}$ mode manifests a pronounced softening accompanied by energy dissipation of the sound wave. The acoustic anomalies are traced up to $T > T_N$, where the thermodynamic properties are determined by fermionic magnetic excitations, the "hallmark" of one-dimensional (1D) spin chains. On the other hand, as established in earlier studies, the AF phase in DTN is governed by bosonic magnetic excitations. Our results suggest the presence of a crossover from a 1D fermionic to a 3D bosonic character of the magnetic excitations in DTN in the vicinity of the QCPs.

cond-mat.stat-mech↗

arXiv2008

A direct measurement of the Bose-Einstein Condensation universality class in NiCl$_2$-4SC(NH$_2$)$_2$ at ultra-low temperatures

In this work, we demonstrate field-induced Bose-Einstein condensation (BEC) in the organic compound NiCl$_2$-4SC(NH$_2$)$_2$ using AC susceptibility measurements down to 1 mK. The Ni $\textsl{S}$=1 spins exhibit 3D $\mathit{XY}$ antiferromagnetism between a lower critical field $H_{c1} \sim$ 2 T and a upper critical field $H_{c2} \sim$ 12 T. The results show a power-law temperature dependence of the phase transition line $H_{c1} (T) -H_{c1} (0) = aT^α$ with $α=$ 1.47$\pm$0.10 and $H_{c1} (0) = 2.053$ T, consistent with the 3D Bose-Einstein Condensation universality class. An abnormal change was found in the phase boundary near $H_{c2}$ at approximately 150 mK.

cond-mat.str-el↗