arXiv subjects

Cornelius Krellner

Publications and source records attributed to Cornelius Krellner.

At least 55 records · Page 3Linked to original sources

arXiv2022

Effect of symmetry reduction on the magnetic properties of LnIr$_2$Si$_2$ polymorphs

Many tetragonal compounds LnIr$_2$Si$_2$ (Ln = lanthanoid) occur in two polymorphous phases and are therefore well suited to study the relationship between crystal structure and magnetic properties. We have grown GdIr$_2$Si$_2$ single crystals of both polymorphs from a high-temperature indium flux and investigated their anisotropic magnetic properties. The higher symmetric form with the ThCr$_2$Si$_2$ structure (space group $I4/mmm$) orders antiferromagnetically at $T_{\rm N}=87\,\rm K$ while for the lower symmetric compound in the CaBe$_2$Ge$_2$ structure (space group $P4/nmm$) we determined a much lower \neel temperature $T_{\rm N}=12\,\rm K$. Our magnetic characterization of the single crystals reveals that for both compounds the magnetic moments are aligned in the $a-a$ plane of the tetragonal lattice, but that the change of the symmetry strongly effects the inplane alignment of the moment orientation. For Ln$=$Er and Ho, we confirmed the existence of LnIr$_2$Si$_2$ in the space group $P4/nmm$. The magnetic properties of these lower symmetric compounds are in remarkable difference to their related compounds in the space group $I4/mmm$.

cond-mat.str-el↗

arXiv2021

Revealing three-dimensional quantum criticality by Sr-substitution in Han Purple

Classical and quantum phase transitions (QPTs), with their accompanying concepts of criticality and universality, are a cornerstone of statistical thermodynamics. An exemplary controlled QPT is the field-induced magnetic ordering of a gapped quantum magnet. Although numerous "quasi-one-dimensional" coupled spin-chain and -ladder materials are known whose ordering transition is three-dimensional (3D), quasi-2D systems are special for several physical reasons. Motivated by the ancient pigment Han Purple (BaCuSi$_{2}$O$_{6}$), a quasi-2D material displaying anomalous critical properties, we present a complete analysis of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$. We measure the zero-field magnetic excitations by neutron spectroscopy and deduce the magnetic Hamiltonian. We probe the field-induced transition by combining magnetization, specific-heat, torque and magnetocalorimetric measurements with low-temperature nuclear magnetic resonance studies near the QPT. By a Bayesian statistical analysis and large-scale Quantum Monte Carlo simulations, we demonstrate unambiguously that observable 3D quantum critical scaling is restored by the structural simplification arising from light Sr-substitution in Han Purple.

cond-mat.str-el↗

arXiv2021

Optical evidence of local and itinerant states in Ce- and Yb-heavy-fermion compounds

The electronic properties of Cerium (Ce) and ytterbium (Yb) intermetallic compounds may display a more local or more itinerant character depending on the interplay of the exchange interactions among the $4f$ electrons and the Kondo coupling between $4f$ and conduction electrons. For the more itinerant case, the materials form heavy-fermions once the Kondo effect is developed at low temperatures. Hence, a temperature variation occurs in the electronic structure that can be traced by investigating the optical conductivity ($σ(ω)$) spectra. Remarkably, the temperature variation in the $σ(ω)$ spectrum is still present in the more localized case, even though the Kondo effect is strongly suppressed. Here, we clarify the local and itinerant character in the electronic structure by investigating the temperature dependence in the $σ(ω)$ spectra of various Ce and Yb compounds with a tetragonal ThCr$_2$Si$_2$-type crystal structure. We explain the temperature change in a unified manner. Above temperatures of about 100 K, the temperature dependence of the $σ(ω)$ spectra is mainly due to the electron-phonon interaction, while the temperature dependence below is due to the Kondo effect.

cond-mat.str-el↗

arXiv2020

Terahertz Conductivity of Heavy-fermion Systems from Time-resolved Spectroscopy

The Drude model describes the free-electron conduction in simple metals, governed by the freedom that the mobile electrons have within the material. In strongly correlated systems, however, a significant deviation of the optical conductivity from the simple metallic Drude behavior is observed. Here, we investigate the optical conductivity of the heavy-fermion system CeCu$_{\mathrm{6-x}}$Au$_{\mathrm{x}}$, using time-resolved, phase-sensitive terahertz spectroscopy. Terahertz electric field creates two types of excitations in heavy-fermion materials: First, the intraband excitations that leave the heavy quasiparticles intact. Second, the resonant interband transitions between the heavy and light parts of the hybridized conduction band that break the Kondo singlet. We find that the Kondo-singlet breaking interband transitions do not create a Drude peak, while the Kondo-retaining intraband excitations yield the expected Drude response; thus, making it possible to separate these two fundamentally different correlated contributions to the optical conductivity.

cond-mat.str-el↗

arXiv2019

Bulk properties of single crystals of the valence-unstable compound SmRh$_2$Si$_2$

We present the crystal growth as well as the structural, chemical and physical chracterization of SmRh$_2$Si$_2$ single crystals. Their ground state is antiferromagnetic, as indicated by the behaviour of the magnetic susceptibility and the specific heat at the second order phase transition observed at T$_{\rm N}$ = 64 K. The Sommerfeld coefficient is small and similar to that of LuRh$_2$Si$_2$ with $γ_0\approx$ J/(molK$^2$). Susceptibility measurements show no Curie-Weiss behaviour at high temperatures which is a consequence of the large Van-Vleck contribution of the excited multiplets of Sm$^{3+}$. Previous angle-resolved photoemission studies showed that at 10 K, the valence of the Sm ions is smaller than three at the surface as well as in the bulk, suggesting a possible Kondo screening of the Sm$^{3+}$ ions. This could not be observed in our thermodynamic and transport measurements.

cond-mat.str-el↗

arXiv2019

Local study of the insulating quantum kagome antiferromagnets YCu3(OH)6OxCl3-x (x=0,1/3)

The quantum kagome antiferromagnets YCu3(OH)6OxCl3-x (x=0,1/3) are produced using a unified solid state synthesis route for polycrystalline samples. From structural refinements based on neutron diffraction data, we clarify the structure of the Y3Cu9(OH)18OCl8 (x=1/3) compound and provide a revised chemical formula. We use muon spin relaxation, as a local probe of magnetism, to investigate the exotic low temperature properties in the two compounds. In agreement with the low temperature neutron diffraction data, we find no evidence for long range ordering in both materials but they exhibit distinct ground states: while disordered static magnetism develops in the x=0 compound, we conclude on the stabilization of a quantum spin liquid in the x=1/3 one, since the local fields remain fully dynamical. Our findings are in contrast to previous reports based on thermodynamical measurements only. We then discuss their origin on the basis of structural details and specific heat measurements. In particular, the x=1/3 compound appears to realize an original spatially anisotropic kagome model.

cond-mat.str-el↗

arXiv2019

Kondo-lattice ferromagnets and their peculiar order along the magnetically hard axis

We show that Ce- and Yb-based Kondo-lattice ferromagnets order mainly along the magnetically hard direction of the ground state Kramers doublet determined by crystalline electric field (CEF). Here we argue that this peculiar phenomenon, that was believed to be rare, is instead the standard case. Moreover, it seems to be independent on the Curie temperature $T_\mathrm{C}$, crystalline structure, size of the ordered moment and type of ground state wave function. On the other hand, all these systems show the Kondo coherence maximum in the temperature dependence of the resistivity just above $T_\mathrm{C}$ which indicates a Kondo temperature of a few Kelvin. An important role of fluctuations is indicated by the non-mean-field like transition in specific heat measurements as well as by the suppression of this effect by a strong Ising-like anisotropy. We discuss possible theoretical scenarios.

cond-mat.str-el↗

arXiv2018

Kagome quantum spin systems in the atacamite family

We present the hydrothermal synthesis, as well as structural and chemical analysis of single crystals on the compounds EuCu$_{3}$(OH)$_{6}$Cl$_{3}$, Zn$_{x}$Cu$_{4-x}$(OH)$_{6}$(NO$_{3}$)$_{2}$ and haydeeite, MgCu$_{3}$(OH)$_{6}$Cl$_{2}$ all arising from the atacamite family. Magnetic and specific-heat measurements down to 1.8 K are carried out for these systems. EuCu$_{3}$(OH)$_{6}$Cl$_{3}$ has a frustrated antiferromagnetic Cu$^{2+}$ ground state with order at 15 K, a strong anisotropy and increased magnetization from Van Vleck paramagnetic Eu$^{3+}$ contributions. ZnCu$_{3}$(OH)$_{6}$(NO$_{3}$)$_{2}$ reveals antiferromagnetic order at 9 K and measurements on haydeeite single crystals confirm the ferromagnetic order at 4.2 K with the easy axis within the kagome plane. These results prove that the atacamite family presents a broad class of materials with interesting magnetic ground states.

cond-mat.str-el↗

arXiv2018

Magnetic anisotropy in HoIr$_2$Si$_2$ ($I4/mmm$)

Single crystals of HoIr$_2$Si$_2$ with the body-centered ThCr$_2$Si$_2$-type structure ($I4/mmm$) were grown by Bridgman method from indium flux. Single crystal structure determination yielded a Si-z position of 0.378(1) in the structure. We excluded the presence of the high temperature phase with the primitive CaBe$_2$Ge$_2$-type structure ($P 4/n m m$) by powder X-ray diffraction. Magnetic measurements on the single crystals yield a Neel temperature of $T_{\rm N}=22\,\rm K$. In the inverse magnetic susceptibility a strong anisotropy with Weiss temperatures $Θ_{W}^{001}=26\,\rm K$ and $Θ_{W}^{100}=-26\,\rm K$ occurs above $T_{\rm N}$. The effective magnetic moment $μ_{\rm eff}^{001}=10.64μ_{B}$ and $μ_{\rm eff}^{100}=10.53μ_{B}$ is close to the expected value for a free Ho$^{3+}$ ion, $μ_{\rm eff}^{calc}=10.6μ_{B}$. The field dependent magnetization shows a step-like behaviour due to crystalline electric field effects.

cond-mat.str-el↗

arXiv2018

Interplay between structure and magnetism in the low-dimensional spin system $K(C_8H_{16}O_4)_2CuCl_3{*}H_2O$

Materials based on a crown ether complex together with magnetic ions, especially Cu(II), can be used to synthesize new low dimesional quantum spin systems. We have prepared the new crown ether complex Di-μ-chloro-bis(12-crown-4)-aquqdichloro-copper(II)-potassium, $K(C_8H_{16}O_4)_2CuCl_3{*}H_2O$ (1), determined its structure, and analyzed its magnetic properties. Complex (1) has a monoclinic structure and crystallizes in space group $P2_1/n$ with the lattice parameters of $a=9.5976(5)Å$, $b=11.9814Å, c=21.8713Å$ and $β=100.945(4)°$. The magnetic properties of this compound have been investigated in the temperature range 1.8 K - 300 K. The magnetic susceptibility shows a maximum at 23 K, but no 3-D long range magnetic order down to 1.8 K. The S=1/2 Cu(II) ions form antiferromagnetically coupled dimers with Cu-Cl distances of $2.2554(8)Å$ and $4.683(6)Å$, and a Cu-Cl-Cu angle of $115.12(2)°$ with $2J_{dimer}=-2.96meV (-23.78 cm^{-1})$. The influence of $H_2O$ on the Cl-Cu-Cl exchange path is analyzed. Our results show that the values of the singlet-triplet splitting are increasing considering $H_2O$ molecules in the bridging interaction. This is supported by Density functional theory (DFT) calculations of coupling constants with Perdew and Wang (PWC), Perdew, Burke and Ernzenrhof (PBE) and strongly constrained and appropriately normed (SCAN) exchange-correlation function show excellent agreement for the studied compound.

cond-mat.mtrl-sci↗

arXiv2017

Nature of optical excitations in the frustrated kagome compound Herbertsmithite

Optical conductivity measurements are combined with density functional theory calculations in order to understand the electrodynamic response of the frustrated Mott insulators Herbertsmithite $\mathrm{ZnCu_{3}(OH)_{6}Cl_{2}}$ and the closely-related kagome-lattice compound $\mathrm{Y_{3}Cu_{9}(OH)_{19}Cl_{8}}$. We identify these materials as charge-transfer rather than Mott-Hubbard insulators, similar to the high-$T_c$ cuprate parent compounds. The band edge is at 3.3 and 3.6 eV, respectively, establishing the insulating nature of these compounds. Inside the gap, we observe dipole-forbidden local electronic transitions between the Cu $3d$ orbitals in the range 1--2 eV. With the help of \textit{ab initio} calculations we demonstrate that the electrodynamic response in these systems is directly related to the role of on-site Coulomb repulsion: while charge-transfer processes have their origin on transitions between the ligand band and the Cu $3d$ upper Hubbard band, \textit{local} $d$-$d$ excitations remain rather unaffected by correlations.

cond-mat.str-el↗

arXiv2017

Angle-dependent electron spin resonance of YbRh$_2$Si$_2$ measured with planar microwave resonators and in-situ rotation

We present a new experimental approach to investigate the magnetic properties of the anisotropic heavy-fermion system YbRh$_2$Si$_2$ as a function of crystallographic orientation. Angle-dependent electron spin resonance (ESR) measurements are performed at a low temperature of 1.6 K and at an ESR frequency of 4.4 GHz utilizing a superconducting planar microwave resonator in a $^4$He-cryostat in combination with in-situ sample rotation. The obtained ESR g-factor of YbRh$_2$Si$_2$ as a function of the crystallographic angle is consistent with results of previous measurements using conventional ESR spectrometers at higher frequencies and fields. Perspectives to implement this experimental approach into a dilution refrigerator and to reach the magnetically ordered phase of YbRh$_2$Si$_2$ are discussed.

cond-mat.str-el↗

arXiv2017

Crystal growth with oxygen partial pressure of the $BaCuSi_2O_6$ and $Ba_{1-x}Sr_xCuSi_2O_6$ spin dimer compounds

$BaCuSi_2O_6$ is a quasi-two dimensional spin dimer system and a model material for studying Bose-Einstein condensation (BEC) of magnons in high magnetic fields. The new $Ba_{1-x}Sr_xCuSi_2O_6$ mixed system, which can be grown with x < 0.3, and $BaCuSi_2O_6$, both grown by using a crystal growth method with enhanced oxygen partial pressure, have the same tetragonal structure ($I4_1/acd$) at room temperature. The mixed system shows no structural phase transition, so that the tetragonal structure is stable down to low temperatures. The oxygen partial pressure acts as control parameter for the growth process. A detailed understanding of the crystal structure depending on the oxygen content will enable the study of the spin dynamics of field-induced order states in this model magnetic compound of high current interest with only one type of dimer layers, which shows the same distance between the Cu atoms, in the structure.

cond-mat.mtrl-sci↗

arXiv2017

Emergence of superconductivity in the canonical heavy-electron metal YbRh2Si2

We report magnetic and calorimetric measurements down to T = 1 mK on the canonical heavy-electron metal YbRh2Si2. The data reveal the development of nuclear antiferromagnetic order slightly above 2 mK. The latter weakens the primary electronic antiferromagnetism, thereby paving the way for heavy-electron superconductivity below Tc = 2 mK. Our results demonstrate that superconductivity driven by quantum criticality is a general phenomenon.

cond-mat.str-el↗

arXiv2017

Strong magnetic frustration in Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$: a distorted kagome antiferromagnet

We present the crystal structure and magnetic properties of Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$, a stoichiometric frustrated quantum spin system with slightly distorted kagome layers. Single crystals of Y$_{3}$Cu$_{9}$(OH)$_{19}$Cl$_{8}$ were grown under hydrothermal conditions. The structure was determined from single crystal X-ray diffraction and confirmed by neutron powder diffraction. The observed structure reveals two different Cu-positions leading to a slightly distored kagome layer in contrast to the closely related YCu$_{3}$(OH)$_{6}$Cl$_{3}$. Curie-Weiss behavior at high-temperatures with a Weiss-temperature $θ_{W}$ of the order of $-100$ K, shows a large dominant antiferromagnetic coupling within the kagome planes. Specific-heat and magnetization measurements on single crystals reveal an antiferromagnetic transition at T$_{N}=2.2$ K indicating a pronounced frustration parameter of $θ_{W}/T_{N}\approx50$. Optical transmission experiments on powder samples and single crystals confirm the structural findings. Specific-heat measurements on YCu$_{3}$(OH)$_{6}$Cl$_{3}$ down to 0.4 K confirm the proposed quantum spin-liquid state of that system. Therefore, the two Y-Cu-OH-Cl compounds present a unique setting to investigate closely related structures with a spin-liquid state and a strongly frustrated AFM ordered state, by slightly releasing the frustration in a kagome lattice.

cond-mat.str-el↗

arXiv2016

Single crystal growth and characterization of GdRh$_2$Si$_2$

High-temperature indium flux growth was applied to prepare single crystals of GdRh$_2$Si$_2$ by a modified Bridgman method leading to mm-sized single crystals with a platelet habitus. Specific heat and susceptibility data of GdRh$_2$Si$_2$ exhibit a pronounced anomaly at $T_N = 107\rm \,K$, where the AFM ordering sets in. Magnetic measurements on the single crystals were performed down to $T = 2$\,K in external fields from B = 0 - 9\,T applied along the $[100]$-, $[110]$- and $[001]$-direction of the tetragonal lattice. The effective magnetic moment determined from a Curie-Weiss fit agrees well with values from literature, and is larger than the theoretically predicted value. Electrical transport data recorded for current flow parallel and perpendicular to the $[001]$-direction show a large anisotropy below $T_N$. The residual resistivity ratio $\rm RRR=ρ_{300K}/ρ_{0}\sim 23$ demonstrates that we succeeded in preparing high-quality crystals using high-temperature indium flux-growth.

cond-mat.str-el↗

arXiv2016

Characterization of YbNi$_4$(P$_{1-{\it x}}$As$_{\it x}$)$_2$, $x = 0, 0.2$ single crystals grown by Czochralski method

We have investigated large single crystals of YbNi$_4$P$_2$ that were grown from a levitating melt by the Czochralski method. The new samples facilitate the determination of the absolute values of the electrical resistivity. Phase pure polycrystalline samples of the non-magnetic reference LuNi$_4$P$_2$ were prepared and the electrical resistivity was measured. Furthermore we have grown a single crystal of the As substituted compound YbNi$_4$(P$_{1-{\it x}}$As$_{\it x}$)$_2$, $x = 0.2$ and investigated the homogenity of the As distribution.

cond-mat.str-el↗

arXiv2016

Metallic coplanar resonators optimized for low-temperature measurements

Metallic coplanar microwave resonators are widely employed at room temperature, but their low-temperature performance has received little attention so far. We characterize compact copper coplanar resonators with multiple modes from 2.5 to 20 GHz at temperatures as low as 5 K. We investigate the influence of center conductor width (20 to 100 μm) and coupling gap size (10 to 50 μm), and we observe a strong increase of quality factor (Q) for wider center conductors, reaching values up to 470. The magnetic-field dependence of the resonators is weak, with a maximum change in Q of 3.5% for an applied field of 7 T. This makes these metallic resonators well suitable for magnetic resonance studies, as we document with electron spin resonance (ESR) measurements at multiple resonance frequencies.

cond-mat.mes-hall↗