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L. H. Tjeng

Publications and source records attributed to L. H. Tjeng.

At least 19 recordsLinked to original sources

Synthesis and structural validation of close-to-stoichiometric NiTe$_2$ single crystals

We report the synthesis of stoichiometric NiTe$_{2}$ single crystals via chemical vapor transport together with precise structural characterization. A combined analysis using powder and single crystal X-ray diffraction (XRD) was performed to determine lattice parameters and structural details. High-resolution single crystal XRD reveals no evidence of interstitial nickel, confirming a close-to-stoichiometric composition. This work establishes a reliable benchmark for the crystal structure of stoichiometric NiTe$_{2}$, offering a reference for future studies on its physical properties.

cond-mat.mtrl-sci

Single-Crystal Growth and Magnetic, Electronic Properties of the FCC Antiferromagnet Ba_2CoMoO_6

This work presents a comprehensive investigation of the structural, magnetic, and electronic properties of the double perovskite Ba$_2$CoMoO$_6$ (BCMO). Single crystals were grown via floating-zone and Czochralski techniques and characterized using a set of complementary methods. X-ray diffraction analysis confirmed that BCMO crystallizes in a face-centered cubic structure with space group $Fm\bar{3}m$. Magnetic susceptibility measurements reveal antiferromagnetic ordering below $T_\mathrm{N} = 20.1(1)$~K, with a spin-flop transition at $μ_0 H = 2.65$~T. Heat-capacity measurements and entropy analysis, $ΔS \approx 0.95\,R\ln 2$, are consistent with a $J_\mathrm{eff} = \tfrac{1}{2}$ effective ground state for Co$^{2+}$ ions. X-ray absorption spectroscopy at the Co~$L_{2,3}$ edges provides insight into the local electronic structure, revealing spin-orbit and crystal-field splitting effects; cluster-model calculations constrained by the XAS spectra yield a Landé $g$ factor $g = 4.52$, consistent with a spin-orbit-entangled $J_\mathrm{eff} = \tfrac{1}{2}$ ground state. Surface photovoltage spectroscopy reveals a strong optical response with a prominent feature at $2.65$~eV. These findings advance the understanding of face-centered cubic lattice antiferromagnets with strong spin-orbit coupling and suggest the technological promise of BCMO for spintronic and energy-conversion applications.

cond-mat.str-el

Direct Evidence of a Near-Ideal Jeff = 1/2 Ground State in Triangular-Lattice Na2BaCo(PO4)2

We investigated the local Co 3d electronic structure of Na2BaCo(PO4)2 using polarization-dependent X-ray absorption spectroscopy (XAS) in combination with full multiplet cluster calculations. We employed the line-fitting inverse partial fluorescence yield (IPFY) technique to obtain accurate XAS spectra from strong insulating materials. Our combined experimental and theoretical analysis reveals a very small effective trigonal distortion of only 11 meV in the CoO6 octahedra, indicating a close to ideal condition to render a ground state with the Jeff = 1/2 character. With our cluster model we were also able to simulate magnetic susceptibility measurements along different directions in the crystal. These findings highlight Na2BaCo(PO4)2 as a promising platform for exploring exotic magnetic phenomena associated with Jeff = 1/2 ground states on triangular lattices.

cond-mat.str-el

Trigonal distortion in the Kitaev candidate honeycomb magnet BaCo2(AsO4)2

We conducted x-ray absorption (XAS) and magnetic circular dichroism (XMCD) measurements at the Co $L_{2,3}$ edges on single crystals of the Kitaev candidate honeycomb lattice compound BaCo$_2$(AsO$_4$)$_2$. The measurements employed the inverse partial fluorescence yield technique, which is ideal for acquiring reliable x-ray absorption spectra from highly insulating samples, enabling precise quantitative analysis. Our experimental results revealed a significant linear dichroic signal, indicating strong trigonal distortion in the CoO$_{6}$ octahedra in BaCo$_2$(AsO$_4$)$_2$. We performed a detailed analysis of the experimental XAS and XMCD spectra using a full-multiplet configuration-interaction cluster model. This analysis unveiled that the $t_{2g}$ hole density is predominantly localized in the $a_{1g}$ orbital. Through XMCD sum rules and theoretical calculations, we quantified both the spin and orbital magnetic moments. Our study demonstrates that the local electronic structure of the CoO$_{6}$ octahedra displays an effective trigonal distortion of approximately $-0.114$ eV. This distortion is larger than the Co $3d$ spin-orbit coupling constant, emphasizing the crucial impact of local structural distortions on the electronic and magnetic properties of BaCo$_2$(AsO$_4$)$_2$.

cond-mat.str-el

Linear dichroic x-ray absorption response of Ti-Ti dimers along the $c$ axis in Ti$_2$O$_3$ upon Mg substitution

Corundum oxide Ti$_2$O$_3$ shows the metal-insulator transition around 400-600 K accompanying the nearest Ti$^{3+}$-Ti$^{3+}$ bond ($a_{1g}a_{1g}$ singlet state) formation along the $c$ axis. In order to clarify the hole-doping effect for the $a_{1g}a_{1g}$ singlet bond in Ti$_2$O$_3$, we investigated Ti $3d$ orbital anisotropy between corundum-type Ti$_2$O$_3$ and ilmenite-type MgTiO$_3$ using linear dichroism of soft x-ray absorption spectroscopy of the Ti $L_{2,3}$ edge. From the linear dichroic spectral weight in Mg$_y$Ti$_{2-y}$O$_3$, we confirmed that the $a_{1g}a_{1g}$ state is dominant not only in $y=0.01$ (almost Ti$_2$O$_3$), but also in $y = 0.29$, indicating that the Ti-Ti bond survives against a certain level of hole doping. In $y=0.63$ corresponding to 46% hole doping per Ti, the $3d$ orbital symmetry changes from $a_{1g}$ to $e_g^π$.

cond-mat.str-el

Single-crystal epitaxial europium iron garnet films with strain-induced perpendicular magnetic anisotropy: structural, strain, magnetic, and spin transport properties

Single-crystal europium iron garnet (EuIG) thin films epitaxially strain-grown on gadolinium gallium garnet (GGG)(100) substrates using off-axis sputtering have strain-induced perpendicular magnetic anisotropy (PMA). By varying the sputtering conditions, we have tuned the europium/iron (Eu/Fe) composition ratios in the films to tailor the film strains. The films exhibited an extremely smooth, particle-free surface with roughness as low as 0.1 nm as observed using atomic force microscopy. High-resolution x-ray diffraction analysis and reciprocal space maps showed in-plane epitaxial film growth, very smooth film/substrate interface, excellent film crystallinity with a small full width at half maximum of 0.012$^{\circ}$ in the rocking curve scans, and an in-plane compressive strain without relaxation. In addition, spherical aberration-corrected scanning transmission electron microscopy showed an atomically abrupt interface between the EuIG film and GGG. The measured squarish out-of-plane magnetization-field hysteresis loops by vibrating sample magnetometry in conjunction with the measurements from angle-dependent x-ray magnetic dichroism demonstrated the PMA in the films. We have tailored the magnetic properties of the EuIG thin films, including saturation magnetization ranging from 71.91 to 124.51 emu/c.c. (increase with the (Eu/Fe) ratios), coercive field from 27 to 157.64 Oe, and the strength of PMA field ($H_\bot$) increasing from 4.21 to 18.87 kOe with the in-plane compressive strain from -0.774 to -1.044%. We have also investigated spin transport in Pt/EuIG bi-layer structure and evaluated the real part of spin mixing conductance to be $3.48\times10^{14} Ω^{-1}m^{-2}$. We demonstrated the current-induced magnetization switching with a low critical switching current density of $3.5\times10^6 A/cm^2$, showing excellent potential for low-dissipation spintronic devices.

cond-mat.mtrl-sci

CaCu$_3$Ru$_4$O$_{12}$: a high Kondo-temperature transition metal oxide

We present a comprehensive study of CaCu$_3$Ru$_4$O$_{12}$ using bulk sensitive hard and soft x-ray spectroscopy combined with local-density approximation (LDA) + dynamical mean-field theory (DMFT) calculations. Correlation effects on both the Cu and Ru ions can be observed. From the Cu $2p$ core level spectra we deduce the presence of magnetic Cu$^{2+}$ ions hybridized with a reservoir of itinerant electrons. The strong photon energy dependence of the valence band allows us to disentangle the Ru, Cu, and O contributions and thus to optimize the DMFT calculations. The calculated spin and charge susceptibilities show that the transition metal oxide CaCu$_3$Ru$_4$O$_{12}$ must be classified as a Kondo system and that the Kondo temperature is in the range of 500-1000 K.

cond-mat.str-el

Emergent 1/3 magnetization plateaus in pyroxene CoGeO$_3$

Despite the absence of an apparent triangular pattern in the crystal structure, we observe unusually well pronounced 1/3 magnetization plateaus in the quasi one-dimensional Ising spin chain compound CoGeO$_3$ which belongs to the class of pyroxene minerals. We succeeded in uncovering the detailed microscopic spin structure of the 1/3 magnetization plateau phase by means of neutron diffraction. We observed changes of the initial antiferromagnetic zero-field spin structure that are resembling a regular formation of antiferromagnetic "domain wall boundaries", resulting in a kind of modulated magnetic structure with 1/3-integer propagation vector. The net ferromagnetic moment emerges at these "domain walls" whereas two third of all antiferromagnetic chain alignments can be still preserved. We propose a microscopic model on the basis of an anisotropic frustrated square lattice to explain the observations.

cond-mat.str-el

Single crystal growth and physical properties of pyroxene CoGeO$_3$

We report on the synthesis and physical properties of cm-sized CoGeO$_3$ single crystals grown in a high pressure mirror furnace at pressures of 80~bar. Direction dependent magnetic susceptibility measurements on our single crystals reveal highly anisotropic magnetic properties that we attribute to the impact of strong single ion anisotropy appearing in this system with T$_N$~$\sim$~33.5~K. Furthermore, we observe effective magnetic moments that are exceeding the spin only values of the Co ions which reveals the presence of sizable orbital moments in CoGeO$_3$.

cond-mat.mtrl-sci

Crystal structure and properties of iron-based spin-chain compound Ba9Fe3Se15

We report the synthesis of a new quasi one-dimensional (1D) iron selenide. Ba9Fe3Se15 was synthesized at high temperature and high pressure of 5.5 GPa and systematically studied via structural, magnetic and transport measurements at ambient and at high-pressures. Ba9Fe3Se15 crystallizes in a monoclinic structure and consists of face-sharing FeSe6 octahedral chains along the c axis. At ambient pressure it exhibits an insulating behavior with a band gap ~460 meV and undergoes a ferrimagnet-like phase transition at 14 K. Under high pressure, a complete metallization occurs at ~29 GPa, which is accompanied by a spin state crossover from high spin (HS) state to low spin (LS) state. The LS appears for pressures P >36 GPa.

cond-mat.supr-con

Selective orbital imaging of excited states with x-ray spectroscopy: the example of $α$-MnS

Herein we show that non-resonant inelastic x-ray scattering involving an $s$ core level is a powerful spectroscopic method to characterize the excited states of transition metal compounds. The spherical charge distribution of the $s$ core hole allows the orientational dependence of the intensities of the various spectral features to produce a spatial charge image of the associated multiplet states in a straightforward manner, thereby facilitating the identification of their orbital character. In addition, the $s$ core hole does not add an extra orbital angular momentum component to the multiplet structure so that the well-established Sugano-Tanabe-Kamimura diagrams can be used for the analysis of the spectra. For $α$-MnS we observe the spherical charge density corresponding to its high spin $3d^5$ ($^6A_1$) ground state configuration and we were able to selectively image its excited states and identify them as $t_{2g}$ ($^5T_2$) and $e_g$ ($^5E$) with an energy splitting $10Dq$ of 0.78\,eV.

cond-mat.str-el

Charge disproportionation and nano phase separation in $R$SrNiO$_4$

We have successfully grown centimeter-sized layered $R$SrNiO$_4$ single crystals under high oxygen pressures of 120 bar by the floating zone technique. This enabled us to perform neutron scattering experiments where we observe close to quarter-integer magnetic peaks below $\sim$77 K that are accompanied by steep upwards dispersing spin excitations. Within the high-frequency Ni-O bond stretching phonon dispersion, a softening at the propagation vector for a checkerboard modulation can be observed. Together with our spin wave simulations these observations reveal that this Ni$^{3+}$ system exhibits charge disproportionation with charges segregating into a checkerboard pattern within a nano phase separation scenario rather than showing a Jahn-Teller effect.

cond-mat.str-el

Interfacing topological insulators and ferrimagnets: Bi$_2$Te$_3$ and Fe$_3$O$_4$ heterostructures grown by molecular beam epitaxy

Relying on the magnetism induced by the proximity effect in heterostructures of topological insulators and magnetic insulators is one of the promising routes to achieve the quantum anomalous Hall effect. Here we investigate heterostructures of Bi$_2$Te$_3$ and Fe$_3$O$_4$. By growing two different types of heterostructures by molecular beam epitaxy, Fe$_3$O$_4$ on Bi$_2$Te$_3$ and Bi$_2$Te$_3$ on Fe$_3$O$_4$, we explore differences in chemical stability, crystalline quality, electronic structure, and transport properties. We find the heterostructure Bi$_2$Te$_3$ on Fe$_3$O$_4$ to be a more viable approach, with transport signatures in agreement with a gap opening in the topological surface states.

cond-mat.mtrl-sci

Charge transfer energy in iridates: a hard x-ray photoelectron spectroscopy study

We have investigated the electronic structure of iridates in the double perovskite crystal structure containing either Ir$^{4+}$ or Ir$^{5+}$ using hard x-ray photoelectron spectroscopy. The experimental valence band spectra can be well reproduced using tight binding calculations including only the Ir $5d$, O $2p$ and O $2s$ orbitals with parameters based on the downfolding of the density-functional band structure results. We found that regardless of the A and B cations, the A$_2$BIrO$_6$ iridates have essentially zero O $2p$ to Ir $5d$ charge transfer energies. Hence, double perovskite iridates turn out to be extremely covalent systems with the consequence being that the magnetic exchange interactions become very long-ranged, thereby hampering the materialization of the long-sought Kitaev physics. Nevertheless, it still would be possible to realize a spin-liquid system using the iridates with a proper tuning of the various competing exchange interactions.

cond-mat.str-el

Orientation of ground-state orbital in CeCoIn$_5$ and CeRhIn$_5$

We present core level non-resonant inelastic x-ray scattering (NIXS) data of the heavy fermion compounds CeCoIn$_5$ and CeRhIn$_5$ measured at the Ce $N_{4,5}$-edges. The higher than dipole transitions in NIXS allow determining the orientation of the $Γ_7$ crystal-field ground-state orbital within the unit cell. The crystal-field parameters of the Ce$M$In$_5$ compounds and related substitution phase diagrams have been investigated in great detail in the past; however, whether the ground-state wavefunction is the $Γ_7^+$ ($x^2\,-\,y^2$) or $Γ_7^-$ ($xy$ orientation) remained undetermined. We show that the $Γ_7^-$ doublet with lobes along the (110) direction forms the ground state in CeCoIn$_5$ and CeRhIn$_5$. For CeCoIn$_5$, however, we find also some contribution of the first excited state crystal-field state in the ground state due to the stronger hybridization of 4$f$ and conduction electrons, suggesting a smaller $α^2$ value than originally anticipated from x-ray absorption. A comparison is made to the results of existing density functional theory plus dynamical mean-field theory calculations.

cond-mat.str-el

Nature of the magnetism of iridium in the double perovskite Sr2CoIrO6

We report on our investigation on the magnetism of the iridate double perovskite Sr$_2$CoIrO$_6$, a nominally Ir$^{5+}$ Van Vleck $J_{eff}=0$ system. Using x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectroscopy at the Ir-$L_{2,3}$ edges, we found a nearly zero orbital contribution to the magnetic moment and thus an apparent breakdown of the $J_{eff}=0$ ground state. By carrying out also XAS and XMCD experiments at the Co-$L_{2,3}$ edges and by performing detailed full atomic multiplet calculations to simulate all spectra, we discovered that the compound consists of about 90% Ir$^{5+}$ ($J_{eff}=0$) and Co$^{3+}$ ($S=2$) and 10% Ir$^{6+}$ ($S=3/2$) and Co$^{2+}$ ($S=3/2$). The magnetic signal of this minority Ir$^{6+}$ component is almost equally strong as that of the main Ir$^{5+}$ component. We infer that there is a competition between the Ir$^{5+}$-Co$^{3+}$ and the Ir$^{6+}$-Co$^{2+}$ configurations in this stoichiometric compound.

cond-mat.str-el

Spin-orbit coupling and crystal-field distortions for a low-spin $3d^5$ state in BaCoO$_{3}$

We have studied the electronic structure of BaCoO$_3$ using soft x-ray absorption spectroscopy at the Co-$L_{2,3}$ and O-$K$ edges, magnetic circular dichroism at the Co-$L_{2,3}$ edges, as well as valence band hard x-ray photoelectron spectroscopy. The quantitative analysis of the spectra established that the Co ions are in the formal low-spin tetravalent 3$d^5$ state and that the system is a negative charge transfer Mott insulator. The spin-orbit coupling plays also an important role for the magnetism of the system. At the same time, a trigonal crystal field is present with sufficient strength to bring the 3$d^5$ ion away from the $J_{eff} = 1/2$ state. The sign of this crystal field is such that the $a_{1g}$ orbital is doubly occupied, explaining the absence of a Peierl's transition in this system which consists of chains of face-sharing CoO$_6$ octahedra. Moreover, with one hole residing in the $e_g^π$, the presence of an orbital moment and strong magneto-crystalline anisotropy can be understood. Yet, we also infer that crystal fields with lower symmetry must be present to reproduce the measured orbital moment quantitatively, thereby suggesting the possibility for orbital ordering to occur in BaCoO$_3$.

cond-mat.str-el

Strain induced changes of electronic properties of B-site ordered double perovskite Sr$_2$CoIrO$_6$ thin films

B-site ordered thin films of double perovskite Sr$_2$CoIrO$_6$ were epitaxially grown by a metal-organic aerosol deposition technique on various substrates, actuating different strain states. X-ray diffraction, transmission electron microscopy and polarized far-field Raman spectroscopy confirm the strained epitaxial growth on all used substrates. Polarization dependent Co $L_{2,3}$ X-ray absorption spectroscopy reveals a change of the magnetic easy axis of the antiferromagnetically ordered (high-spin) Co$^{3+}$ sublattice within the strain series. By reversing the applied strain direction from tensile to compressive, the easy axis changes abruptly from in-plane to out-of-plane orientation. The low-temperature magnetoresistance changes its sign respectively and is described by a combination of weak anti-localization and anisotropic magnetoresistance effects.

cond-mat.str-el