arXiv subjects

C. T. Chen

Publications and source records attributed to C. T. Chen.

At least 37 records · Page 2Linked to original sources

arXiv2021

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↗

arXiv2020

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↗

arXiv2020

Development of the Soft X-ray AGM-AGS RIXS Beamline at Taiwan Photon Source

We report on the development of a high-resolution and highly efficient beamline for soft-X-ray resonant inelastic X-ray scattering (RIXS) located at Taiwan Photon Source. This beamline adopts an optical design that uses an active grating monochromator (AGM) and an active grating spectrometer (AGS) to implement the energy compensation principle of grating dispersion. Active gratings are utilized to diminish defocus, coma and higher-order aberrations as well as to decrease the slope errors caused by thermal deformation and optical polishing. The AGS is mounted on a rotatable granite platform to enable momentum-resolved RIXS measurements with scattering angle over a wide range. Several high-precision instruments developed in house for this beamline are briefly described. The best energy resolution obtained from this AGM-AGS beamline was 12.4 meV at 530 eV, achieving a resolving power 42,000, while the bandwidth of the incident soft X-rays was kept at 0.5 eV. To demonstrate the scientific impacts of high-resolution RIXS, we present an example of momentum-resolved RIXS measurements on a high-temperature superconducting cuprate, La$_{2-x}$Sr$_x$CuO$_4$. The measurements reveal the A$_{1g}$ apical oxygen phonons in superconducting cuprates, opening a new opportunity to investigate the coupling between these phonons and charge density waves.

physics.ins-det↗

arXiv2020

Electronic structure investigation of GdNi using X-ray absorption, magnetic circular dichroism and hard x-ray photoemission spectroscopy

GdNi is a ferrimagnetic material with a Curie temperature Tc = 69 K which exhibits a large magnetocaloric effect, making it useful for magnetic refrigerator applications. We investigate the electronic structure of GdNi by carrying out x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) at T = 25 K in the ferrimagnetic phase. We analyze the Gd M$_{4,5}$-edge ($3d$ - $4f$) and Ni L$_{2,3}$-edge ($2p$ - $3d$) spectra using atomic multiplet and cluster model calculations, respectively. The atomic multiplet calculation for Gd M$_{4,5}$-edge XAS indicates that Gd is trivalent in GdNi, consistent with localized $4f$ states. On the other hand, a model cluster calculation for Ni L$_{2,3}$-edge XAS shows that Ni is effectively divalent in GdNi and strongly hybridized with nearest neighbour Gd states, resulting in a $d$-electron count of 8.57. The Gd M$_{4,5}$-edge XMCD spectrum is consistent with a ground state configuration of S = 7/2 and L=0. The Ni L$_{2,3}$-edge XMCD results indicate that the antiferromagnetically aligned Ni moments exhibit a small but finite magnetic moment ( $m_{tot}$ $\sim$ 0.12 $μ_B$ ) with the ratio $m_{o}/m_{s}$ $\sim$ 0.11. Valence band hard x-ray photoemission spectroscopy shows Ni $3d$ features at the Fermi level, confirming a partially filled $3d$ band, while the Gd $4f$ states are at high binding energies away from the Fermi level. The results indicate that the Ni $3d$ band is not fully occupied and contradicts the charge-transfer model for rare-earth based alloys. The obtained electronic parameters indicate that GdNi is a strongly correlated charge transfer metal with the Ni on-site Coulomb energy being much larger than the effective charge-transfer energy between the Ni $3d$ and Gd $4f$ states.

cond-mat.str-el↗

arXiv2019

Superconductivity in a unique type of copper oxide

The mechanism of superconductivity in cuprates remains one of the big challenges of condensed matter physics.High Tc cuprates crystallize into layered perovskite structure featuring copper oxygen octahedral coordination. Due to the Jahn Teller effect in combination with the strong static Coulomb interaction, the octahedra in high Tc cuprates are elongated along the c axis, leading to a 3dx2-y2 orbital at the top of the band structure wherein the doped holes reside.This scenario gives rise to two dimensional characteristics in high Tc cuprates that favor d wave pairing symmetry. Here we report superconductivity in a cuprate Ba2CuO4-y wherein the local octahedron is in a very exceptional compressed version.The Ba2CuO4-y compound was synthesized at high pressure at high temperatures, and shows bulk superconductivity with critical temperature Tc above 70 K at ambient conditions. This superconducting transition temperature is more than 30 K higher than the Tc for the isostructural counterparts based on classical La2CuO4. X-ray absorption measurements indicate the heavily doped nature of the Ba2CuO4-y superconductor. In compressed octahedron the 3d3z2-r2 orbital will be lifted above the 3dx2-y2 orbital, leading to significant three dimensional nature in addition to the conventional 3dx2-y2 orbital. This work sheds important new light on advancing our comprehensive understanding of the superconducting mechanism of high Tc in cuprate materials.

cond-mat.supr-con↗

arXiv2019

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↗

arXiv2018

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↗

arXiv2017

The $c$-axis dimer and its electronic break-up: the insulator-to-metal transition in Ti$_2$O$_3$

We report on our investigation of the electronic structure of Ti$_2$O$_3$ using (hard) x-ray photoelectron and soft x-ray absorption spectroscopy. From the distinct satellite structures in the spectra we have been able to establish unambiguously that the Ti-Ti $c$-axis dimer in the corundum crystal structure is electronically present and forms an $a_{1g}a_{1g}$ molecular singlet in the low temperature insulating phase. Upon heating we observed a considerable spectral weight transfer to lower energies with orbital reconstruction. The insulator-metal transition may be viewed as a transition from a solid of isolated Ti-Ti molecules into a solid of electronically partially broken dimers where the Ti ions acquire additional hopping in the $a$-$b$ plane via the $e_g^π$ channel, the opening of which requires the consideration of the multiplet structure of the on-site Coulomb interaction.

cond-mat.str-el↗

arXiv2017

Electronic signature of the vacancy ordering in NbO (Nb3O3)

We investigated the electronic structure of the vacancy-ordered 4d-transition metal monoxide NbO (Nb3O3) using angle-integrated soft- and hard-x-ray photoelectron spectroscopy as well as ultra-violet angle-resolved photoelectron spectroscopy. We found that density-functional-based band structure calculations can describe the spectral features accurately provided that self-interaction effects are taken into account. In the angle-resolved spectra we were able to identify the so-called vacancy band that characterizes the ordering of the vacancies. This together with the band structure results indicates the important role of the very large inter-Nb-4d hybridization for the formation of the ordered vacancies and the high thermal stability of the ordered structure of niobium monoxide.

cond-mat.mtrl-sci↗

arXiv2017

Coulomb correlations intertwined with spin and orbital excitations in LaCoO$_3$

We carried out temperature-dependent (20 - 550 K) measurements of resonant inelastic X-ray scattering on LaCoO$_3$ to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantized the renormalized crystal-field excitation energies and spin-state populations. We show that the screening of the on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO$_3$. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition.

cond-mat.str-el↗

arXiv2016

Dynamic atomic reconstruction: how Fe3O4 thin films evade polar catastrophe for epitaxy

Polar catastrophe at the interface of oxide materials with strongly correlated electrons has triggered a flurry of new research activities. The expectations are that the design of such advanced interfaces will become a powerful route to engineer devices with novel functionalities. Here we investigate the initial stages of growth and the electronic structure of the spintronic Fe3O4/MgO (001) interface. Using soft x-ray absorption spectroscopy we have discovered that the so-called A-sites are completely missing in the first Fe3O4 monolayer. This allows us to develop an unexpected but elegant growth principle in which during deposition the Fe atoms are constantly on the move to solve the divergent electrostatic potential problem, thereby ensuring epitaxy and stoichiometry at the same time. This growth principle provides a new perspective for the design of interfaces.

cond-mat.mtrl-sci↗

arXiv2016

Orbital engineering in nickelate heterostructures driven by anisotropic oxygen hybridization rather than orbital energy levels

Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking $\mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni $3d$ orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O $K$-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena.

cond-mat.str-el↗

arXiv2016

Jahn-Teller distortion driven magnetic polarons in magnetite

The first known magnetic mineral, magnetite (Fe$_3$O$_4$), has unusual properties which have fascinated mankind for centuries; it undergoes the Verwey transition at $T_{\rm V}$ $\sim$120 K with an abrupt change in structure and electrical conductivity. The mechanism of the Verwey transition however remains contentious. Here we use resonant inelastic X-ray scattering (RIXS) over a wide temperature range across the Verwey transition to identify and separate out the magnetic excitations derived from nominal Fe$^{2+}$ and Fe$^{3+}$ states. Comparison of the RIXS results with crystal-field multiplet calculations shows that the spin-orbital $dd$ excitons of the Fe$^{2+}$ sites arise from a tetragonal Jahn-Teller active polaronic distortion of the Fe$^{2+}$O$_6$ octahedra. These low-energy excitations, which get weakened for temperatures above 350 K but persist at least up to 550 K, are distinct from optical excitations and best explained as magnetic polarons.

cond-mat.str-el↗

arXiv2015

Raman and fluorescence characteristics of resonant inelastic X-ray scattering from doped superconducting cuprates

Measurements of spin excitations are essential for an understanding of spin-mediated pairing for superconductivity; and resonant inelastic X-ray scattering (RIXS) provides a considerable opportunity to probe high-energy spin excitations. However, whether RIXS correctly measures the collective spin excitations of doped superconducting cuprates remains under debate. Here we demonstrate distinct Raman- and fluorescence-like RIXS excitations of Bi$_{1.5}$Pb$_{0.6}$Sr$_{1.54}$CaCu$_{2}$O$_{8+δ}$ in the mid-infrared energy region. Combining photon-energy and momentum dependent RIXS measurements with theoretical calculations using exact diagonalization provides conclusive evidence that the Raman-like RIXS excitations correspond to collective spin excitations, which are magnons in the undoped Mott insulators and evolve into paramagnons in doped superconducting compounds. In contrast, the fluorescence-like shifts are due primarily to the continuum of particle-hole excitations in the charge channel. Our results show that under the proper experimental conditions RIXS indeed can be used to probe paramagnons in doped high-$T_c$ cuprate superconductors.

cond-mat.supr-con↗

arXiv2015

Photoemission and X-ray Absorption Studies of the Diluted Magnetic Semiconductor Ba$_{1-y}$K$_{y}$(Zn$_{1-x}$Mn$_{x}$)$_{2}$As$_{2}$ Isostructural to Fe-based Superconductors

The electronic and magnetic properties of a new diluted magnetic semiconductor (DMS) Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$, which is isostructural to so-called 122-type Fe-based superconductors, are investigated by x-ray absorption spectroscopy (XAS) and resonance photoemission spectroscopy (RPES). Mn $L_{2,3}$-edge XAS indicates that the doped Mn atoms have the valence 2+ and strongly hybridize with the $4p$ orbitals of the tetrahedrally coordinating As ligands. The Mn $3d$ partial density of states (PDOS) obtained by RPES shows a peak around 4 eV and relatively high between 0-2 eV below the Fermi level ($E_{F}$) with little contribution at $E_{F}$, similar to that of the archetypal DMS Ga$_{1-x}$Mn$_{x}$As. This energy level creates $d^{5}$ electron configuration with $S=5/2$ local magnetic moments at the Mn atoms. Hole carriers induced by K substitution for Ba atoms go into the top of the As $4p$ valence band and are weakly bound to the Mn local spins. The ferromagnetic correlation between the local spins mediated by the hole carriers induces ferromagnetism in Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$

cond-mat.mtrl-sci↗

arXiv2014

Reverberation Mapping of the Seyfert 1 Galaxy NGC 7469

A large reverberation mapping study of the Seyfert 1 galaxy NGC 7469 has yielded emission-line lags for Hbeta 4861 and He II 4686 and a central black hole mass measurement of about 10 million solar masses, consistent with previous measurements. A very low level of variability during the monitoring campaign precluded meeting our original goal of recovering velocity-delay maps from the data, but with the new Hbeta measurement, NGC 7469 is no longer an outlier in the relationship between the size of the Hbeta-emitting broad-line region and the AGN luminosity. It was necessary to detrend the continuum and Hbeta and He II 4686 line light curves and those from archival UV data for different time-series analysis methods to yield consistent results.

astro-ph.GA↗

arXiv2013

Observation of magnetically hard grain boundaries in double-perovskite Sr$_{2}$FeMoO$_{6}$

Unusual low temperature magneto-resistance (MR) of ferromagnetic Sr$_{2}$FeMoO$_{6}$ polycrystals has been attributed to magnetically hard grain boundaries which act as spin valves. We detected the different magnetic hysteresis curves for the grains and the grain boundaries of polycrystalline Sr$_{2}$FeMoO$_{6}$ by utilizing the different probing depths of the different detection modes of x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD), namely, the total electron yield (TEY) mode (probing depth $\sim$5 nm) and the total fluorescence yield (TFY) mode (probing depth $\sim$100 nm). At 20 K, the magnetic coercivity detected in the TEY mode ($H_{\rm c,TEY}$) was several times larger than that in the TFY mode ($H_{\rm c,TFY}$), indicating harder ferromagnetism of the grain boundaries than that of the grains. At room temperature, the grain boundary magnetism became soft and $H_{\rm c,TEY}$ and $H_{\rm c,TFY}$ were nearly the same. From line-shape analysis of the XAS and XMCD spectra, we found that in the grain boundary region the ferromagnetic component is dominated by Fe$^{2+}$ or well-screened signals while the non-magnetic component is dominated by Fe$^{3+}$ or poorly-screened signals.

cond-mat.str-el↗

arXiv2013

Correlation effects in CaCu3Ru4O12

We have investigated the electronic structure of CaCu3Ru4O12 and LaCu3Ru4O12 using soft x-ray photoelectron and absorption spectroscopy together with band structure and cluster configuration interaction calculations. We found the Cu to be in a robust divalent ionic state while the Ru is more itinerant in character and stabilizes the metallic state. Substitution of Ca by La predominantly affects the Ru states. We observed strong correlation effects in the Cu 3d states affecting the valence band line shape considerably. Using resonant photoelectron spectroscopy at the Cu L3 edge we were able to unveil the position of the Zhang-Rice singlet states in the one-electron removal spectrum of the Cu with respect to the Ru-derived metallic bands in the vicinity of the chemical potential.

cond-mat.str-el↗