arXiv subjects

J. W. Allen

Publications and source records attributed to J. W. Allen.

At least 19 recordsLinked to original sources

arXiv2025

Layer-dependent spin-resolved electronic structure of ferromagnetic triple-layered ruthenate Sr$_4$Ru$_3$O$_{10}$

High-resolution angle- and spin-resolved photoemission spectroscopy (ARPES) of the triple-layered ruthenate Sr$_4$Ru$_3$O$_{10}$ reveals features of the electronic structure that extend our understanding of the layered strontium ruthenates. The spectra near the Fermi energy are very different from the non-magnetic analogues Sr$_2$RuO$_4$ and Sr$_3$Ru$_2$O$_7$ with distinct Fermi surfaces for wide electron-like minority spin bands around the zone center and narrow hole-like majority spin Fermi surface contours around the zone corners. The most dramatic results are two narrow spectral peaks $\sim$30 meV below the Fermi-level, a spin-minority hole-like band at the Brillouin zone center, and a spin-majority saddle-band van Hove singularity at the zone edge, which exhibits almost 100\% spin-polarization at low temperature, and a strong temperature dependent coherence-incoherence crossover attributed to Hund metal correlations. Quantitative comparison of the ARPES to spin-polarized density functional theory (DFT) calculations identify the specific antibonding and nonbonding orbital origins of the narrow bands, with a prediction of different spatial localization in the central and outer layers. This is shown to be consistent with experimental ARPES multi-zone matrix element intensity variations, and implicates outer-layer-specific control of the in-plane metamagnetism. The renormalization of the bands relative to the mean-field DFT, the demonstration of spin-polarized oxygen bands, and of spin-minority and spin-majority band-crossing hybridization, provide a more complete picture of the magnetism which displays aspects of both delocalized and local moment behavior.

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arXiv2023

Wannier-Orbital theory and ARPES for the quasi-1D conductor LiMo$_{6}$O$_{17}$

In this set of three papers, we present the results of a combined study by density-functional (LDA) band theory (NMTO) and angle-resolved photoemission spectroscopy (ARPES) of lithium purple bronze, 2(Li$_{1x}$Mo$_{6}$O$_{17}$). This material is particularly notable for its unusually robust quasi-one-dimensional (quasi-1D) behavior. The band structure, in a large energy window around the Fermi energy, is basically 2D and formed by three Mo $t_{2g}$-like extended Wannier orbitals (WOs) per cell, each one giving rise to a 1D band running at a 120$^{\circ }$ angle to the two others. A structural "dimerization" from $\mathbf{c}/2$ to $\mathbf{c}$ gaps the $xz$ and $yz$ bands while leaving the $xy$ bands metallic in the gap but resonantly coupled to the gap edges and, hence, to the two other directions. The resulting complex shape of the quasi-1D Fermi surface (FS), verified by our ARPES, thus depends strongly on the Fermi energy position in the gap, implying a great sensitivity to Li stoichiometry of properties dependent on the FS, such as FS nesting or superconductivity. The band structure, expressed as a six-band, analytical tight-binding (TB) Hamiltonian, is verified in detail by the recognition and application of an ARPES selection rule that enables, for the first time, the separation in ARPES spectra of the two barely split $xy$ bands and the observation of their complex split FS. The strong resonances prevent either a two-band TB model or a related real-space ladder picture from giving a valid description of the low-energy electronic structure. Down to a temperature of 6$\,$K we find no evidence for a theoretically expected downward renormalization of perpendicular single particle hopping due to LL fluctuations in the quasi-1D chains.

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arXiv2022

Global perspectives of the bulk electronic structure of URu$_2$Si$_2$ from angle-resolved photoemission

Previous high-resolution angle-resolved photoemission (ARPES) studies of URu$_2$Si$_2$ have characterized the temperature-dependent behavior of narrow-band states close to the Fermi level ($E_\mathrm{F}$) at low photon energies near the zone center, with an emphasis on electronic reconstruction due to Brillouin zone folding. A substantial challenge to a proper description is that these states interact with other hole-band states that are generally absent from bulk-sensitive soft x-ray ARPES measurements. Here we provide a more global $k$-space context for the presence of such states and their relation to the bulk Fermi surface topology using synchrotron-based wide-angle and photon energy-dependent ARPES mapping of the electronic structure using photon energies intermediate between the low-energy regime and the high-energy soft x-ray regime. Small-spot spatial dependence, $f$-resonant photoemission, Si 2$p$ core-levels, x-ray polarization, surface-dosing modification, and theoretical surface slab calculations are employed to assist identification of bulk versus surface state character of the $E_\mathrm{F}$-crossing bands and their relation to specific U- or Si-terminations of the cleaved surface. The bulk Fermi surface topology is critically compared to density functional theory and to dynamical mean field theory calculations. In addition to clarifying some aspects of the previously measured high symmetry $Γ$, Z and X points, incommensurate 0.6a* nested Fermi-edge states located along Z-N-Z are found to be distinctly different from the density functional theory Fermi surface prediction. The temperature evolution of these states above $T_{HO}$, combined with a more detailed theoretical investigation of this region, suggests a key role of the N-point in the hidden order transition.

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arXiv2021

Pressure-induced structural transitions triggering dimensional crossover in lithium purple bronze Li0.9M6O17

At ambient pressure, lithium molybdenum purple bronze (Li0.9Mo6O17) is a quasi-one dimensional solid in which the anisotropic crystal structure and the linear dispersion of the underlying bands produced by electronic correlations possibly bring about a rare experimental realization of Tomomaga-Luttinger liquid physics. It is also the sole member of the broader purple molybdenum bronzes family where a Peierls instability has not been identified at low temperatures. The present study reports a pressure-induced series of phase transitions between 0 and 12 GPa. These transitions are strongly reflected in infrared spectroscopy, Raman spectroscopy, and x-ray diffraction. The most dramatic effect seen in optical conductivity is the metallization of the c-axis, concomitant to the decrease of conductivity along the b-axis. This indicates that high pressure drives the material away from its quasi-one dimensional behavior at ambient pressure. While the first pressure-induced structure of the series is resolved, the identification of the underlying mechanisms driving the dimensional change in the physics remains a challenge.

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arXiv2017

Insight into the temperature dependent properties of the ferromagnetic Kondo lattice YbNiSn

Analyzing temperature dependent photoemission (PE) data of the ferromagnetic Kondo-lattice (KL) system YbNiSn in the light of the Periodic Anderson model (PAM) we show that the KL behavior is not limited to temperatures below a temperature T_K, defined empirically from resistivity and specificic heat measurements. As characteristic for weakly hybridized Ce and Yb systems, the PE spectra reveal a 4f-derived Fermi level peak, which reflects contributions from the Kondo resonance and its crystal electric field (CEF) satellites. In YbNiSn this peak has an unusual temperature dependence: With decreasing temperature a steady linear increase of intensity is observed which extends over a large interval ranging from 100 K down to 1 K without showing any peculiarities in the region of T_K ~ TC= 5.6 K. In the light of the single-impurity Anderson model (SIAM) this intensity variation reflects a linear increase of 4f occupancy with decreasing temperature, indicating an onset of Kondo screening at temperatures above 100 K. Within the PAM this phenomenon could be described by a non-Fermi liquid like T- linear damping of the self-energy which accounts phenomenologically for the feedback from the closely spaced CEF-states.

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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.

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arXiv2016

Fermi Surface of Metallic V$_2$O$_3$ from Angle-Resolved Photoemission: Mid-level Filling of $e_g^π$ Bands

Using angle resolved photoemission spectroscopy (ARPES) we report the first band dispersions and distinct features of the bulk Fermi surface (FS) in the paramagnetic metallic phase of the prototypical metal-insulator transition material V$_2$O$_3$. Along the $c$-axis we observe both an electron pocket and a triangular hole-like FS topology, showing that both V 3$d$ $a_{1g}$ and $e_g^π$ states contribute to the FS. These results challenge the existing correlation-enhanced crystal field splitting theoretical explanation for the transition mechanism and pave the way for the solution of this mystery.

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arXiv2016

Gapped electron fractionalization in robustly one dimensional Li0.9Mo6O17

The angle resolved photoemission spectroscopy lineshapes of quasi one-dimensional (1d) Li0.9Mo6O17 display both agreement with and departures from the one-band Tomonaga-Luttinger model. We show that the departures can be understood by explicitly accounting for the four modes arising from the two quasi-1d bands known to cross the Fermi energy. The key assumption is that the antisymmetric charge mode is gapped with a magnitude near the temperature (T) of a mysterious 25K powerlaw resistivity upturn. The gap is consistent with the lack of a charge or spin density wave accompanying the upturn, is able to control the upturn T, and prevents crossover to a Fermi liquid (FL) down to the superconducting transition at 1.9K.

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arXiv2016

Electronic structure of YbB$_{6}$: Is it a Topological Insulator or not?

To resolve the controversial issue of the topological nature of the electronic structure of YbB$_{6}$, we have made a combined study using density functional theory (DFT) and angle resolved photoemission spectroscopy (ARPES). Accurate determination of the low energy band topology in DFT requires the use of modified Becke-Johnson exchange potential incorporating the spin-orbit coupling and the on-site Coulomb interaction $U$ of Yb $4f$ electrons as large as 7 eV. We have double-checked the DFT result with the more precise GW band calculation. ARPES is done with the non-polar (110) surface termination to avoid band bending and quantum well confinement that have confused ARPES spectra taken on the polar (001) surface termination. Thereby we show definitively that YbB$_{6}$ has a topologically trivial B 2$p$-Yb 5$d$ semiconductor band gap, and hence is a non-Kondo non-topological insulator (TI). In agreement with theory, ARPES shows pure divalency for Yb and a $p$-$d$ band gap of 0.3 eV, which clearly rules out both of the previous scenarios of $f$-$d$ band inversion Kondo TI and $p$-$d$ band inversion non-Kondo TI. We have also examined the pressure-dependent electronic structure of YbB$_{6}$, and found that the high pressure phase is not a Kondo TI but a \emph{p}-\emph{d} overlap semimetal.

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arXiv2016

Consistency of Photoemission and Quantum Oscillations for Surface States of SmB6

The mixed valent compound SmB6 is of high current interest as the first candidate example of topologically protected surface states in a strongly correlated insulator and also as a possible host for an exotic bulk many-body state that would manifest properties of both an insulator and a metal. Two different de Haas van Alphen (dHvA) experiments have each supported one of these possibilities, while angle resolved photoemission spectroscopy (ARPES) for the (001) surface has supported the first, but without quantitative agreement to the dHvA results. We present new ARPES data for the (110) surface and a new analysis of all published dHvA data and thereby bring ARPES and dHvA into substantial consistency around the basic narrative of two dimensional surface states.

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arXiv2015

Magnetotransport Measurements of the Surface States of Samarium Hexaboride using Corbino Structures

The recent conjecture of a topologically-protected surface state in SmB$_6$ and the verification of robust surface conduction below 4 K have prompted a large effort to understand the surface states. Conventional Hall transport measurements allow current to flow on all surfaces of a topological insulator, so such measurements are influenced by contributions from multiple surfaces of varying transport character. Instead, we study magnetotransport of SmB$_6$ using a Corbino geometry, which can directly measure the conductivity of a single, independent surface. Both (011) and (001) crystal surfaces show a strong negative magnetoresistance at all magnetic field angles measured. The (011) surface has a carrier mobility of $122\text{ cm}^2/\text{V}\cdot\text{sec}$ with a carrier density of $2.5\times10^{13} \text{ cm}^{-2}$, which are significantly smaller than indicated by Hall transport studies. This mobility value can explain a failure so far to observe Shubnikov-de Haas oscillations. Analysis of the angle-dependence of conductivity on the (011) surface suggests a combination of a field-dependent enhancement of the carrier density and a suppression of Kondo scattering from native oxide layer magnetic moments as the likely origin of the negative magnetoresistance. Our results also reveal a hysteretic behavior whose magnitude depends on the magnetic field sweep rate and temperature. Although this feature becomes smaller when the field sweep is slower, does not disappear or saturate during our slowest sweep-rate measurements, which is much slower than a typical magnetotransport trace. These observations cannot be explained by quantum interference corrections such as weak anti-localization, but are more likely due to an extrinsic magnetic effect such as the magnetocaloric effect or glassy ordering.

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arXiv2015

Soft X-ray Angle Resolved Photoemission with Micro Positioning Techniques for Metallic V$_2$O$_3$

We have performed soft-X-ray angle resolved photoemission for metallic V$_2$O$_3$. Combining a micro focus beam (40 x 65 $μ$m$^2$) and micro positioning techniques with a long working distance microscope, we have succeeded in observing band dispersions from tiny cleavage surfaces with typical size of the several tens of $μ$m. The photoemission spectra show a clear position dependence reflecting the morphology of the cleaved sample surface. By selecting high quality flat regions on the sample surface, we have succeeded in band mapping using both photon-energy and polar-angle dependences, opening the door to three-dimensional ARPES for typical three dimensional correlated materials where large cleavage planes are rarely obtained.

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arXiv2014

Fermi Arcs in a Doped Pseudospin-1/2 Heisenberg Antiferromagnet

High temperature superconductivity in cuprates arises from an electronic state that remains poorly understood. We report the observation of a related electronic state in a non-cuprate material Sr2IrO4 in which the unique cuprate Fermiology is largely reproduced. Upon surface electron doping through in situ deposition of alkali-metal atoms, angle-resolved photoemission spectra of Sr2IrO4 display disconnected segments of zero-energy states, known as Fermi arcs, and a gap as large as 80 meV. Its evolution toward a normal metal phase with a closed Fermi surface as a function of doping and temperature parallels that in the cuprates. Our result suggests that Sr2IrO4 is a useful model system for comparison to the cuprates.

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arXiv2014

Persistent non-metallic behavior in Sr2IrO4 and Sr3Ir2O7 at high pressures

Iridium-based 5d transition-metal oxides are attractive candidates for the study of correlated electronic states due to the interplay of enhanced crystal-field, Coulomb and spin-orbit interaction energies. At ambient pressure, these conditions promote a novel Jeff = 1/2 Mott insulating state, characterized by a gap of the order of ~0.1 eV. We present high-pressure electrical resistivity measurements of single crystals of Sr2IrO4 and Sr3Ir2O7. While no indications of a pressure-induced metallic state up to 55 GPa were found in Sr2IrO4, a strong decrease of the gap energy and of the resistance of Sr3Ir2O7 between ambient pressure and 104 GPa confirm that this compound is in the proximity of a metal-insulator transition.

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arXiv2014

Temperature Dependence of Linked Gap and Surface State Evolution in the Mixed Valent Topological Insulator SmB6

Taken together and viewed holistically, recent theory, low temperature (T) transport, photoelectron spectroscopy and quantum oscillation experiments have built a very strong case that the paradigmatic mixed valence insulator SmB6 is currently unique as a three-dimensional strongly correlated topological insulator (TI). As such, its many-body T-dependent bulk gap brings an extra richness to the physics beyond that of the weakly correlated TI materials. How will the robust, symmetry-protected TI surface states evolve as the gap closes with increasing T? For SmB6 exploiting this opportunity first requires resolution of other important gap-related issues, its origin, its magnitude, its T-dependence and its role in bulk transport. In this paper we report detailed T-dependent angle resolved photoemission spectroscopy (ARPES) measurements that answer all these questions in a unified way.

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arXiv2013

Low-temperature surface conduction in the Kondo insulator SmB$_6$

We study the transport properties of the Kondo insulator SmB$_6$ with a specialized configuration designed to distinguish bulk-dominated conduction from surface-dominated conduction. We find that as the material is cooled below 4 K, it exhibits a crossover from bulk to surface conduction with a fully insulating bulk. We take the robustness and magnitude of the surface conductivity, as is manifest in the literature of SmB$_6$, to be strong evidence for the topological insulator metallic surface states recently predicted for this material.

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arXiv2013

Yb Valence Change in (Ce,Yb)CoIn5 from spectroscopy and bulk properties

The electronic structure of (Ce,Yb)CoIn5 has been studied by a combination of photoemission, x-ray absorption and bulk property measurements. Previous findings of a Ce valence near 3+ for all x and of an Yb valence near 2.3+ for x>0.3 were confirmed. One new result of this study is that the Yb valence for x<0.2 increases rapidly with decreasing x from 2.3+ toward 3+, which correlates well with de Haas van Alphen results showing a change of Fermi surface around x=0.2. Another new result is the direct observation by angle resolved photoemission Fermi surface maps of about 50% cross sectional area reductions of the α- and β-sheets for x=1 compared to x=0, and a smaller, essentially proportionate, size change of the α-sheet for x=0.2. These changes are found to be in good general agreement with expectations from simple electron counting. The implications of these results for the unusual robustness of superconductivity and Kondo coherence with increasing x in this alloy system are discussed.

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arXiv2013

Topological crystalline Kondo insulators and universal topological surface states of SmB$_6$

We prove theoretically that certain strongly correlated Kondo insulators are topological crystalline insulators with nontrivial topology protected by crystal symmetries. In particular, we find that SmB$_6$ is such a material. In addition to a nontrivial Z$_2$ topological index protected by time reversal symmetry, SmB$_6$ also has nontrival mirror Chern numbers protected by mirror symmetries. On the $(100)$ surface of SmB$_6$, the nontrivial mirror Chern numbers do not generate additional surface states beyond those predicted by the Z$_2$ topological index. However, on the $(110)$ surface, two more surface Dirac points are predicted. Remarkably, we find that for SmB$_6$ both the Z$_2$ topological index and the mirror Chern numbers are independent of microscopic details, which enables us to obtain surface state properties that are universal.

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