arXiv subjects

J. F. Mitchell

Publications and source records attributed to J. F. Mitchell.

At least 37 records · Page 2Linked to original sources

arXiv2024

Low temperature dynamic polaron liquid in a manganite exhibiting colossal magnetoresistance

Polarons - fermionic charge carriers bearing a strong companion lattice deformation - exhibit a natural tendency for self-localization due to the recursive interaction between electrons and the lattice. While polarons are ubiquitous in insulators, how they evolve in transitions to metallic and superconducting states in quantum materials remains an open question. Here, we use resonant inelastic x-ray scattering (RIXS) to track the electron-lattice coupling in the colossal magneto-resistive bi-layer manganite La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ across its metal-to-insulator transition. The response in the insulating high-temperature state features harmonic emissions of a dispersionless oxygen phonon at small energy transfer. Upon cooling into the metallic state, we observe a drastic redistribution of spectral weight from the region of these harmonic emissions to a broad high energy continuum. In concert with theoretical calculations, we show that this evolution implies a shift in electron-lattice coupling from static to dynamic lattice distortions that leads to a distinct polaronic ground state in the low temperature metallic phase - a dynamic polaron liquid.

cond-mat.str-el↗

arXiv2024

Resolving Length Scale Dependent Transient Disorder Through an Ultrafast Phase Transition

Material functionality can be strongly determined by structure extending only over nanoscale distances. The pair distribution function presents an opportunity to shift structural studies beyond idealized crystal models and investigate structure over varying length scales. Applying this method with ultrafast time resolution has the potential to similarly disrupt the study of structural dynamics and phase transitions. Here, we demonstrate such a measurement of CuIr$_{2}$S$_{4}$ optically pumped from its low temperature Ir-dimerized phase. Dimers are optically suppressed without spatial correlation, generating a structure whose level of disorder depends strongly on length scale. The re-development of structural ordering over tens of picoseconds is directly tracked over both space and time as a transient state is approached. This measurement demonstrates both the crucial role of local structure and disorder in non-equilibrium processes and the feasibility of accessing this information with state-of-the-art XFEL facilities.

cond-mat.mtrl-sci↗

arXiv2023

Pressure-dependent "Insulator-Metal-Insulator" Behavior in Sr-doped La$_3$Ni$_2$O$_7$

Recently, superconductivity at high temperatures has been observed in bulk La$_3$Ni$_2$O$_{7-δ}$ under high pressure. However, the attainment of high-purity La$_3$Ni$_2$O$_{7-δ}$ single crystals, exhibiting controlled and homogeneous stoichiometry through the post-annealing process in an oxygen-rich floating zone furnace, remains a formidable challenge. Here, we report the crystal structure and physical properties of single crystals of Sr-doped La$_3$Ni$_2$O$_7$ synthesized at high pressure (20 GPa) and high temperature (1400 °C). Through single crystal X-ray diffraction, we showed that high-pressure-synthesized paramagnetic Sr-doped La$_3$Ni$_2$O$_7$ crystallizes in an orthorhombic structure with Ni-O-Ni bond angles of 173.4(2)°out-of-plane and 175.0(2)°and 176.7(2)°in plane. The substitution of Sr alters in band filling and the ratio of Ni$^{2+}$/Ni$^{3+}$ in Sr-doped La$_3$Ni$_2$O$_7$, aligning them with those of "La$_3$Ni$_2$O$_{7.05}$", thereby leading to significant modifications in properties under high pressure relative to the unsubstituted parent phase. At ambient pressure, Sr-doped La$_3$Ni$_2$O$_7$ exhibits insulating properties, and the conductivity increases as pressure goes up to 10 GPa. However, upon further increasing pressure beyond 10.7 GPa, Sr-doped La$_3$Ni$_2$O$_7$ transits back from a metal-like behavior to an insulator. The insulator-metal-insulator trend under high pressure dramatically differs from the behavior of the parent compound La$_3$Ni$_2$O$_{7-δ}$, despite their similar behavior in the low-pressure regime. These experimental results underscore the considerable challenge in achieving superconductivity in nickelates.

cond-mat.supr-con↗

arXiv2023

Polymorphism in Ruddlesden-Popper $La_{3}Ni_{2}O_{7}$: Discovery of a Hidden Phase with Distinctive Layer Stacking

We report the discovery of a novel form of Ruddlesden-Popper (RP) oxide, which stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase $La_{3}Ni_{2}O_{7}$adopts a novel stacking sequence in which single and trilayer blocks of $NiO_{6}$ octahedra alternate in a 1313 sequence. Crystals of this new polymorph are described in space group Cmmm, although we note evidence for a competing Imcm variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with onset at T = 134 K, which lies intermediate between that of the standard 2222 polymorph of $La_{3}Ni_{2}O_{7}$ (space group Amam) and the trilayer RP phase, $La_{4}Ni_{3}O_{10}$. The discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity with $T_{c}$ as high as 80 K above 14 GPa in bilayer $La_{3}Ni_{2}O_{7}$.

cond-mat.supr-con↗

arXiv2023

Electronic structure in a transition metal dipnictide TaAs2

The family of transition metal dipnictides (TMDs) has been of theoretical and experimental interest because this family hosts topological states and extremely large magnetoresistance (MR). Recently, TaAs2, a member of this family, has been predicted to support a topological crystalline insulating state. Here, by using high resolution. Angle resolved photoemission spectroscopy (ARPES), we reveal both closed and open pockets in the metallic Fermi surface and linearly dispersive bands on the (201) surface, along with the presence of extreme MR observed from magneto-transport measurements. A comparison of the ARPES results with first-principles computations show that the linearly dispersive bands on the measured surface of TaAs2 are trivial bulk bands. The absence of symmetry-protected surface state on the (201) surface indicates its topologically dark nature. The presence of open Fermi surface features suggests that the open orbit fermiology could contribute to the extremely large MR of TaAs.

cond-mat.mes-hall↗

arXiv2023

Heterogeneous field response of hierarchical polar laminates in relaxor ferroelectrics

Relaxor ferroelectrics are a class of materials that are widely perceived as deriving their exotic properties from structural heterogeneities. Understanding the microscopic origin of the superior electromechanical response requires knowledge not only concerning the formation of polar nanodomains (PNDs) built from individual atoms but more importantly the spatial distribution of PNDs over longer distances. The mesoscale PND arrangement is shaped by the interactions between these domains and, in turn, dictates the electric-field driven PND response directly relevant to the macroscopic material properties. Here, we show the emergence of mesoscale lattice order that we name "polar laminates" in the canonical relaxor ferroelectric 0.68PbMg$_{1/3}$Nb$_{2/3}$O$_{3}$-0.32PbTiO$_{3}$ (PMN-0.32PT) using X-ray coherent nano-diffraction. These laminates are nematic with a size of ~350 nm and arise from the staggered arrangement of ~13 nm monoclinic PNDs along the <110> of the pseudocubic lattice. The spatial distribution of c-axis strain is directly correlated with the tilting of the PNDs and is most prominent between the laminates. Further operando nano-diffraction studies demonstrate heterogeneous electric-field-driven responses. The most active regions tend to reside inside the laminates while the spatial pinning centers are between the laminates. This observation reveals the hierarchical assembly of lattice order as a novel form of electron and lattice self-organization in heterogenous materials and establishes the role of such mesoscale spatial arrangement in connecting the nanoscale heterogeneity and macroscopic material properties. These findings provide a guiding principle for the design and optimization of future relaxors and may shed light on the existence of similar behavior in a wide range of quantum and functional materials.

cond-mat.mtrl-sci↗

arXiv2023

Resonant inelastic x-ray scattering data for Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates

Ruddlesden-Popper and reduced Ruddlesden-Popper nickelates are intriguing candidates for mimicking the properties of high-temperature superconducting cuprates. The degree of similarity between these nickelates and cuprates has been the subject of considerable debate. Resonant inelastic x-ray scattering (RIXS) has played an important role in exploring their electronic and magnetic excitations, but these efforts have been stymied by inconsistencies between different samples and the lack of publicly available data for detailed comparison. To address this issue, we present open RIXS data on La4Ni3O10 and La4Ni3O8.

cond-mat.str-el↗

arXiv2023

Electronic character of charge order in square planar low valence nickelates

Charge order is a central feature of the physics of cuprate superconductors and is known to arise from a modulation of holes with primarily oxygen character. Low-valence nickelate superconductors also host charge order, but the electronic character of this symmetry breaking is unsettled. Here, using resonant inelastic x-ray scattering at the Ni $L_2$-edge, we identify intertwined involvements of Ni $3d_{x^2-y^2}$, $3d_{3z^2-r^2}$, and O $2p_σ$ orbitals in the formation of diagonal charge order in an overdoped low-valence nickelate La$_{4}$Ni$_{3}$O$_{8}$. The Ni $3d_{x^2-y^2}$ orbitals, strongly hybridized with planar O $2p_σ$, largely shape the spatial charge distribution and lead to Ni site-centered charge order. The $3d_{3z^2-r^2}$ orbitals play a small, but non-negligible role in the charge order as they hybridize with the rare-earth $5d$ orbitals. Our results reveal that the low-energy physics and ground-state character of these nickelates are more complex than those in cuprates.

cond-mat.str-el↗

arXiv2022

Superconducting properties and gap structure of the topological superconductor candidate Ti_(3)Sb

We present a study of the superconducting properties of the candidate topological superconductor Ti_(3)Sb. Electrical transport measurements show zero resistance with a T_(c,onset) of ~ 5.9 K with a transition width ΔT_c~ 0.6 K. The superconducting phase boundaries as derived from magneto-transport and magnetic susceptibility measurements agree well. We estimate an upper critical field Bc2(0)~4.5 T. A Ginzburg-Landau (GL) analysis yields values of the coherence length and penetration depth of ζ = 6.2 nm and λ = 340 nm, respectively, and a GL parameter ~ 55, indicating extreme type-II behavior. Furthermore, we observed a step height in the specific heat (ΔC_e)/(γT_c )~1.61, a value larger than the Bardeen-Cooper-Schrieffer (BCS) value of 1.43, suggesting modest coupling. Measurements of the temperature dependence of the London penetration depth via the tunnel-diode oscillator (TDO) technique down to ~ 450 mK show a full superconducting gap, consistent with a conventional s-wave gap structure.

cond-mat.supr-con↗

arXiv2022

Magnetic Breakdown and Topology in the Kagome Superconductor CsV3Sb5 under High Magnetic Field

The recently discovered layered Kagome metals of composition AV3Sb5 (A = K, Rb, Cs) exhibit a complex interplay among superconductivity, charge density wave order, topologically non-trivial electronic band structure and geometrical frustration. Here, we probe the electronic band structure underlying these exotic correlated electronic states in CsV3Sb5 with quantum oscillation measurements in pulsed fields up to 86 T. The high-field data reveal a sequence of magnetic breakdown orbits that allows the construction of a model for the folded Fermi surface of CsV3Sb5. The dominant features are large triangular Fermi surface sheets that cover almost half of the folded Brillouin zone that have not yet been detected in angle resolved photoemission spectroscopy (ARPES). These sheets display pronounced nesting at the charge density wave (CDW) vectors, which may stabilize the CDW state. The Berry phases of the electron orbits have been deduced from Landau level fan diagrams near the quantum limit without the need for extrapolations, thereby unambiguously establishing the non-trivial topological character of several electron bands in this Kagome lattice superconductor.

cond-mat.str-el↗

arXiv2022

Bootstrapped Dimensional Crossover of a Spin Density Wave

Quantum materials display rich and myriad types of magnetic, electronic, and structural ordering, often with these ordering modes either competing with one another or 'intertwining', that is, reinforcing one another. Low dimensional quantum materials, influenced strongly by competing interactions and/or geometric frustration, are particularly susceptible to such ordering phenomena and thus offer fertile ground for understanding the consequent emergent collective quantum phenomena. Such is the case of the quasi-2D materials R4Ni3O10(R=La, Pr), in which intertwined charge-and spin-density waves (CDW and SDW) on the Ni sublattice have been identified and characterized. Not unexpectedly, these density waves are largely 2D as a result of weak coupling between planes, compounded with magnetic frustration. In the case of R=Pr, however, we show here that exchange coupling between the transition metal and rare earth sublattices upon cooling overcomes both obstacles, leading to a dimensional crossover into a fully 3D ordered and coupled SDW state on both sublattices, as an induced moment on notionally nonmagnetic Pr3+ opens exchange pathways in the third dimension. In the process, the structure of the SDW on the Ni sublattice is irreversibly altered, an effect that survives reheating of the material until the underlying CDW melts. This 'bootstrapping' mechanism linking incommensurate SDWs on the two sublattices illustrates a new member of the multitude of quantum states that low-dimensional magnets can express, driven by coupled orders and modulated by frustrated exchange pathways.

cond-mat.str-el↗

arXiv2022

Electronic structure and correlations in planar trilayer nickelate Pr4Ni3O8

The recent discovery of superconductivity in hole-doped planar nickelates R1-xSrNiO2 (R=Pr,Nd) raises the foundational question of how the electronic structure and electronic correlations of these Ni1+ compounds compare to those of the Cu2+ cuprate superconductors. Here, we present an Angle-Resolved Photoemission Spectroscopy (ARPES) study of the trilayer nickelate Pr4Ni3O8, revealing an electronic structure and Fermi surface very similar to that of the hole-doped cuprates but with a few critical differences. Specifically, the main portions of the Fermi surface are extremely similar to that of the bilayer cuprates, with an additional piece that can accommodate additional hole doping. We find that the electronic correlations are about twice as strong in the nickelates and are almost k-independent, indicating that they originate from a local effect-likely the Mott interaction, whereas the cuprate interactions are somewhat less local. Nevertheless, the nickelates still demonstrate an approximately linear in energy and linear in temperature scattering rate. Understanding the similarities and differences between these two related families of strongly-correlated novel superconductors is an important challenge.

cond-mat.supr-con↗

arXiv2022

Superconducting properties of the spin Hall candidate Ta3Sb with eightfold degeneracy

We report the synthesis and characterization of phase pure Ta3Sb, a material predicted to be topological with eightfold degenerate fermionic states [Science 353, aaf5037 (2016)] and to exhibit a large spin Hall effect [Sci. Adv. 5, eaav8575 (2019]. We observe superconductivity in Ta3Sb with Tc~ 0.67 K in both electrical resistivity \r{ho}(T) and specific heat C(T) measurements. Field dependent measurements yield the superconducting phase diagram with an upper critical field of Hc2(0) ~ 0.95 T, corresponding to a superconducting coherence length of ξ ~18.6 nm. The gap ratio deduced from specific heat anomaly, 2Δ0/kBTc is 3.46, a value close to the Bardeen-Cooper-Schrieffer (BCS) value of 3.53. From a detailed analysis of both the transport and thermodynamic data within the Ginsburg-Landau (GL) framework, a GL parameter of \k{appa} ~90 is obtained identifying Ta3Sb as an extreme type-II superconductor. The observation of superconductivity in an eightfold degenerate fermionic compound with topological surface states and predicted large spin Hall conductance positions Ta3Sb as an appealing platform to further explore exotic quantum states in multifold degenerate systems.

cond-mat.supr-con↗

arXiv2022

Magnetic terahertz resonances above the Néel temperature in the frustrated kagome antiferromagnet averievite

Time-domain magneto-THz spectroscopy is utilized to study the frustrated magnet averievite Cu$_{5-x}$Zn$_x$V$_2$O$_{10}$(CsCl). Pronounced THz resonances are observed in unsubstituted samples ($x=0$) when cooling below the onset of short-range magnetic correlations. The influence of external magnetic effects confirms the magnetic origin of these resonances. Increasing Zn substitution suppresses the resonances, as frustration effects dominate, reflecting the non-magnetic phases for $x> 0.25$ compounds. The temperature evolution of the THz spectra is complemented with electron spin resonance spectroscopy. This comparison allows a direct probe of the different contributions from magnetic order, frustration, and structural properties in the phase diagram of averievite. Our results illustrate the effect of magnetic interactions in THz spectra of frustrated magnets.

cond-mat.str-el↗

arXiv2022

Role of Oxygen States in the Low Valence Nickelate La$_4$Ni$_3$O$_8$

The discovery of superconductivity in square-planar low valence nickelates has ignited a vigorous debate regarding their essential electronic properties: Do these materials have appreciable oxygen charge-transfer character akin to the cuprates, or are they in a distinct Mott-Hubbard regime where oxygen plays a minimal role? Here, we resolve this question using O $K$-edge resonant inelastic x-ray scattering (RIXS) measurements of the low valence nickelate La$_{4}$Ni$_{3}$O$_{8}$ and a prototypical cuprate La$_{2-x}$Sr$_{x}$CuO$_{4}$ ($x=0.35$). As expected, the cuprate lies deep in the charge-transfer regime of the Zaanen-Sawatzky-Allen scheme. The nickelate, however, is not well described by either limit of the ZSA scheme and is found to be of mixed charge-transfer/Mott-Hubbard character with the Coulomb repulsion $U$ of similar size to the charge-transfer energy $Δ$. Nevertheless, the transition-metal-oxygen hopping is larger in La$_{4}$Ni$_{3}$O$_{8}$ than in La$_{2-x}$Sr$_{x}$CuO$_{4}$, leading to a significant superexchange interaction and an appreciable hole occupation of the ligand O orbitals in La$_{4}$Ni$_{3}$O$_{8}$ despite its larger $Δ$. Our results clarify the essential characteristics of low valence nickelates and put strong constraints on theoretical interpretations of superconductivity in these materials.

cond-mat.supr-con↗

arXiv2021

A Nickelate Renaissance

The 2019 discovery of high temperature superconductivity in layered nickelate films, Nd$_{1-x}$SrNiO$_2$, has galvanized a community that has been studying nickelates for more than 30 years both as cuprate analogs and in their own right. On the surface, infinite layer nickelates, and their multilayer analogs, should be promising candidates based on our understanding of cuprates: square planar coordination and a parent d9 configuration that places a single hole in a dx2-y2 planar orbital makes nickelates seem poised for superconductivity. But creating crystals and films of sufficient quality of this d9 configuration in Ni1+ has proven to be a synthetic challenge, only recently overcome. These crystalline specimens are opening windows that shed new light on the cuprate-nickelate analogy and revealing nuances that leave the relationship between cuprates and nickelates very much an area open to debate further study. This Perspective gives a qualitative, phenomenological account of these newly discovered superconductors and multilayer members of the infinite layer nickelate family. The focus is on our current understanding of electronic and magnetic properties of these materials as well as some future opportunities, explored from the viewpoint of synthetic challenges and some suggested developments in materials discovery and growth to make further progress in this rejuvenated field.

cond-mat.supr-con↗

arXiv2021

Local electronic structure of rutile RuO$_2$

Recently, rutile RuO$_2$ has raised interest for its itinerant antiferromagnetism, crystal Hall effect, and strain-induced superconductivity. Understanding and manipulating these properties demands resolving the electronic structure and the relative roles of the rutile crystal field and $4d$ spin-orbit coupling (SOC). Here, we use O-K and Ru $M_3$ x-ray absorption (XAS) and Ru $M_3$ resonant inelastic x-ray scattering (RIXS) to disentangle the contributions of crystal field, SOC, and electronic correlations in RuO$_2$. The locally orthorhombic site symmetry of the Ru ions introduces significant crystal field contributions beyond the approximate octahedral coordination yielding a crystal field energy scale of $Δ(t_{2g})\approx 1$ eV breaking the degeneracy of the $t_{2g}$ orbitals. This splitting exceeds the Ru SOC ($\approx160$ meV) suggesting a more subtle role of SOC, primarily through the modification of itinerant (rather than local) $4d$ electronic states, ultimately highlighting the importance of the local symmetry in RuO$_2$. Remarkably, our analysis can be extended to other members of the rutile family, thus advancing the comprehension of the interplay among crystal field symmetry, electron correlations, and SOC in transition metal compounds with the rutile structure.

cond-mat.str-el↗

arXiv2021

The essential role of magnetic frustration in the phase diagrams of doped cobaltites

Doped perovskite cobaltites (e.g., La$_{1-x}$Sr$_x$CoO$_3$) have been extensively studied for their spin-state physics, electronic inhomogeneity, and insulator-metal transitions. Ferromagnetically-interacting spin-state polarons emerge at low $x$ in the phase diagram of these compounds, eventually yielding long-range ferromagnetism. The onset of long-range ferromagnetism ($x \approx 0.18$) is substantially delayed relative to polaron percolation ($x \approx 0.05$), however, generating a troubling inconsistency. Here, Monte-Carlo simulations of a disordered classical spin model are used to establish that previously ignored magnetic frustration is responsible for this effect, enabling faithful reproduction of the magnetic phase diagram.

cond-mat.str-el↗