arXiv subjects

Jacob P. C. Ruff

Publications and source records attributed to Jacob P. C. Ruff.

At least 37 records · Page 2Linked to original sources

arXiv2022

Magnetic excitations in double perovskite iridates La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn) mediated by 3$\mathit{d}$-5$\mathit{d}$ hybridization

By performing resonant inelastic x-ray scattering (RIXS) measurements at the Ir $\mathit{L_{\mathrm{3}}}$ edge, we have investigated the low-energy elementary excitations in a series of double perovskite iridate single crystals, La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn). Almost dispersionless magnetic excitations at $\sim$ 42(6) meV and $\sim$ 35(5) meV have been observed in crystals containing magnetic 3$\mathit{d}$ ions, La$_{2}$CoIrO$_{6}$ and La$_{2}$NiIrO$_{6}$, respectively. In contrast, this low-energy magnetic excitation is absent in La$_{2}$ZnIrO$_{6}$ in which the 3$\mathit{d}$ ions are non-magnetic, suggesting the importance of 3$\mathit{d}$-5$\mathit{d}$ hybridization in the magnetic properties of these double perovskite iridates. The magnetic excitation is suppressed completely above the magnetic ordering temperature, suggesting the inadequacy of using a simple spin Hamiltonian to describe magnetism of these materials.

cond-mat.str-el↗

arXiv2021

Fermi surface mapping and the nature of charge density wave order in the kagome superconductor CsV$_3$Sb$_5$

The recently discovered family of AV$_3$Sb$_5$ (A: K, Rb Cs) kagome metals possess a unique combination of nontrivial band topology, superconducting ground states, and signatures of electron correlations manifest via competing charge density wave order. Little is understood regarding the nature of the charge density wave (CDW) instability inherent to these compounds and the potential correlation with the accompanying onset of a large anomalous Hall response. To understand the impact of the CDW order on the electronic structure in these systems, we present quantum oscillation measurements on single crystals of CsV$_3$Sb$_5$. Our data provides direct evidence that the CDW invokes a substantial reconstruction of the Fermi surface pockets associated with the vanadium orbitals and the kagome lattice framework. In conjunction with density functional theory modeling, we are able to identify split oscillation frequencies originating from reconstructed pockets built from vanadium orbitals and Dirac-like bands. Complementary diffraction measurements are further able to demonstrate that the CDW instability has a correlated phasing between neighboring V$_3$Sb$_5$ planes. These results provide critical insights into the underlying CDW instability in AV$_3$Sb$_5$ kagome metals and support minimal models of CDW order arising from within the vanadium-based kagome lattice.

cond-mat.str-el↗

arXiv2021

Disorder Dynamics in Battery Nanoparticles During Phase Transitions Revealed by Operando Single-Particle Diffraction

Structural and ion-ordering phase transitions limit the viability of sodium-ion intercalation materials in grid scale battery storage by reducing their lifetime. However, the combination of phenomena in nanoparticulate electrodes creates complex behavior that is difficult to investigate, especially on the single nanoparticle scale under operating conditions. In this work, operando single-particle x-ray diffraction (oSP-XRD) is used to observe single-particle rotation, interlayer spacing, and layer misorientation in a functional sodium-ion battery. oSP-XRD is applied to Na$_{2/3}$[Ni$_{1/3}$Mn$_{2/3}$]O$_{2}$, an archetypal P2-type sodium-ion positive electrode material with the notorious P2-O2 phase transition induced by sodium (de)intercalation. It is found that during sodium extraction, the misorientation of crystalline layers inside individual particles increases before the layers suddenly align just prior to the P2-O2 transition. The increase in the long-range order coincides with an additional voltage plateau signifying a phase transition prior to the P2-O2 transition. To explain the layer alignment, a model for the phase evolution is proposed that includes a transition from localized to correlated Jahn-Teller distortions. The model is anticipated to guide further characterization and engineering of sodium-ion intercalation materials with P2-O2 type transitions. oSP-XRD therefore opens a powerful avenue for revealing complex phase behavior in heterogeneous nanoparticulate systems.

cond-mat.mtrl-sci↗

arXiv2021

Structure-selective operando x-ray spectroscopy

The relationship between charge and structure dictates the properties of electrochemical systems. For example, reversible Na-ion intercalation - a low-cost alternative to Li-ion technology - often induces detrimental structural phase transformations coupled with charge compensation reactions. However, little is known about the underpinning charge-structure mechanisms because the reduction-oxidation (redox) reactions within coexisting structural phases have so far eluded direct operando investigation. Here, we distinguish x-ray spectra of individual crystalline phases operando during a redox-induced phase transformation in P2-Na2/3Ni1/3Mn2/3O2 - an archetypal layered oxide for sodium-ion batteries. We measure the resonant elastic scattering on the Bragg reflection corresponding to the P2-phase lattice spacing. These resonant spectra become static midway through the sodium extraction in an operando coin cell, while the overall sodium extraction proceeds as evidenced by the X-ray absorption averaging over all electrochemically active Ni atoms. The stop of redox activity in the P2-structure signifies its inability to host Ni4+ ions. The coincident emergence of the O2- structure reveals the rigid link between the local redox and the long-range order during the phase transformation. The structure-selective x-ray spectroscopy thus opens a powerful avenue for resolving the dynamic chemistry of different structural phases in multi-phase electrochemical systems.

cond-mat.mtrl-sci↗

arXiv2021

Unconventional hysteretic transition in a charge density wave

Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe4. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observed that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge-density-wave (CDW) phase of EuTe4 with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly-coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.

cond-mat.mtrl-sci↗

arXiv2021

Structural and Magnetic Transitions in the Planar Antiferromagnet Ba$_4$Ir$_3$O$_{10}$

We report the structural and magnetic ground state properties of the monoclinic compound barium iridium oxide Ba$_4$Ir$_3$O$_{10}$ using a combination of resonant x-ray scattering, magnetometry, and thermodynamic techniques. Magnetic susceptibility exhibits a pronounced antiferromagnetic transition at $T_{\text{N}}$ $\approx$ 25K, a weaker anomaly at $T_{\text{S}}$ $\approx$ 142K, and strong magnetic anisotropy at all temperatures. Resonant elastic x-ray scattering experiments reveal a second order structural phase transition at $T_{\text{S}}$ and a magnetic transition at $T_{\text{N}}$. Both structural and magnetic superlattice peaks are observed at $L$ = half integer values. The magnetization anomaly at $T_{\text{S}}$ implies the presence of magneto-elastic coupling, which conceivably facilitates the symmetry lowering. Mean field critical scattering is observed above $T_{\text{S}}$. The magnetic structure of the antiferromagnetic ground state is discussed based on the measured magnetic superlattice peak intensity. Our study not only presents essential information for understanding the intertwined structural and magnetic properties in Ba$_4$Ir$_3$O$_{10}$, but also highlights the necessary ingredients for exploring novel ground states with octahedra trimers.

cond-mat.str-el↗

arXiv2020

Charge density wave with anomalous temperature dependence in UPt2Si2

Using single crystal neutron and x-ray diffraction, we discovered a charge density wave (CDW) below 320 K, which accounts for the long-sought origin of the heat capacity and resistivity anomalies in UPt2Si2. The modulation wavevector, Qmod, is intriguingly similar to the Fermi surface nesting wavevector of URu2Si2. Qmod shows an unusual temperature dependence, shifting from commensurate to incommensurate position upon cooling and becoming locked at ~ (0.42 0 0) near 180 K. Bulk measurements indicate a cross-over toward a correlated coherent state around the same temperature, suggesting an interplay between the CDW and Kondo-lattice-like coherence before coexisting antiferromagnetic order sets in at TN = 35 K.

cond-mat.supr-con↗

arXiv2019

Optical detection and manipulation of spontaneous gyrotropic electronic order in a transition-metal dichalcogenide semimetal

The observation of chirality is ubiquitous in nature. Contrary to intuition, the population of opposite chiralities is surprisingly asymmetric at fundamental levels. Examples range from parity violation in the subatomic weak force to the homochirality in essential biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks any mirror plane, space inversion center or roto-inversion axis. Typically, the geometrical chirality is predefined by a material's chiral lattice structure, which is fixed upon the formation of the crystal. By contrast, a particularly unconventional scenario is the gyrotropic order, where chirality spontaneously emerges across a phase transition as the electron system breaks the relevant symmetries of an originally achiral lattice. Such a gyrotropic order, proposed as the quantum analogue of the cholesteric liquid crystals, has attracted significant interest. However, to date, a clear observation and manipulation of the gyrotropic order remain challenging. We report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal $1T$-TiSe$_2$. We show that shining mid-infrared circularly polarized light near the critical temperature leads to the preferential formation of one chiral domain. As a result, we are able to observe an out-of-plane circular photogalvanic current, whose direction depends on the optical induction. Our study provides compelling evidence for the spontaneous emergence of chirality in the correlated semimetal TiSe$_2$. Such chiral induction provides a new way of optical control over novel orders in quantum materials.

cond-mat.mes-hall↗

arXiv2019

Evolution of structure and magnetism across the metal-insulator transition in the pyrochlore iridate $($Nd$_{1-x}$Ca$_x)_2$Ir$_2$O$_7$

We report on the evolution of the thermal metal-insulator transition in polycrystalline samples of Nd$_2$Ir$_2$O$_7$ upon hole-doping via substitution of Ca$^{2+}$ for Nd$^{3+}$. Ca substitution mediates a filling-controlled Mott-like transition with minimal resolvable structural changes and without altering site symmetry. Local structure confirms that Ca substitution does not result in local chemical phase separation, and absorption spectroscopy establishes that Ir cations maintain a spin-orbit entangled electronic configuration. The metal-insulator transition coincides with antiferromagnetic ordering on the Ir sublattice for all measured samples, and both decrease in onset temperature with Ca content. Weak low-temperature upturns in susceptibility and resistivity for samples with high Ca content suggest that Nd sublattice antiferromagnetism continues to couple to carriers in the metallic regime.

cond-mat.mtrl-sci↗

arXiv2019

Disorder raises the critical temperature of a cuprate superconductor

With the discovery of charge density waves (CDW) in most members of the cuprate high temperature superconductors, the interplay between superconductivity and CDW has become a key point in the debate on the origin of high temperature superconductivity. Some experiments in cuprates point toward a CDW state competing with superconductivity, but others raise the possibility of a CDW-superconductivity intertwined order, or more elusive pair-density wave (PDW). Here we have used proton irradiation to induce disorder in crystals of La$_{1.875}$Ba$_{0.125}$CuO$_4$ and observed a striking 50% increase of $T_\mathrm{c}$ accompanied by a suppression of the CDW. This is in clear contradiction with the behaviour expected of a d-wave superconductor for which both magnetic and non-magnetic defects should suppress $T_\mathrm{c}$. Our results thus make an unambiguous case for the strong detrimental effect of the CDW on bulk superconductivity in La$_{1.875}$Ba$_{0.125}$CuO$_4$. Using tunnel diode oscillator (TDO) measurements, we find evidence for dynamic layer decoupling in PDW phase. Our results establish irradiation-induced disorder as a particularly relevant tuning parameter for the many families of superconductors with coexisting density waves, which we demonstrate on superconductors such as the dichalcogenides and Lu$_5$Ir$_4$Si$_{10}$.

cond-mat.supr-con↗

arXiv2019

Reciprocal Space Imaging of Ionic Correlations in Intercalation Compounds

The intercalation of alkali ions into layered materials has played an essential role in battery technology since the development of the first lithium-ion electrodes. Coulomb repulsion between the intercalants leads to ordering of the intercalant sublattice, which hinders ionic diffusion and impacts battery performance. While conventional diffraction can identify the long-range order that can occur at discrete intercalant concentrations during the charging cycle, it cannot determine short-range order at other concentrations that also disrupt ionic mobility. In this article, we show that the use of real-space transforms of single crystal diffuse scattering, measured with high-energy synchrotron x-rays, allows a model-independent measurement of the temperature dependence of the length scale of ionic correlations along each of the crystallographic axes in a sodium-intercalated V$_2$O$_5$. The techniques described here provide a new way of probing the evolution of structural ordering in crystalline materials.

cond-mat.mtrl-sci↗

arXiv2018

Sr$_3$Ir$_2$O$_7$F$_2$: Topochemical conversion of a relativistic Mott state into a spin-orbit driven band insulator

The topochemical transformation of single crystals of Sr$_3$Ir$_2$O$_7$ into Sr$_3$Ir$_2$O$_7$F$_2$ is reported via fluorine insertion. Characterization of the newly formed Sr$_3$Ir$_2$O$_7$F$_2$ phase shows a nearly complete oxidation of Ir$^{4+}$ cations into Ir$^{5+}$ that in turn drives the system from an antiferromagnetic Mott insulator with a half-filled J$_{eff}=1/2$ band into a nonmagnetic $J=0$ band insulator. First principles calculations reveal a remarkably flat insertion energy that locally drives the fluorination process to completion. Band structure calculations support the formation of a band insulator whose charge gap relies on the strong spin-orbit coupling inherent to the Ir metal ions of this compound.

cond-mat.str-el↗

arXiv2018

The dual nature of magnetism in a uranium heavy fermion system

The duality between localized and itinerant nature of magnetism in $5\textit{f}$ electron systems has been a longstanding puzzle. Here, we report inelastic neutron scattering measurements, which reveal both local and itinerant aspects of magnetism in a single crystalline system of UPt$_{2}$Si$_{2}$. In the antiferromagnetic state, we observe broad continuum of diffuse magnetic scattering with a resonance-like gap of $\approx$ 7 meV, and surprising absence of coherent spin-waves, suggestive of itinerant magnetism. While the gap closes above the Neel temperature, strong dynamic spin correlations persist to high temperature. Nevertheless, the size and temperature dependence of the total magnetic spectral weight can be well described by local moment with $J=4$. Furthermore, polarized neutron measurements reveal that the magnetic fluctuations are mostly transverse, with little or none of the longitudinal component expected for itinerant moments. These results suggest that a dual description of local and itinerant magnetism is required to understand UPt$_{2}$Si$_{2}$, and by extension, other 5$f$ systems in general.

cond-mat.supr-con↗

arXiv2018

Unidirectional spin density wave state in metallic (Sr1-xLax)2IrO4

Materials that exhibit both strong spin orbit coupling and electron correlation effects are predicted to host numerous new electronic states. One prominent example is the Jeff =1/2 Mott state in Sr2IrO4, where introducing carriers is predicted to manifest high temperature superconductivity analogous to the S=1/2 Mott state of La2CuO4. While bulk superconductivity currently remains elusive, anomalous quasi-particle behaviors paralleling those in the cuprates such as pseudogap formation and the formation of a d-wave gap are observed upon electron-doping Sr2IrO4. Here we establish a magnetic parallel between electron-doped Sr2IrO4 and hole-doped La2CuO4 by unveiling a spin density wave state in electron-doped Sr2IrO4. Our magnetic resonant x-ray scattering data reveal the presence of an incommensurate magnetic state reminiscent of the diagonal spin density wave state observed in the monolayer cuprate (La1-xSrx)2CuO4. This link supports the conjecture that the quenched Mott phases in electron-doped Sr2IrO4 and hole-doped La2CuO4 support common competing electronic phases.

cond-mat.mtrl-sci↗

arXiv2017

Observation of a Charge Density Wave Incommensuration Near the Superconducting Dome in CuxTiSe2

X-ray diffraction was employed to study the evolution of the charge density wave (CDW) in CuxTiSe2 as a function of copper intercalation in order to clarify the relationship between the CDW and superconductivity. The results show a CDW incommensuration arising at an intercalation value coincident with the onset of superconductivity at around x=0.055(5). Additionally, it was found that the charge density wave persists to higher intercalant concentrations than previously assumed, demonstrating that the CDW does not terminate inside the superconducting dome. A charge density wave peak was observed in samples up to x=0.091(6), the highest copper concentration examined in this study. The phase diagram established in this work suggests that charge density wave incommensuration may play a role in the formation of the superconducting state.

cond-mat.supr-con↗

arXiv2016

Characterization of CdTe Sensors with Schottky Contacts Coupled to Charge-Integrating Pixel Array Detectors for X-Ray Science

Pixel Array Detectors (PADs) consist of an x-ray sensor layer bonded pixel-by-pixel to an underlying readout chip. This approach allows both the sensor and the custom pixel electronics to be tailored independently to best match the x-ray imaging requirements. Here we present characterizations of CdTe sensors hybridized with two different charge-integrating readout chips, the Keck PAD and the Mixed-Mode PAD (MM-PAD), both developed previously in our laboratory. The charge-integrating architecture of each of these PADs extends the instantaneous counting rate by many orders of magnitude beyond that obtainable with photon counting architectures. The Keck PAD chip consists of rapid, 8-frame, in-pixel storage elements with framing periods $<$150 ns. The second detector, the MM-PAD, has an extended dynamic range by utilizing an in-pixel overflow counter coupled with charge removal circuitry activated at each overflow. This allows the recording of signals from the single-photon level to tens of millions of x-rays/pixel/frame while framing at 1 kHz. Both detector chips consist of a 128$\times$128 pixel array with (150 $μ$m)$^2$ pixels.

physics.ins-det↗

arXiv2012

Definitive Evidence for Order-by-Quantum-Disorder in Er2Ti2O7

Here we establish the systematic existence of a U(1) degeneracy of all symmetry-allowed Hamiltonians quadratic in the spins on the pyrochlore lattice, at the mean-field level. By extracting the Hamiltonian of Er2Ti2O7 from inelastic neutron scattering measurements, we then show that the U(1)-degenerate states of Er2Ti2O7 are its classical ground states, and unambiguously show that quantum fluctuations break the degeneracy in a way which is confirmed by experiment. This is the first definitive observation of order-by-disorder in any material. We provide further verifiable consequences of this phenomenon, and several additional comparisons between theory and experiment.

cond-mat.str-el↗

arXiv2012

A single-solenoid pulsed-magnet system for single-crystal scattering studies

We present a pulsed-magnet system that enables x-ray single-crystal diffraction in addition to powder and spectroscopic studies with the magnetic field applied on or close to the scattering plane. The apparatus consists of a single large-bore solenoid, cooled by liquid nitrogen. A second independent closed-cycle cryostat is used for cooling samples near liquid helium temperatures. Pulsed magnetic fields close to $\sim 30$ T with a zero-to-peak-field rise time of $\sim$2.9 ms are generated by discharging a 40 kJ capacitor bank into the magnet coil. The unique characteristic of this instrument is the preservation of maximum scattering angle ($\sim 23.6^\circ$) on the entrance and exit sides of the magnet bore by virtue of a novel double-funnel insert. This instrument will facilitate x-ray diffraction and spectroscopic studies that are impractical, if not impossible, to perform using split-pair and narrow-opening solenoid magnets, and offers a practical solution for preserving optical access in future higher-field pulsed magnets.

physics.ins-det↗