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Robert J. Cava

Publications and source records attributed to Robert J. Cava.

At least 91 records · Page 5Linked to original sources

Peaks in the electronic density of states are not strong predictors of Superconductivity

Electronic bands near the Fermi energy with minimal energy dispersion in k-space, i.e. "flat bands", are often said to be an important characteristic of superconducting materials. When extending over a significant region of the k-space, this leads to peaks in the electronic density of states. If one could systematically search the calculated electronic structures of materials, already available through the Materials Genome Initiative, for such peaks, then the rate of new superconductor discovery could be accelerated greatly. Here we test whether this characteristic actually distinguishes known superconductors from known non-superconductors. We find that there is an anticorrelation for tetragonal symmetry materials, but that hexagonal symmetry superconductors exhibit such peaks more frequently than hexagonal non-superconductors. More generally, our study's limitations underscore the importance of standardizing digital resources for achieving the accelerated materials discovery paradigm promised by the Materials Genome Initiative.

cond-mat.supr-con↗

The range of non-Kitaev terms and fractional particles in RuCl$_3$

Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct comparison of the Raman susceptibility of RuCl3 with quantum Monte Carlo (QMC) results for the Kitaev QSLs. Moreover, we further confirm the fractional nature of the magnetic excitations, which is given by creating a pair of fermionic quasiparticles. Interestingly, this fermionic response remains valid in the non-Kitaev range. Our results and focus on the use of the Raman susceptibility provide a stringent new test for future theoretical and experimental studies of QSLs.

cond-mat.str-el↗

New material platform for superconducting transmon qubits with coherence times exceeding 0.3 milliseconds

The superconducting transmon qubit is a leading platform for quantum computing and quantum science. Building large, useful quantum systems based on transmon qubits will require significant improvements in qubit relaxation and coherence times, which are orders of magnitude shorter than limits imposed by bulk properties of the constituent materials. This indicates that relaxation likely originates from uncontrolled surfaces, interfaces, and contaminants. Previous efforts to improve qubit lifetimes have focused primarily on designs that minimize contributions from surfaces. However, significant improvements in the lifetime of two-dimensional transmon qubits have remained elusive for several years. Here, we fabricate two-dimensional transmon qubits that have both lifetimes and coherence times with dynamical decoupling exceeding 0.3 milliseconds by replacing niobium with tantalum in the device. We have observed increased lifetimes for seventeen devices, indicating that these material improvements are robust, paving the way for higher gate fidelities in multi-qubit processors.

quant-ph↗

Understanding the Instability of the Halide Perovskite CsPbI$_3$ through Temperature-Dependent Structural Analysis

Despite the tremendous interest in halide perovskites in solar cells, the reason that the all-inorganic perovskite CsPbI$_3$ is unstable at room temperature remains mysterious. Here single-crystal X-ray diffraction and powder pair distribution function (PDF) measurements characterize bulk perovskite CsPbI$_3$ from 100 to 295 K to elucidate its thermodynamic instability. While Cs occupies a single site from 100 to 150 K, it splits between two sites from 175 to 295 K with the second site having a lower effective coordination number, which along with other structural parameters suggests that Cs rattles in its coordination polyhedron. PDF measurements reveal that on the length scale of the unit cell, the Pb-I octahedra concurrently become greatly distorted, with one of the I-Pb-I angles approaching 82° compared to the ideal 90°. The rattling of Cs, low number of Cs-I contacts, and high degree of octahedral distortion cause the instability of perovskite-phase CsPbI$_3$. These results provide detailed structural information that may help to engineer greater stability of CsPbI$_3$ and other all-inorganic perovskites for use in solar cells.

cond-mat.mtrl-sci↗

Concurrent probing of electron-lattice dephasing induced by photoexcitation in 1T-TaSeTe using ultrafast electron diffraction

It has been technically challenging to concurrently probe the electrons and the lattices in materials during non-equilibrium processes, allowing their correlations to be determined. Here, in a single set of ultrafast electron diffraction patterns taken on the charge-density-wave (CDW) material 1T-TaSeTe, we discover a temporal shift in the diffraction intensity measurements as a function of scattering angle. With the help of dynamic models and theoretical calculations, we show that the ultrafast electrons probe both the valence-electron and lattice dynamic processes, resulting in the temporal shift measurements. Our results demonstrate unambiguously that the CDW is not merely a result of the periodic lattice deformation ever-present in 1T-TaSeTe but has significant electronic origin. This method demonstrates a novel approach for studying many quantum effects that arise from electron-lattice dephasing in molecules and crystals for next-generation devices.

cond-mat.mtrl-sci↗

Multiple ferromagnetic transitions and structural distortion in the van-der-Waals ferromagnet VI$_3$ at ambient and finite pressures

We present a combined study of zero-field $^{51}$V and $^{127}$I NMR at ambient pressure and specific heat and magnetization measurements under pressure up to 2.08 GPa on bulk single crystals of the van-der-Waals ferromagnet VI$_3$. At ambient pressure, our results consistently demonstrate that VI$_3$ undergoes a structural transition at $T_s \approx $78 K, followed by two subsequent ferromagnetic transitions at $T_{FM1} \approx $50 K and $T_{FM2} \approx $36 K upon cooling. At lowest temperature ($T < T_{FM2}$), two magnetically-ordered V sites exist, whereas only one magnetically-ordered V site is observed for $T_{FM1} < T\,< T_{FM2}$. Whereas $T_{FM1}$ is almost unaffected by external pressure, $T_{FM2}$ is highly responsive to pressure and merges with the $T_{FM1}$ line at $p \approx 0.6 $GPa. At even higher pressures ($p \approx $1.25\,GPa), the $T_{FM2}$ line merges with the structural transition at $T_s$ which becomes moderately suppressed with $p$ for $p < 1.25$ GPa. Taken together, our data point towards a complex magnetic structure and an interesting interplay of magnetic and structural degrees of freedom in VI$_3$.

cond-mat.str-el↗

Weak-field induced nonmagnetic state in a Co-based honeycomb

Layered honeycomb magnets are of interest as potential realizations of the Kitaev quantum spin liquid (KQSL), a quantum state with long-range spin entanglement and an exactly solvable Hamiltonian. Conventional magnetically ordered states are present for all currently known candidate materials, however, because non-Kitaev terms in the Hamiltonians obscure the Kitaev physics. Current experimental studies of the KQSL are focused on 4d- or 5d-transition-metal-based honeycombs, in which strong spin-orbit coupling can be expected, yielding Kitaev interaction that dominate in an applied magnetic field. In contrast, for 3d-based layered honeycomb magnets, spin orbit coupling is weak and thus Kitaev-physics should be substantially less accessible. Here we report our studies on BaCo2(AsO4)2, for which we find that the magnetic order associated with the non-Kitaev interactions can be fully suppressed by a relatively low magnetic field, yielding a non-magnetic material and implying the presence of strong magnetic frustration and weak non-Kitaev interactions.

cond-mat.str-el↗

Narrow optical linewidths in erbium implanted in TiO$_2$

Atomic and atom-like defects in the solid-state are widely explored for quantum computers, networks and sensors. Rare earth ions are an attractive class of atomic defects that feature narrow spin and optical transitions that are isolated from the host crystal, allowing incorporation into a wide range of materials. However, the realization of long electronic spin coherence times is hampered by magnetic noise from abundant nuclear spins in the most widely studied host crystals. Here, we demonstrate that Er$^{3+}$ ions can be introduced via ion implantation into TiO$_2$, a host crystal that has not been studied extensively for rare earth ions and has a low natural abundance of nuclear spins. We observe efficient incorporation of the implanted Er$^{3+}$ into the Ti$^{4+}$ site (40% yield), and measure narrow inhomogeneous spin and optical linewidths (20 and 460 MHz, respectively) that are comparable to bulk-doped crystalline hosts for Er$^{3+}$. This work demonstrates that ion implantation is a viable path to studying rare earth ions in new hosts, and is a significant step towards realizing individually addressed rare earth ions with long spin coherence times for quantum technologies.

physics.app-ph↗

Direct Evidence for Fermi Statistics from Proximity to the Kitaev Spin Liquid in RuCl3

A key characteristic of quantum spin liquids(QSL) is the presence of fractional excitations related to their entanglement properties, yet experimental verification of their statistics is missing. For example, in the potential Kitaev spin liquid, RuCl3 experiments uncovered signs of fractional particles, though not their Fermi statistics. Here we employ Raman scattering to reveal the true nature of the magnetic excitations, using improved experimental methods and analysis to remove the influence of laser heating and thermal fluctuations. Via the energy loss and gain spectra, we extract the energy and temperature dependence of the Raman susceptibility to prove RuCl3's magnetic response is given by pair creation of fermionic excitations. Furthermore, by comparing with quantum Monte Carlo (QMC) results for the exact Kitaev limit, we are able to discern the energy and temperature range where additional interaction terms are important. Our results open new directions in QSL research by providing a new way to investigate fractional excitations and the importance of terms causing spinon confinement.

cond-mat.str-el↗

Single crystals of the layered dichalcogenides MoS2 and WS2 grown by liquid phase transport

The growth of single crystals of MoS2 and WS2 by materials transport through a liquid salt flux made from a low melting mixture of NaCl and CsCl is described. The crystals are characterized by single crystal X-ray diffraction, which reveals that they are 2H-MoS2 with a small percentage (about 3%) of 3R intergrowths. The 2H-WS2 crystals display less than 1% of 3R intergrowths. Photoluminescence spectra of exfoliated monolayers suggest that MoS2 grown by this method has superior crystallinity in comparison to commercially-available MoS2 crystals.

cond-mat.mtrl-sci↗

Kinetically Stable Single Crystals of Perovskite-Phase CsPbI${_3}$

We use solid-state methods to synthesize single crystals of perovskite-phase cesium lead iodide ($γ$-CsPbI3) that are kinetically stable at room temperature. Single crystal X-ray diffraction characterization shows that the compound is orthorhombic with the GdFeO3 structure at room temperature. Unlike conventional semiconductors, the optical absorption and the joint density-of-states of bulk $γ$-CsPbI3 is greatest near the band edge and decreases beyond Eg for at least 1.9 eV. Bulk $γ$-CsPbI3 does not show an excitonic resonance and has an optical band gap of 1.63(3) eV, ~90 meV smaller than has been reported in thin films; these and other differences indicate that previously-measured thin film $γ$-CsPbI3 shows signatures of quantum confinement. By flowing gases over $γ$-CsPbI3 during in situ powder X-ray diffraction measurements, we confirm that $γ$-CsPbI3 is stable to oxygen but rapidly and catalytically converts to non-perovskite $δ$-CsPbI3 in the presence of moisture. Our results on bulk $γ$-CsPbI3 provide vital parameters for theoretical and experimental investigations into perovskite-phase CsPbI3 that will the guide the design and synthesis of atmospherically stable inorganic halide perovskites.

physics.app-ph↗

Strong quantum fluctuations in a quantum spin liquid candidate with a Co-based triangular lattice

Currently under active study in condensed matter physics, both theoretically and experimentally, are quantum spin liquid (QSL) states, in which no long-range magnetic ordering appears at low temperatures due to strong quantum fluctuations of the magnetic moments. The existing QSL candidates all have their intrinsic disadvantages, however, and solid evidence for quantum fluctuations is scarce. Here we report a new compound, Na$_{2}$BaCo(PO$_{4}$)$_{2}$, a geometrically frustrated system with effective spin-1/2 local moments for Co$^{2+}$ ions on an isotropic two-dimensional triangular lattice. Magnetic susceptibility and neutron scattering experiments show no magnetic ordering down to 0.05 K. Thermodynamic measurements show that there is a tremendous amount of magnetic entropy present below 1 K in zero applied magnetic field. The presence of localized low-energy spin fluctuations is revealed by inelastic neutron measurements. At low applied fields, these spin excitations are confined to low energy and contribute to the anomalously large specific heat. In larger applied fields, the system reverts to normal behavior as evident by both neutron and thermodynamic results. Our experimental characterization thus reveals that this new material is an excellent candidate for the experimental realization of a quantum spin liquid state.

cond-mat.str-el↗

Real-space imaging and flux noise spectroscopy of magnetic dynamics in Ho$_2$Ti$_2$O$_7$

Holmium titanate (Ho$_2$Ti$_2$O$_7$) is a rare earth pyrochlore and a canonical example of a classical spin ice material. Despite the success of magnetic monopole models, a full understanding of the energetics and relaxation rates in this material has remained elusive, while recent studies have shown that defects play a central role in the magnetic dynamics. We used a scanning superconducting quantum interference device (SQUID) microscope to study the spatial and temporal magnetic fluctuations in three regions with different defect densities from a Ho$_2$Ti$_2$O$_7$ single crystal as a function of temperature. We found that the magnetic flux noise power spectra are not determined by simple thermally-activated behavior and observed evidence of magnetic screening that is qualitatively consistent with Debye-like screening due to a dilute gas of low-mobility magnetic monopoles. This work establishes magnetic flux spectroscopy as a powerful tool for studying materials with complex magnetic dynamics, including frustrated correlated spin systems.

cond-mat.str-el↗

Ultrafast decoupling of atomic sublattices in a charge-density-wave material

Atomic rearrangements within crystals lie at the foundation of electron-phonon-coupled phenomena such as metal-insulator transition and superconductivity. Advanced laser-pump-probe studies have recently focused on various charge-density-wave (CDW) materials to sharpen our understanding of the charge-lattice entanglement, where non-thermal melting of the CDW state is evident from the enhanced Bragg diffraction peak intensities - attributed to the dominance of the metal-atom dynamics over the nonmetal-anion one. Here using ultrafast MeV electron diffraction on the prototypical CDW material 1T-TaSeTe, we observe an unusual coexistence of systematically enhanced and suppressed Bragg peak intensities upon the CDW suppression, indicating a dominance of nonmetal-anion dynamics during photoexcitation. By tracking these atomic trajectories quantitatively through the ultrafast process, we identify a transient state that manifests itself as an unexpected decoupling of the Ta and Se/Te sublattices. These findings unambiguously unveil a new kind of laser manipulations of lattice order parameters, which has potentials in creating new quantum states and discerning hidden phases such as intra-unit-cell orders.

cond-mat.mtrl-sci↗

A New Magnetic Topological Quantum Material Candidate by Design

Magnetism, when combined with an unconventional electronic band structure, can give rise to forefront electronic properties such as the quantum anomalous Hall effect, axion electrodynamics, and Majorana fermions. Here we report the characterization of high-quality crystals of EuSn$_2$P$_2$, a new quantum material specifically designed to engender unconventional electronic states plus magnetism. EuSn$_2$P$_2$ has a layered, Bi$_2$Te$_3$-type structure. Ferromagnetic interactions dominate the Curie-Weiss susceptibility, but a transition to antiferromagnetic ordering occurs near 30 K. Neutron diffraction reveals that this is due to two-dimensional ferromagnetic spin alignment within individual Eu layers and antiferromagnetic alignment between layers - this magnetic state surrounds the Sn-P layers at low temperatures. The bulk electrical resistivity is sensitive to the magnetism. Electronic structure calculations reveal that EuSn$_2$P$_2$ might be a strong topological insulator, which can be a new magnetic topological quantum material (MTQM) candidate. The calculations show that surface states should be present, and they are indeed observed by ARPES measurements.

cond-mat.mtrl-sci↗

Ionic and electronic properties of the topological insulator Bi$_2$Te$_2$Se investigated using $β$-detected nuclear magnetic relaxation and resonance of $^8$Li

We report measurements on the high temperature ionic and low temperature electronic properties of the 3D topological insulator Bi$_2$Te$_2$Se using ion-implanted $^8$Li $β$-detected nuclear magnetic relaxation and resonance. With implantation energies in the range 5-28 keV, the probes penetrate beyond the expected range of the topological surface state, but are still within 250 nm of the surface. At temperatures above ~150 K, spin-lattice relaxation measurements reveal isolated $^8$Li$^{+}$ diffusion with an activation energy $E_{A} = 0.185(8)$ eV and attempt frequency $τ_{0}^{-1} = 8(3) \times 10^{11}$ s$^{-1}$ for atomic site-to-site hopping. At lower temperature, we find a linear Korringa-like relaxation mechanism with a field dependent slope and intercept, which is accompanied by an anomalous field dependence to the resonance shift. We suggest that these may be related to a strong contribution from orbital currents or the magnetic freezeout of charge carriers in this heavily compensated semiconductor, but that conventional theories are unable to account for the extent of the field dependence. Conventional NMR of the stable host nuclei may help elucidate their origin.

cond-mat.mtrl-sci↗

Observation of the nonlinear Hall effect under time reversal symmetric conditions

The electrical Hall effect is the production of a transverse voltage under an out-of-plane magnetic field. Historically, studies of the Hall effect have led to major breakthroughs including the discoveries of Berry curvature and the topological Chern invariants. In magnets, the internal magnetization allows Hall conductivity in the absence of external magnetic field. This anomalous Hall effect (AHE) has become an important tool to study quantum magnets. In nonmagnetic materials without external magnetic fields, the electrical Hall effect is rarely explored because of the constraint by time-reversal symmetry. However, strictly speaking, only the Hall effect in the linear response regime, i.e., the Hall voltage linearly proportional to the external electric field, identically vanishes due to time-reversal symmetry. The Hall effect in the nonlinear response regime, on the other hand, may not be subject to such symmetry constraints. Here, we report the observation of the nonlinear Hall effect (NLHE) in the electrical transport of the nonmagnetic 2D quantum material, bilayer WTe2. Specifically, flowing an electrical current in bilayer WTe2 leads to a nonlinear Hall voltage in the absence of magnetic field. The NLHE exhibits unusual properties sharply distinct from the AHE in metals: The NLHE shows a quadratic I-V characteristic; It strongly dominates the nonlinear longitudinal response, leading to a Hall angle of about 90 degree. We further show that the NLHE directly measures the "dipole moment" of the Berry curvature, which arises from layer-polarized Dirac fermions in bilayer WTe2. Our results demonstrate a new Hall effect and provide a powerful methodology to detect Berry curvature in a wide range of nonmagnetic quantum materials in an energy-resolved way.

cond-mat.mes-hall↗

Electrically Tunable Low Density Superconductivity in a Monolayer Topological Insulator

The capability to switch electrically between superconducting and insulating states of matter represents a novel paradigm in the state-of-the-art engineering of correlated electronic systems. An exciting possibility is to turn on superconductivity in a topologically non-trivial insulator, which provides a route to search for non-Abelian topological states. However, existing demonstrations of superconductor-insulator switches have involved only topologically trivial systems, and even those are rare due to the stringent requirement to tune the carrier density over a wide range. Here we report reversible, in-situ electrostatic on off switching of superconductivity in a recently established quantum spin Hall insulator, namely monolayer tungsten ditelluride (WTe2). Fabricated into a van der Waals field effect transistor, the monolayer's ground state can be continuously gate-tuned from the topological insulating to the superconducting state, with critical temperatures Tc up to ~ 1 Kelvin. The critical density for the onset of superconductivity is estimated to be ~ 5 x 10^12 cm^-2, among the lowest for two-dimensional (2D) superconductors. Our results establish monolayer WTe2 as a material platform for engineering novel superconducting nanodevices and topological phases of matter.

cond-mat.mes-hall↗