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Stephen D. Wilson

Publications and source records attributed to Stephen D. Wilson.

At least 91 records · Page 5Linked to original sources
arXiv2023

Pressure evolution of electron dynamics in the superconducting kagome metal CsV$_3$Sb$_5$

The coexistence of the charge-density wave (CDW) and superconducting phases and their tunability under external pressure remains one of the key points in understanding the electronic structure of $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) kagome metals. Here, we employ synchrotron-based infrared spectroscopy assisted by density-functional calculations to study the pressure evolution of the electronic structure at room temperature up to 17 GPa experimentally. The optical spectrum of CsV$_3$Sb$_5$ is characterized by the presence of localized carriers seen as a broad peak at finite frequencies in addition to the conventional metallic Drude response. The pressure dependence of this low-energy peak reflects the re-entrant behavior of superconductivity and may be interpreted in terms of electron-phonon coupling, varying with the growth and shrinkage of the Fermi surface. Moreover, drastic modifications in the low-energy interband absorptions are observed upon the suppression of CDW. These changes are related to the upward shift of the Sb2 $p_x+p_y$ band that eliminates part of the Fermi surface around the $M$-point, whereas band saddle points do not move significantly. These observations shed new light on the mixed electronic and lattice origin of the CDW in CsV$_3$Sb$_5$.

cond-mat.str-el↗
arXiv2023

Quantitative investigation of the short-range magnetic correlations in candidate quantum spin liquid NaYbO$_2$

We present a neutron diffraction study of NaYbO$_2$, a candidate quantum spin liquid compound hosting a geometrically frustrated triangular lattice of magnetic Yb$^{3+}$ ions. We observe diffuse magnetic scattering that persists to at least 20 K, demonstrating the presence of short-range magnetic correlations in this system up to a relatively high energy scale. Using reverse Monte Carlo and magnetic pair distribution function analysis, we confirm the predominant antiferromagnetic nature of these correlations and show that the diffuse scattering data can be well described by noninteracting layers of XY spins on the triangular lattice. We rule out Ising spins and short-range-ordered stripe or 120$^{\circ}$ phases as candidate ground states of NaYbO$_2$. These results are consistent with a possible QSL ground state in NaYbO$_2$ and showcase the benefit of combined reciprocal- and real-space analysis of materials with short-range magnetic correlations.

cond-mat.str-el↗
arXiv2023

Canted Antiferromagnetism in Polar MnSiN$_2$ with High Néel Temperature

MnSiN$_2$ is a transition metal nitride with Mn and Si ions displaying an ordered distribution on the cation sites of a distorted wurtzite-derived structure. The Mn$^{2+}$ ions reside on a 3D diamond-like covalent network with strong superexchange pathways. We simulate its electronic structure and find that the N anions in MnSiN$_2$ act as $σ$- and $π$-donors, which serve to enhance the N-mediated superexchange, leading to the high Néel ordering temperature of $T_N$ = 443 K. Polycrystalline samples of MnSiN$_2$ were prepared to reexamine the magnetic structure and resolve previously reported discrepancies. An additional magnetic canting transition is observed at $T_\mathrm{cant}$ = 433 K and the precise canted ground state magnetic structure has been resolved using a combination of DFT calculations and powder neutron diffraction. The calculations favor a $G$-type antiferromagnetic spin order with lowering to $Pc^\prime$. Irreducible representation analysis of the magnetic Bragg peaks supports the lowering of the magnetic symmetry. The computed model includes a 10$^\circ$ rotation of the magnetic spins away from the crystallographic $c$-axis consistent with measured powder neutron diffraction data modeling and a small canting of 0.6$^\circ$.

cond-mat.mtrl-sci↗
arXiv2023

Revisiting spin ice physics in the ferromagnetic Ising pyrochlore Pr$_2$Sn$_2$O$_7$

Pyrochlore materials are characterized by their hallmark network of corner-sharing rare-earth tetrahedra, which can produce a wide array of complex magnetic ground states. Ferromagnetic Ising pyrochlores often obey the "two-in-two-out" spin ice rules, which can lead to a highly-degenerate spin structure. Large moment systems, such as Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, tend to host a classical spin ice state with low-temperature spin freezing and emergent magnetic monopoles. Systems with smaller effective moments, such as Pr$^{3+}$-based pyrochlores, have been proposed as excellent candidates for hosting a "quantum spin ice" characterized by entanglement and a slew of exotic quasiparticle excitations. However, experimental evidence for a quantum spin ice state has remained elusive. Here, we show that the low-temperature magnetic properties of Pr$_2$Sn$_2$O$_7$ satisfy several important criteria for continued consideration as a quantum spin ice. We find that Pr$_2$Sn$_2$O$_7$ exhibits a partially spin-frozen ground state with a large volume fraction of dynamic magnetism. Our comprehensive bulk characterization and neutron scattering measurements enable us to map out the magnetic field-temperature phase diagram, producing results consistent with expectations for a ferromagnetic Ising pyrochlore. We identify key hallmarks of spin ice physics, and show that the application of small magnetic fields ($μ_0 H_c \sim$0.75T) suppresses the spin ice state and induces a long-range ordered magnetic structure. Together, our work clarifies the current state of Pr$_2$Sn$_2$O$_7$ and encourages future studies aimed at exploring the potential for a quantum spin ice ground state in this system.

cond-mat.str-el↗
arXiv2023

Soft-Chemical Synthesis, Structure Evolution, and Insulator-to-Metal Transition in a Prototypical Metal Oxide, λ-RhO$_2$

$λ$-RhO$_2$, a prototype 4d transition metal oxide, has been prepared by oxidative delithiation of spinel LiRh$_2$O$_4$ using ceric ammonium nitrate. Average-structure studies of this RhO$_2$ polytype, including synchrotron powder X-ray diffraction and electron diffraction, indicate the room temperature structure to be tetragonal, in the space group I41/amd, with a first-order structural transition to cubic Fd-3m at T = 345 K on warming. Synchrotron X-ray pair distribution function analysis and $^7$Li solid state nuclear magnetic resonance measurements suggest that the room temperature structure displays local Rh-Rh bonding. The formation of these local dimers appears to be associated with a metal-to insulator transition with a non-magnetic ground state, as also supported by density functional theory-based electronic structure calculations. This contribution demonstrates the power of soft chemistry to kinetically stabilize a surprisingly simple binary oxide compound.

cond-mat.mtrl-sci↗
arXiv2023

Frustrated charge order and cooperative distortions in ScV6Sn6

Here we study the stability of charge order in the kagome metal ScV6Sn6. Synchrotron x-ray diffraction measurements reveal high-temperature, short-range charge correlations at the wave vectors along q=(1/3,1/3,1/2) whose inter-layer correlation lengths diverge upon cooling. At the charge order transition, this divergence is interrupted and long-range order freezes in along q=(1/3,1/3,1/3), as previously reported, while disorder enables the charge correlations to persist at the q=(1/3,1/3,1/2) wave vector down to the lowest temperatures measured. Both short-range and long-range charge correlations seemingly arise from the same instability and both are rapidly quenched upon the introduction of larger Y ions onto the Sc sites. Our results validate the theoretical prediction of the primary lattice instability at q=(1/3,1/3,1/2), and we present a heuristic picture for viewing the frustration of charge order in this compound.

cond-mat.str-el↗
arXiv2023

Electronic properties of kagome metal ScV6Sn6 using high field torque magnetometry

This work presents electronic properties of the kagome metal ScV6Sn6 using de Haas-van Alphen (dHvA) oscillations and density functional theory (DFT) calculations. The torque signal with the applied fields up to 43 T shows clear dHvA oscillations with six major frequencies, five of them are below 400 T (low frequencies) and one is nearly 2800 T (high frequency). The Berry phase calculated using the Landau level fan diagram near the quantum limit is approximately π, which suggests the non-trivial band topology in ScV6Sn6. To explain the experimental data, we computed the electronic band structure and Fermi surface using DFT in both the pristine and charge density wave (CDW) phases. Our results confirm that the CDW phase is energetically favorable, and the Fermi surface undergoes a severe reconstruction in the CDW state. Furthermore, the angular dependence of the dHvA frequencies are consistent with the DFT calculations. The detailed electronic properties presented here are invaluable for understanding the electronic structure and CDWorder in ScV6Sn6, as well as in other vanadium-based kagome systems.

cond-mat.str-el↗
arXiv2023

Three-state nematicity and magneto-optical Kerr effect in the charge density waves in kagome superconductors

The kagome lattice provides a fascinating playground to study geometrical frustration, topology and strong correlations. The newly-discovered kagome metals AV$_3$Sb$_5$ (where A can refer to K, Rb, or Cs) exhibit phenomena including topological band structure, symmetry-breaking charge-density waves and superconductivity. Nevertheless, the nature of the symmetry breaking in the charge-density wave phase is not yet clear, despite the fact that it is crucial in order to understand whether the superconductivity is unconventional. In this work, we perform scanning birefringence microscopy on all three members of this family and find that six-fold rotation symmetry is broken at the onset of the charge-density wave transition in all these compounds. We show that the three nematic domains are oriented at 120$^\circ$ to each other and propose that staggered charge-density wave orders with a relative $π$ phase shift between layers is a possibility that can explain these observations. We also perform magneto-optical Kerr effect and circular dichroism measurements. The onset of both signals is at the transition temperature, indicating broken time-reversal symmetry and the existence of the long-sought loop currents in that phase.

cond-mat.str-el↗
arXiv2023

Magnetic order in the $S_{\mathrm{eff}}$ = 1/2 triangular-lattice compound NdCd$_3$P$_3$

We present and characterize a new member of the $R$Cd$_3$P$_3$ ($R$= rare earth) family of materials, NdCd$_3$P$_3$, which possesses Nd$^{3+}$ cations arranged on well-separated triangular lattice layers. Magnetic susceptibility and heat capacity measurements demonstrate a likely $S_{\mathrm{eff}}$ = 1/2 ground state, and also reveal the formation of long-range antiferromagnetic order at $T_{N} = 0.34$ K. Via measurements of magnetization, heat capacity, and electrical resistivity, we characterize the electronic properties of NdCd$_3$P$_3$ and compare results to density functional theory calculations.

cond-mat.str-el↗
arXiv2023

YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$, vanadium-based kagome metals with Yb$^{2+}$ and Eu$^{2+}$ zig-zag chains

Here we present YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$, two new compounds exhibiting slightly distorted vanadium-based kagome nets interleaved with zig-zag chains of divalent Yb$^{2+}$ and Eu$^{2+}$ ions. Single crystal growth methods are reported alongside magnetic, electronic, and thermodynamic measurements. YbV$_3$Sb$_4$ is a nonmagnetic metal with no collective phase transitions observed between 60mK and 300K. Conversely, EuV$_3$Sb$_4$ is a magnetic kagome metal exhibiting easy-plane ferromagnetic-like order below $T_\text{C}$=32K with signatures of noncollinearity under low field. Our discovery of YbV$_3$Sb$_4$ and EuV$_3$Sb$_4$ demonstrate another direction for the discovery and development of vanadium-based kagome metals while incorporating the chemical and magnetic degrees of freedom offered by a rare-earth sublattice.

cond-mat.mtrl-sci↗
arXiv2023

Refined Spin Wave Model and Multi-magnon Bound States in $Li_{2}CuO_{2}$

Here we report a study of the spin dynamics in the ferromagnetic chain compound $Li_{2}CuO_{2}$. Inelastic neutron scattering measurements allow for the spin Hamiltonian to be determined using a $J_{1}-J_{2}$ $XXZ$-Heisenberg spin chain model with weak interchain interactions. The primary exchange parameters determined from our data are qualitatively consistent with those of Lorenz $et$ $al.$ [Europhys. Lett. 88, 37002 (2009)], and our data allow for the resolution of additional interchain exchange interactions. We also observe the formation of two- and, potentially, three-magnon bound states. The two-magnon bound state exists only in the magnetically ordered phase of this material, consistent with stabilization by the weak, Ising-like exchange anisotropy of the nearest-neighbor intrachain interaction. In contrast, the potential three-magnon state persists in a finite temperature regime above $T_{N}$, indicating an unconventional character. Our results establish $Li_{2}CuO_{2}$ as an experimental platform for the study of exchange anisotropy-stabilized bound states in a ferromagnetic chain.

cond-mat.str-el↗
arXiv2023

Unidirectional coherent quasiparticles in the high-temperature rotational symmetry broken phase of AV3Sb5 kagome superconductors

Kagome metals AV3Sb5 (where the A can stand for K, Cs, or Rb) display a rich phase diagram of correlated electron states, including superconductivity and density waves. Within this landscape, recent experiments revealed signs of a transition below approximately 35 K attributed to an electronic nematic phase that spontaneously breaks rotational symmetry of the lattice. Here, we show that rotational symmetry breaking initiates universally at a high temperature in these materials, toward the 2 x 2 charge density wave transition temperature. We do this via spectroscopic-imaging scanning tunneling microscopy and study atomic-scale signatures of electronic symmetry breaking across several materials in the AV3Sb5 family: CsV3Sb5, KV3Sb5 and Sn-doped CsV3Sb5. Below a significantly lower temperature of about 30 K, we measure quantum interference of quasiparticles, a key signature for the formation of a coherent electronic state. These quasiparticles display a pronounced unidirectional feature in reciprocal space that strengthens as the superconducting state is approached. Our experiments reveal that high-temperature rotation symmetry breaking and the charge ordering states are separated from the superconducting ground state by an intermediate-temperature regime with coherent unidirectional quasiparticles. This picture is phenomenologically different compared to that in high-temperature superconductors, shedding light on the complex nature of rotation symmetry breaking in AV3Sb5 kagome superconductors.

cond-mat.str-el↗
arXiv2023

Electron-hole asymmetry in the phase diagram of carrier-tuned CsV$_3$Sb$_5$

Here we study the effect of electron doping the kagome superconductor CsV$_3$Sb$_5$. Single crystals and powders of CsV$_3$Sb$_{5-x}$Te$_x$ are synthesized and characterized via magnetic susceptibility, nuclear quadrupole resonance, and x-ray diffraction measurements, where we observe a slight suppression of the charge density wave transition temperature and superconducting temperature with the introduction of electron dopants. In contrast to hole-doping, both transitions survive relatively unperturbed up to the solubility limit of Te within the lattice. A comparison is presented between the electronic phase diagrams of electron- and hole-tuned CsV$_3$Sb$_5$.

cond-mat.supr-con↗
arXiv2023

Electronic nematicity without charge density waves in titanium-based kagome metal

Layered crystalline materials that consist of transition metal atoms on a kagome network have emerged as a versatile platform to study unusual electronic phenomena. For example, in the vanadium-based kagome superconductors AV3Sb5 (where A can stand for K, Cs, or Rb) there is a parent charge density wave phase that appears to simultaneously break both the translational and the rotational symmetry of the lattice. Here, we show a contrasting situation where electronic nematic order - the breaking of rotational symmetry without the breaking of translational symmetry - can occur without a corresponding charge density wave. We use spectroscopic-imaging scanning tunneling microscopy to study the kagome metal CsTi3Bi5 that is isostructural to AV3Sb5 but with a titanium atom kagome network. CsTi3Bi5 does not exhibit any detectable charge density wave state, but comparison to density functional theory calculations reveals substantial electronic correlation effects at low energies. Comparing the amplitudes of scattering wave vectors along different directions, we discover an electronic anisotropy that breaks the six-fold symmetry of the lattice, arising from both in-plane and out-of-plane titanium-derived d orbitals. Our work uncovers the role of electronic orbitals in CsTi3Bi5, suggestive of a hexagonal analogue of the nematic bond order in Fe-based superconductors.

cond-mat.str-el↗
arXiv2023

A $j_{\rm eff}=1/2$ Kitaev material on the triangular lattice: The case of NaRuO$_2$

Motivated by recent reports of a quantum disordered ground state in the triangular lattice compound NaRuO$_2$, we derive a $j_{\rm eff}=1/2$ magnetic model for this system by means of first-principles calculations. The pseudospin Hamiltonian is dominated by bond-dependent off-diagonal $Γ$ interactions, complemented by a ferromagnetic Heisenberg exchange and a notably antiferromagnetic Kitaev term. In addition to bilinear interactions, we find a sizable four-spin ring exchange contribution with a strongly anisotropic character, which has been so far overlooked when modeling Kitaev materials. The analysis of the magnetic model, based on the minimization of the classical energy and exact diagonalization of the quantum Hamiltonian, points toward the existence of a rather robust easy-plane ferromagnetic order, which cannot be easily destabilized by physically relevant perturbations.

cond-mat.str-el↗
arXiv2023

NaRuO$_2$: Kitaev-Heisenberg exchange in triangular-lattice setting

Kitaev exchange, a new paradigm in quantum magnetism research, occurs for 90$^{\circ}$ metal-ligand-metal links, $t_{2g}^5$ transition ions, and sizable spin-orbit coupling. It is being studied in honeycomb compounds but also on triangular lattices. While for the former it is known by now that the Kitaev intersite couplings are ferromagnetic, for the latter the situation is unclear. Here we pin down the exchange mechanisms and determine the effective coupling constants in the $t_{2g}^5$ triangular-lattice material NaRuO$_2$, recently found to host a quantum spin liquid ground state. We show that, compared to honeycomb compounds, the characteristic triangular-lattice cation surroundings dramatically affect exchange paths and effective coupling parameters, changing the Kitaev interactions to antiferromagnetic. The quantum chemical analysis and subsequent effective spin model computations provide perspective onto the nature of the experimentally observed quantum spin liquid -- it seemingly implies finite longer-range exchange, and the atypical proximity to ferromagnetic order is related to sizable ferromagnetic Heisenberg nearest-neighbor couplings.

cond-mat.str-el↗
arXiv2023

Incommensurate Magnetic Order in the $\mathbb{Z}_2$ Kagome Metal GdV$_6$Sn$_6$

We characterize the magnetic ground state of the topological kagome metal GdV$_6$Sn$_6$ via resonant X-ray diffraction. Previous magnetoentropic studies of GdV$_6$Sn$_6$ suggested the presence of a modulated magnetic order distinct from the ferromagnetism that is easily polarized by the application of a magnetic field. Diffraction data near the Gd-$L_2$ edge directly resolve a $c$-axis modulated spin structure order on the Gd sublattice with an incommensurate wave vector that evolves upon cooling toward a partial lock-in transition. While equal moment (spiral) and amplitude (sine) modulated spin states can not be unambiguously discerned from the scattering data, the overall phenomenology suggests an amplitude modulated state with moments predominantly oriented in the $ab$-plane. Comparisons to the ``double-flat" spiral state observed in Mn-based $R$Mn$_6$Sn$_6$ kagome compounds of the same structure type are discussed.

cond-mat.str-el↗
arXiv2023

High Resolution Polar Kerr Effect Studies of CsV${}_3$Sb${}_5$: Tests for Time Reversal Symmetry Breaking Below the Charge Order Transition

We report high resolution polar Kerr effect measurements on CsV${}_3$Sb${}_5$ single crystals in search for signatures of spontaneous time reversal symmetry breaking below the charge order transition at $T^* \approx 94$ K. Utilizing two different versions of zero-area loop Sagnac interferometers operating at 1550 nm wavelength, each with the fundamental attribute that without a time reversal symmetry breaking sample at its path, the interferometer is perfectly reciprocal, we find no observable Kerr effect to within the noise floor limit of the apparatus at 30 nanoradians. Simultaneous coherent reflection ratio measurements confirm the sharpness of the charge order transition in the same optical volume as the Kerr measurements. At finite magnetic field we observe a sharp onset of a diamagnetic shift in the Kerr signal at $T^*$, which persists down to the lowest temperature without change in trend. Since 1550 nm is an energy that was shown to capture all features of the optical properties of the material that interact with the charge order transition, we are led to conclude that it is highly unlikely that time reversal symmetry is broken in the charge ordered state in CsV${}_3$Sb${}_5$.

cond-mat.str-el↗