arXiv subjects

Stephen M. Winter

Publications and source records attributed to Stephen M. Winter.

45 records · Page 3Linked to original sources

arXiv2018

Evidence for electronically-driven ferroelectricity in the family of strongly correlated dimerized BEDT-TTF molecular conductors

By applying measurements of the dielectric constants and relative length changes to the dimerized molecular conductor $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl, we provide evidence for order-disorder type electronic ferroelectricity which is driven by charge order within the (BEDT-TTF)$_2$ dimers and stabilized by a coupling to the anions. According to our density functional theory calculations, this material is characterized by a moderate strength of dimerization. This system thus bridges the gap between strongly dimerized materials, often approximated as dimer-Mott systems at 1/2 filling, and non- or weakly dimerized systems at 1/4 filling exhibiting charge order. Our results indicate that intra-dimer charge degrees of freedom are of particular importance in correlated $κ$-(BEDT-TTF)$_2$X salts and can create novel states, such as electronically-driven multiferroicity or charge-order-induced quasi-1D spin liquids.

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arXiv2018

Detuning the Honeycomb of $α$-RuCl$_{3}$: Pressure-Dependent Optical Studies Reveal Broken Symmetry

The honeycomb Mott insulator $α$-RuCl$_3$ loses its low-temperature magnetic order by pressure. We report clear evidence for a dimerized structure at $P>1$ GPa and observe the breakdown of the relativistic $j_{\rm eff}$ picture in this regime strongly affecting the electronic properties. A pressure-induced Kitaev quantum spin liquid cannot occur in this broken symmetry state. We shed light on the new phase by broad-band infrared spectroscopy of the low-temperature properties of $α$-RuCl$_{3}$ and ab initio density functional theory calculations, both under hydrostatic pressure.

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arXiv2018

Insights from experiment and $ab\,initio$ calculations into the glass-like transition in the molecular conductor $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl

We present high-resolution measurements of the relative length change as a function of temperature of the organic charge-transfer salt $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl. We identify anomalous features at $T_g \approx\,63$ K which can be assigned to a kinetic glass-like ordering transition. By determining the activation energy $E_A$, this glass-like transition can be related to conformational degrees of freedom of the ethylene endgroups of the organic building block BEDT-TTF. As opposed to other $κ$-(BEDT-TTF)$_2X$ salts, we identify a peculiar ethylene endgroup ordering in the present material in which only one of the two crystallographically inequivalent ethylene endgroups is subject to glass-like ordering. This experimental finding is fully consistent with our predictions from $ab\,initio$ calculations from which we estimate the energy differences $ΔE$ and the activation energies $E_A$ between different conformations. The present results indicate that the specific interaction between the ethylene endgroups and the nearby anion layers leads to different energetics of the inequivalent ethylene endgroups, as evidenced by different ratios $E_A/ΔE$. We infer that the ratio $E_A/ΔE$ is a suitable parameter to identify the tendency of ethylene endgroups towards glass-like freezing.

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arXiv2018

Probing $α$-RuCl$_3$ Beyond Magnetic Order: Effects of Temperature and Magnetic Field

Recent studies have brought $α$-RuCl$_3$ to the forefront of experimental searches for materials realizing Kitaev spin-liquid physics. This material exhibits strongly anisotropic exchange interactions afforded by the spin-orbit coupling of the 4d Ru centers. We investigate the dynamical response at finite temperature and magnetic field for a realistic model of the magnetic interactions in $α$-RuCl$_3$. These regimes are thought to host unconventional paramagnetic states that emerge from the suppression of magnetic order. Using exact diagonalization calculations of the quantum model complemented by semi-classical analysis, we find a very rich evolution of the spin dynamics as the applied field suppresses the zigzag order and stabilizes a quantum paramagnetic state that is adiabatically connected to the fully polarized state at high fields. At finite temperature, we observe large redistributions of spectral weight that can be attributed to the anisotropic frustration of the model. These results are compared to recent experiments, and provide a roadmap for further studies of these regimes.

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arXiv2017

Models and Materials for Generalized Kitaev Magnetism

The exactly solvable Kitaev model on the honeycomb lattice has recently received enormous attention linked to the hope of achieving novel spin-liquid states with fractionalized Majorana-like excitations. In this review, we analyze the mechanism proposed by G. Jackeli and G. Khaliullin to identify Kitaev materials based on spin-orbital dependent bond interactions and provide a comprehensive overview of its implications in real materials. We set the focus on experimental results and current theoretical understanding of planar honeycomb systems (Na$_2$IrO$_3$, $α$-Li$_2$IrO$_3$, and $α$-RuCl$_3$), three-dimensional Kitaev materials ($β$- and $γ$-Li$_2$IrO$_3$), and other potential candidates, completing the review with the list of open questions awaiting new insights.

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arXiv2017

Breakdown of Magnons in a Strongly Spin-Orbital Coupled Magnet

The description of quantized collective excitations stands as a landmark in the quantum theory of condensed matter. A prominent example occurs in conventional magnets, which support bosonic magnons - quantized harmonic fluctuations of the ordered spins. In striking contrast is the recent discovery that strongly spin-orbital coupled magnets, such as $α$-RuCl$_3$, may display a broad excitation continuum inconsistent with conventional magnons. Due to incomplete knowledge of the underlying interactions unraveling the nature of this continuum remains challenging. The most discussed explanation refers to a coherent continuum of fractional excitations analogous to the celebrated Kitaev spin liquid. Here we present a more general scenario. We propose that the observed continuum represents incoherent excitations originating from strong magnetic anharmoniticity that naturally occurs in such materials. This scenario fully explains the observed inelastic magnetic response of $α$-RuCl$_3$ and reveals the presence of nontrivial excitations in such materials extending well beyond the Kitaev state.

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arXiv2016

Electronic excitations in $γ$-Li$_2$IrO$_3$

We investigate the electronic properties of the three-dimensional stripyhoneycomb $γ$-Li$_2$IrO$_3$ via relativistic density functional theory calculations as well as exact diagonalization of finite clusters and explore the details of the optical conductivity. Our analysis of this quantity reveals the microscopic origin of the experimentally observed (i) optical transitions and (ii) anisotropic behavior along the various polarization directions. In particular we find that the optical excitations are overall dominated by transitions between $j_\text{eff}$ = 1/2 and 3/2 states and the weight of transitions between $j_\text{eff}$ = 1/2 states at low frequencies can be correlated to deviations from a pure Kitaev description. We furthermore reanalyze within this approach the electronic excitations in the known two-dimensional honeycomb systems $α$-Li$_2$IrO$_3$ and Na$_2$IrO$_3$ and discuss the results in comparison to $γ$-Li$_2$IrO$_3$.

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arXiv2016

Importance of Spin-Orbit Coupling in Organic BEDT-TTF and BEDT-TSF Salts

We investigate the spin-orbit coupling (SOC) effects in $α$- and $κ$-phase BEDT-TTF and BEDT-TSF organic salts. Contrary to the assumption that SOC in organics is negligible due to light C, S, H atoms, we show the relevance of such an interaction in a few representative cases. In the weakly correlated regime, SOC manifests primarily in the opening of energy gaps at degenerate band touching points. This effect becomes especially important for Dirac semimetals such as $α$-(ET)$_2$I$_3$. Furthermore, in the magnetic insulating phase, SOC results in additional anisotropic exchange interactions, which provide a compelling explanation for the controversial field-induced behaviour of the quantum spin-liquid candidate $κ$-(ET)$_2$Cu$_2$(CN)$_3$. We conclude by discussing the importance of SOC for the description of low-energy properties in organics.

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arXiv2016

Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales

In this study, we reanalyze the magnetic interactions in the Kitaev spin liquid candidate materials Na$_2$IrO$_3$, $α$-RuCl$_3$, and $α$-Li$_2$IrO$_3$ using nonperturbative exact diagonalization methods. These methods are more appropriate given the relatively itinerant nature of the systems suggested in previous works. We treat all interactions up to third neighbours on equal footing. The computed terms reveal significant long range coupling, bond-anisotropy, and/or off-diagonal couplings which we argue naturally explain the observed ordered phases in these systems. Given these observations, the potential for realizing the spin-liquid state in real materials is analyzed, and synthetic challenges are defined and explained.

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