An official website of the United States government
Abstract Understanding the interplay between the inherent disorder and the correlated fluctuating-spin ground state is a key element in the search for quantum spin liquids. H3LiIr2O6is considered to be a spin liquid that is proximate to the Kitaev-limit quantum spin liquid. Its ground state shows no magnetic order or spin freezing as expected for the spin liquid state. However, hydrogen zero-point motion and stacking faults are known to be present. The resulting bond disorder has been invoked to explain the existence of unexpected low-energy spin excitations, although data interpretation remains challenging. Here, we use resonant X-ray spectroscopies to map the collective excitations in H3LiIr2O6and characterize its magnetic state. In the low-temperature correlated state, we reveal a broad bandwidth of magnetic excitations. The central energy and the high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. Furthermore, the absence of a momentum dependence to these excitations are consistent with disorder-induced broken translational invariance. Our low-energy data and the energy and width of the crystal field excitations support an interpretation of H3LiIr2O6as a disordered topological spin liquid in close proximity to bond-disordered versions of the Kitaev quantum spin liquid.
more »
« less
Sleuthing out exotic quantum spin liquidity in the pyrochlore magnet Ce2Zr2O7
Abstract The search for quantum spin liquids—topological magnets with fractionalized excitations—has been a central theme in condensed matter and materials physics. Despite numerous theoretical proposals, connecting experiment with detailed theory exhibiting a robust quantum spin liquid has remained a central challenge. Here, focusing on the strongly spin-orbit coupled effectiveS = 1/2 pyrochlore magnet Ce2Zr2O7, we analyze recent thermodynamic and neutron-scattering experiments, to identify a microscopic effective Hamiltonian through a combination of finite temperature Lanczos, Monte Carlo, and analytical spin dynamics calculations. Its parameter values suggest the existence of an exotic phase, aπ-flux U(1) quantum spin liquid. Intriguingly, the octupolar nature of the moments makes them less prone to be affected by magnetic disorder, while also hiding some otherwise characteristic signatures from neutrons, making this spin liquid arguably more stable than its more conventional counterparts.
more »
« less
- PAR ID:
- 10381739
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- npj Quantum Materials
- Volume:
- 7
- Issue:
- 1
- ISSN:
- 2397-4648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract We report on the largest open‐shell graphenic bilayer and also the first example of triply negatively charged radical π‐dimer. Upon three‐electron reduction, bilayer nanographene fragment molecule (C96H24Ar6)2(Ar=2,6‐dimethylphenyl) (12) was transformed to a triply negatively charged species123.−, which has been characterized by single‐crystal X‐ray diffraction, electron paramagnetic resonance (EPR) spectroscopy and magnetic properties on a superconducting quantum interference device (SQUID).123.−features a 96‐center‐3‐electron (96c/3e) pancake bond with a doublet ground state, which can be thermally excited to a quartet state. It consists of 34 π‐fused rings with 96 conjugatedsp2carbon atoms. Spin frustration is observed with the frustration parameterf>31.8 at low temperatures in123.−, which indicates graphene upon reduction doping may behave as a quantum spin liquid.more » « less
-
A<sc>bstract</sc> We analyze a Higgs transition from a U(1) Dirac spin liquid to a gapless ℤ2spin liquid. This ℤ2spin liquid is of relevance to the spinS= 1/2 square lattice antiferromagnet, where recent numerical studies have given evidence for such a phase existing in the regime of high frustration between nearest neighbor and next-nearest neighbor antiferromagnetic interactions (theJ1-J2model), appearing in a parameter regime between the vanishing of Néel order and the onset of valence bond solid ordering. The proximate Dirac spin liquid is unstable to monopole proliferation on the square lattice, ultimately leading to Néel or valence bond solid ordering. As such, we conjecture that this Higgs transition describes the critical theory separating the gapless ℤ2spin liquid of theJ1-J2model from one of the two proximate ordered phases. The transition into the other ordered phase can be described in a unified manner via a transition into an unstable SU(2) spin liquid, which we have analyzed in prior work. By studying the deconfined critical theory separating the U(1) Dirac spin liquid from the gapless ℤ2spin liquid in a 1/Nfexpansion, withNfproportional to the number of fermions, we find a stable fixed point with an anisotropic spinon dispersion and a dynamical critical exponentz≠ 1. We analyze the consequences of this anisotropic dispersion by calculating the angular profiles of the equal-time Néel and valence bond solid correlation functions, and we find them to be distinct. We also note the influence of the anisotropy on the scaling dimension of monopoles.more » « less
-
Abstract We determine the phase diagram of a bilayer, Yao-Lee spin-orbital model with inter-layer interactions (J), for several stackings and moiré superlattices. For AA stacking, a gapped$${{\mathbb{Z}}}_{2}$$ quantum spin liquid phase emerges at a finiteJc. We show that this phase survives in the well-controlled large-Jlimit, where an isotropic honeycomb toric code emerges. For moiré superlattices, a finite-qinter-layer hybridization is stabilized. This connects inequivalent Dirac points, effectively ‘untwisting’ the system. Our study thus provides insight into the spin-liquid phases of bilayer spin-orbital Kitaev materials.more » « less
-
Abstract Polarons and spin-orbit (SO) coupling are distinct quantum effects that play a critical role in charge transport and spin-orbitronics. Polarons originate from strong electron-phonon interaction and are ubiquitous in polarizable materials featuring electron localization, in particular 3d transition metal oxides (TMOs). On the other hand, the relativistic coupling between the spin and orbital angular momentum is notable in lattices with heavy atoms and develops in 5d TMOs, where electrons are spatially delocalized. Here we combine ab initio calculations and magnetic measurements to show that these two seemingly mutually exclusive interactions are entangled in the electron-doped SO-coupled Mott insulator Ba2Na1−xCaxOsO6(0 < x < 1), unveiling the formation ofspin-orbital bipolarons. Polaron charge trapping, favoured by the Jahn-Teller lattice activity, converts the Os 5d1spin-orbital Jeff = 3/2 levels, characteristic of the parent compound Ba2NaOsO6(BNOO), into a bipolaron 5d2Jeff = 2 manifold, leading to the coexistence of different J-effective states in a single-phase material. The gradual increase of bipolarons with increasing doping creates robust in-gap states that prevents the transition to a metal phase even at ultrahigh doping, thus preserving the Mott gap across the entire doping range from d1BNOO to d2Ba2CaOsO6(BCOO).more » « less
