Unconventional Excitations Research Articles

Chiral Dirac Fermion in a Collinear Antiferromagnet

In a Dirac semimetal, the massless Dirac fermion has zero chirality, leading to surface states connected adiabatically to a topologically trivial surface state as well as vanishing anomalous Hall effect. Recently, it is predicted that in the nonrelativistic limit of certain collinear antiferromagnets, there exists a type of chiral “Dirac-like” fermion, whose dispersion manifests four-fold degenerate crossing points formed by spin-degenerate linear bands, with topologically protected Fermi arcs. Such an unconventional chiral fermion, protected by a hidden SU(2) symmetry in the hierarchy of an enhanced crystallographic group, namely spin space group, is not experimentally verified yet. Here, by angle-resolved photoemission spectroscopy measurements, we reveal the surface origin of the electron pocket at the Fermi surface in collinear antiferromagnet CoNb3S6. Combining with neutron diffraction and first-principles calculations, we suggest a multidomain collinear antiferromagnetic configuration, rendering the the existence of the Fermi-arc surface states induced by chiral Dirac-like fermions. Our work provides spectral evidence of the chiral Dirac-like fermion caused by particular spin symmetry in CoNb3S6, paving an avenue for exploring new emergent phenomena in antiferromagnets with unconventional quasiparticle excitations.

Spin skyrmion gaps as signatures of strong-coupling insulators in magic-angle twisted bilayer graphene

The flat electronic bands in magic-angle twisted bilayer graphene (MATBG) host a variety of correlated insulating ground states, many of which are predicted to support charged excitations with topologically non-trivial spin and/or valley skyrmion textures. However, it has remained challenging to experimentally address their ground state order and excitations, both because some of the proposed states do not couple directly to experimental probes, and because they are highly sensitive to spatial inhomogeneities in real samples. Here, using a scanning single-electron transistor, we observe thermodynamic gaps at even integer moiré filling factors at low magnetic fields. We find evidence of a field-tuned crossover from charged spin skyrmions to bare particle-like excitations, suggesting that the underlying ground state belongs to the manifold of strong-coupling insulators. From the spatial dependence of these states and the chemical potential variation within the flat bands, we infer a link between the stability of the correlated ground states and local twist angle and strain. Our work advances the microscopic understanding of the correlated insulators in MATBG and their unconventional excitations.

Unconventional room-temperature carriers in the triangular-lattice Mott insulator TbInO3

The strong correlations between electrons in Mott insulator materials may produce highly entangled many-body states with unconventional emergent excitations. The signatures of such excitations, if any, are commonly believed to be observable only at low temperatures. Here, we challenge this common belief and show using terahertz time-domain spectroscopy that exotic carriers exist even at room temperature in TbInO3, a candidate material for realizing a low-temperature quantum spin-liquid phase. In particular, over the entire temperature range of 1.5–300 K, we observe a quadratic frequency dependence in the real part of the in-plane optical conductivity as well as Fano asymmetry of an optical phonon mode strongly interacting with the excitation continuum. These features are robust even under external magnetic fields of up to 7 T. Our data confirm the presence of emergent charge carriers within the Mott charge gap of TbInO3, suggesting that it is possible to probe and manipulate highly entangled quantum many-body states at room temperature.

Magnetic properties of S=12 distorted J1−J2 honeycomb lattice compound NaCuIn(PO4)2

The subtle interplay between low-dimensionality and spin correlations can lead to exotic ground states with unconventional excitations in two-dimensional honeycomb-lattice-based quantum magnets. Herein, we present the structural, magnetic, and heat capacity measurements; density functional theory $+$ Hubbard $U$ ($\mathrm{DFT}+U$) based electronic structure calculations; and quantum Monte Carlo simulations for $\mathrm{NaCuIn}{({\mathrm{PO}}_{4})}_{2}$. The structure of $\mathrm{NaCuIn}{({\mathrm{PO}}_{4})}_{2}$ consists of a well-separated, $\mathit{S}=\frac{1}{2}$ distorted ${\mathit{J}}_{1}\text{\ensuremath{-}}{\mathit{J}}_{2}$ honeycomb layer which is a combination of the magnetic couplings ${\mathit{J}}_{1}$ (forming spin dimers) and ${\mathit{J}}_{2}$ (constituting spin chains). At high temperatures, the magnetic susceptibility $\ensuremath{\chi}(T)$ follows paramagnetic behavior with a Curie-Weiss temperature ${\ensuremath{\theta}}_{\mathrm{CW}}\ensuremath{\approx}\ensuremath{-}16$ K, implying the presence of antiferromagnetic interactions. A broad maximum is observed at about $13\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ in $\ensuremath{\chi}(T)$, indicating the presence of short-range spin correlations. The quantum Monte Carlo simulations using the $\mathit{S}=\frac{1}{2}\phantom{\rule{4pt}{0ex}}{\mathit{J}}_{1}\text{\ensuremath{-}}{\mathit{J}}_{2}$ Heisenberg model on a distorted honeycomb lattice are in good agreement with the measured magnetic susceptibility data. The obtained ratio of the exchange couplings ($\frac{{\mathit{J}}_{2}}{{\mathit{J}}_{1}}$) is 2.63, which is consistent with the value obtained from our $\mathrm{DFT}+U$ calculations. The title material undergoes a magnetic long-range order at 0.4 K in the heat capacity, which is suppressed with an applied magnetic field of 10 kOe. The magnetic heat capacity data follow a linear temperature-dependent behavior well above the transition temperature, suggesting the presence of gapless excitations. The observed behavior can be attributed to the presence of low connectivity and weak magnetic frustration in this two-dimensional distorted honeycomb lattice.

Spin-polarized sextuple excitations in ferromagnetic materials

The most fundamental symmetry in condensed matter physics is the crystallographic symmetry, such that solids could exhibit unconventional excitations beyond Dirac and Weyl fermions. Among the unconventional fermions, the sextuple excitation has been predicted in many nonmagnetic materials. However, the study of magnetic sextuple excitations has fallen behind because of the complicated magnetic structures of materials. Here we perform a systematic search for ferromagnetic (FM) sextuple points (SPs) in the absence of spin-orbit coupling. Based on 230 space groups (SGs), we find there are 5 SGs that could host SPs at high-symmetry points. Regarding the stability of the sextuple excitation, we reveal that the minimum little point group at where the SP locates is ${\mathrm{T}}_{d}$. To support this result, we construct the effective model based on the $k\ifmmode\cdot\else\textperiodcentered\fi{}p$ method, from which the linear dispersion can be read off. Via first-principles calculations, we also identify 67 FM material candidates, which realize the SPs with completely/incompletely spin polarized. To support our theory, we pick one of the FM materials, ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$, as an example in which there is a fully spin-polarized SP. Finally, our work paves the way to study the spin-polarized SPs and provides a platform to realize the spintronic associated with sextuple excitations.

Coexistence of topological and nontopological Fermi-superfluid phases

The two-dimensional spin-imbalanced Fermi gas subject to s-wave pairing and spin-orbit coupling is considered a promising platform for realizing a topological chiral-p-wave superfluid. In the BCS limit of s-wave pairing, i.e., when Cooper pairs are only weakly bound, the system enters the topological phase via a second-order transition driven by increasing the Zeeman spin-splitting energy. Stronger attractive two-particle interactions cause the system to undergo the BCS-BEC crossover, in the course of which the topological transition becomes first-order. As a result, topological and nontopological superfluids coexist in spatially separated domains in an extended region of phase space spanned by the strength of s-wave interactions and the Zeeman energy. Here we investigate this phase-coexistence region theoretically using a zero-temperature mean-field approach. Exact numerical results are presented to illustrate basic physical characteristics of the coexisting phases and to validate an approximate analytical description derived for weak spin-orbit coupling. Besides extending our current understanding of spin-imbalanced superfluid Fermi systems, the present approach also provides a platform for future studies of unconventional Majorana excitations that, according to topology, should be present at the internal interface between coexisting topological and nontopological superfluid parts of the system.

Eightfold fermionic excitation in a charge density wave compound

Unconventional quasiparticle excitations in condensed matter systems have become one of the most important research frontiers. Beyond two- and fourfold degenerate Weyl and Dirac fermions, three-, six- and eightfold symmetry protected degeneracies have been predicted however remain challenging to realize in solid state materials. Here, charge density wave compound TaTe4 is proposed to hold eightfold fermionic excitation and Dirac point in energy bands. High quality TaTe4 single crystals are prepared, where the charge density wave is revealed by directly imaging the atomic structure and a pseudogap of about 45 meV on the surface. Shubnikov de-Haas oscillations of TaTe4 are consistent with band structure calculation. Scanning tunneling microscopy reveals atomic step edge states on the surface of TaTe4. This work uncovers that charge density wave is able to induce new topological phases and sheds new light on the novel excitations in condensed matter materials.

Optical and magnetic excitations in the underscreened quasiquartet Kondo lattice

The underscreened Kondo lattice consisting of a single twofold degenerate conduction band and a CEF split 4f-electron quasi-quartet has non-conventional quasiparticle dispersions obtained from the constrained mean-field theory. An additional genuinely heavy band is found in the main hybridization band gap of the upper and lower hybridzed bands whose heavy effective mass is controlled by the CEF splitting. Its presence should profoundly influence the dynamical optical and magnetic response functions. In the former, the onset of the optical conductivity is not the main hybridisation energy but the much lower Kondo energy scale which appears in the direct transitions to the additional heavy band. The dynamical magnetic response is also strongly modified by the in-gap heavy band which can lead to unconventional resonant excitations that may be interpreted as coherent CEF-Kondo lattice magnetic exciton bands. Their instability at low temperature signifies the onset of induced excitonic magnetism in the underscreened Kondo lattice.

Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids?

Quantum spin liquids are prime examples of strongly entangled phases of matter with unconventional exotic excitations. Here, strong quantum fluctuations prohibit the freezing of the spin system. On the other hand, frustrated magnets, the proper platforms to search for the quantum spin liquid candidates, still show a magnetic ground state in most of the cases. Pressure is an effective tuning parameter of structural properties and electronic correlations. Nevertheless, the ability to influence the magnetic phases should not be forgotten. We review experimental progress in the field of pressure-tuned magnetic interactions in candidate systems. Elaborating on the possibility of tuned quantum phase transitions, we further show that chemical or external pressure is a suitable parameter in these exotic states of matter.

Quantum-critical phase from frustrated magnetism in a strongly correlated metal

Strange-metal phenomena often develop at the border of antiferromagnetic order in strongly correlated metals. It has been well established that they can originate from the fluctuations anchored by the point of continuous quantum phase transition out of the antiferromagnetic order, i.e., a quantum critical point. What has been unclear is how these phenomena can be associated with a potential new phase of matter at zero temperature. Here we show that magnetic frustration of the 4f-local moments in the distorted Kagome intermetallic compound CePdAl gives rise to such a paramagnetic quantum-critical phase. Moreover, we demonstrate that this phase turns into a Fermi liquid through a Mott-like crossover; in a two-dimensional parameter space of pressure and magnetic field, this crossover is linked to a line of zero-temperature 4f-electron localization-delocalization phase transitions at low and moderate pressures. Our discovery motivates a new design principle for strongly correlated metallic states with unconventional excitations that may underlie the development of such effects as high temperature superconductivity.

Hybridization and Decay of Magnetic Excitations in Two-Dimensional Triangular Lattice Antiferromagnets

Elementary quasiparticles in solids such as phonons and magnons occasionally have nontrivial interactions between them, as well as among themselves. As a result, their energy eigenvalues are renormalized, the quasiparticles spontaneously decay into a multi-particle continuum state, or they are hybridized with each other when their energies are close. As discussed in this review, such anomalous features can appear dominantly in quantum magnets but are not, a priori, negligible for magnetic systems with larger spin values and noncollinear magnetic structures. We review the unconventional magnetic excitations in two-dimensional triangular lattice antiferromagnets and discuss their implications on related issues.

Robust Twin Pairs of Weyl Fermions in Ferromagnetic Oxides.

The ferromagnetic Weyl semimetals with inversion symmetry usually possess odd pairs of Weyl fermions. Here, we present an inversion eigenvalue argument to dictate the existence of even pairs of ferromagnetic Weyl fermions. We show, by a combination of first-principles calculations and symmetry analyses, that this exotic topological feature can be verified in ferromagnetic oxides in different space groups. In particular, a realistic candidate, i.e., hollandite RbCr_{4}O_{8} with a high Curie temperature (∼295 K), hosts intriguing twin pairs of Weyl fermions, which are robustly stable against perturbations. Moreover, our effective model and symmetry analysis show that the twin pairs of Weyl fermions originate from a mirrored nodal ring pair. The nontrivial surface states and Fermi arcs of RbCr_{4}O_{8} are clearly visible, further revealing the topological features. This work strengthens the understanding of the parity analysis in exploring ferromagnetic topological materials with unconventional fermionic excitations.

Multipolar edge states in the anisotropic kagome antiferromagnet

Excitations of ordered insulating magnets gain renewed interest due to their potential topological properties and the natural realization of magnetic analogues of the celebrated topological models. In this paper we go beyond these parallels and explore what else is there in the unconventional excitations of quantum magnets. We study the topologically nontrivial multiplet excitations of the antiferromagnetic spin-1/2 kagome system with strong breathing anisotropy and Dzyaloshinskii-Moriya interaction. We show that in the chiral magnetic ground state the excitations can be characterized by a spin-1/2 doublet and a spin-3/2 quartet. With the use of magnetic field we can tune the quartet through a band touching topological phase transition, when a novel spin-3/2 Dirac cone is formed by the touching of four bands. In the topologically nontrivial regime the spin-3/2 bands have large Chern numbers -3, -1, 1, 3. In an open system the emerging chiral edge states naturally inherit the multipolar characters and we find novel quadrupolar edge modes.

Nonsymmorphic cubic Dirac point and crossed nodal rings across the ferroelectric phase transition in LiOsO3

Crystalline symmetries can generate exotic band-crossing features, which can lead to unconventional fermionic excitations with interesting physical properties. We show how a cubic Dirac point---a four-fold-degenerate band-crossing point with cubic dispersion in a plane and a linear dispersion in the third direction---can be stabilized through the presence of a nonsymmorphic glide mirror symmetry in the space group of the crystal. Notably, the cubic Dirac point in our case appears on a threefold axis, even though it has been believed previously that such a point can only appear on a sixfold axis. We show that a cubic Dirac point involving a threefold axis can be realized close to the Fermi level in the non-ferroelectric phase of LiOsO$_3$. Upon lowering temperature, LiOsO$_3$ has been shown experimentally to undergo a structural phase transition from the non-ferroelectric phase to the ferroelectric phase with spontaneously broken inversion symmetry. Remarkably, we find that the broken symmetry transforms the cubic Dirac point into three mutually-crossed nodal rings. There also exist several linear Dirac points in the low-energy band structure of LiOsO$_3$, each of which is transformed into a single nodal ring across the phase transition.

Fracton Topological Phases from Strongly Coupled Spin Chains

We provide a new perspective on fracton topological phases, a class of three-dimensional topologically ordered phases with unconventional fractionalized excitations that are either completely immobile or only mobile along particular lines or planes. We demonstrate that a wide range of these fracton phases can be constructed by strongly coupling mutually intersecting spin chains and explain via a concrete example how such a coupled-spin-chain construction illuminates the generic properties of a fracton phase. In particular, we describe a systematic translation from each coupled-spin-chain construction into a parton construction where the partons correspond to the excitations that are mobile along lines. Remarkably, our construction of fracton phases is inherently based on spin models involving only two-spin interactions and thus brings us closer to their experimental realization.

Anomalous metallic behaviour in the doped spin liquid candidate \u03ba-(ET)4Hg2.89Br8

Quantum spin liquids are exotic Mott insulators that carry extraordinary spin excitations. Therefore, when doped, they are expected to afford metallic states with unconventional magnetic excitations. Here, we report experimental results which are suggestive of a doped spin liquid with anomalous metallicity in a triangular-lattice organic conductor. The spin susceptibility is nearly perfectly scaled to that of a non-doped spin liquid insulator in spite of the metallic state. Furthermore, the charge transport that is confined in the layer at high temperatures becomes sharply deconfined on cooling, coinciding with the rapid growth of spin correlations or coherence as signified by a steep decrease in spin susceptibility. The present results substantiate the desired doped spin liquid and suggest a strange metal, in which the coherence of the underlying spin liquid promotes the deconfinement of charge from the layers while preserving the non-Fermi-liquid nature.

Back to the Structural and Dynamical Properties of Neutral-Ionic Phase Transitions

Although the Neutral-Ionic transition in mixed stack charge-transfer crystals was discovered almost forty years ago, many features of this intriguing phase transition, as well as open questions, remain at the heart of today’s science. First of all, there is the most spectacular manifestation of electronic ferroelectricity, in connection with a high degree of covalency between alternating donor and acceptor molecules along stacks. In addition, a charge-transfer instability from a quasi-neutral to a quasi-ionic state takes place concomitantly with the stack dimerization, which breaks the inversion symmetry. Moreover, these systems exhibit exceptional one-dimensional fluctuations, with an enhancement of the effects of electron-lattice interaction. This may lead to original physical pictures for the dynamics of pre-transitional phenomena, as the possibility of a pronounced Peierls-type instability and/or the generation of unconventional non-linear excitations along stacks. Last but not least, these mixed stack charge-transfer systems constitute a valuable test bed to explore some of the key questions of ultrafast photo-induced phenomena, such as multiscale dynamics, selective coherent excitations and non-linear responsiveness. These different aspects will be discussed through the structural and dynamical features of the neutral-ionic transition, considering old and recent results, open questions and future opportunities. In particular, we revisit the structural changes and symmetry considerations, the pressure-temperature phase diagrams and conclude by their interplay with the photo-induced dynamics.

Putative spin liquid in the triangle-based iridate Ba3IrTi2O9

We report on thermodynamic, magnetization, and muon spin relaxation measurements of the strong spin-orbit coupled iridate Ba$_3$IrTi$_2$O$_9$, which constitutes a new frustration motif made up a mixture of edge- and corner-sharing triangles. In spite of strong antiferromagnetic exchange interaction of the order of 100~K, we find no hint for long-range magnetic order down to 23 mK. The magnetic specific heat data unveil the $T$-linear and -squared dependences at low temperatures below 1~K. At the respective temperatures, the zero-field muon spin relaxation features a persistent spin dynamics, indicative of unconventional low-energy excitations. A comparison to the $4d$ isostructural compound Ba$_3$RuTi$_2$O$_9$ suggests that a concerted interplay of compass-like magnetic interactions and frustrated geometry promotes a dynamically fluctuating state in a triangle-based iridate.

Anomalous Thermal Conductivity and Magnetic Torque Response in the Honeycomb Magnet α-RuCl_{3}.

We report on the unusual behavior of the in-plane thermal conductivity κ and torque τ response in the Kitaev-Heisenberg material α-RuCl_{3}. κ shows a striking enhancement with linear growth beyond H=7 T, where magnetic order disappears, while τ for both of the in-plane symmetry directions shows an anomaly at the same field. The temperature and field dependence of κ are far more complex than conventional phonon and magnon contributions, and require us to invoke the presence of unconventional spin excitations whose properties are characteristic of a field-induced spin-liquid phase related to the enigmatic physics of the Kitaev model in an applied magnetic field.

Weyl magnons in breathing pyrochlore antiferromagnets.

Frustrated quantum magnets not only provide exotic ground states and unusual magnetic structures, but also support unconventional excitations in many cases. Using a physically relevant spin model for a breathing pyrochlore lattice, we discuss the presence of topological linear band crossings of magnons in antiferromagnets. These are the analogues of Weyl fermions in electronic systems, which we dub Weyl magnons. The bulk Weyl magnon implies the presence of chiral magnon surface states forming arcs at finite energy. We argue that such antiferromagnets present a unique example, in which Weyl points can be manipulated in situ in the laboratory by applied fields. We discuss their appearance specifically in the breathing pyrochlore lattice, and give some general discussion of conditions to find Weyl magnons, and how they may be probed experimentally. Our work may inspire a re-examination of the magnetic excitations in many magnetically ordered systems.