Driving a two-dimensional Mott insulator with circularly polarized light breaks time-reversal and inversion symmetry, which induces an optically-tunable synthetic scalar spin chirality interaction in the effective low-energy spin Hamiltonian. Here, we show that this mechanism can stabilize topological magnon excitations in honeycomb ferromagnets and in optical lattices. We find that the irradiated quantum magnet is described by a Haldane model for magnons that hosts topologically-protected edge modes. We study the evolution of the magnon spectrum in the Floquet regime and via time propagation of the magnon Hamiltonian for a slowly varying pulse envelope. Compared to similar but conceptually distinct driving schemes based on the Aharanov-Casher effect, the dimensionless light-matter coupling parameter $λ= eEa/\hbarω$ at fixed electric field strength is enhanced by a factor $\sim 10^5$. This increase of the coupling parameter allows to induce a topological gap of the order of $Δ\approx 2$ meV with realistic laser pulses, bringing an experimental realization of light-induced topological magnon edge states within reach.
The bosonic analogues of topological insulators have been proposed in numerous theoretical works, but their experimental realization is still very rare, especially for spin systems. Recently, two-dimensional (2D) honeycomb van der Waals (vdW) ferromagnets have emerged as a new platform for topological spin excitations. Here, via a comprehensive inelastic neutron scattering study and theoretical analysis of the spin-wave excitations, we report the realization of topological magnon insulators in CrXTe$_3$ (X=Si, Ge) compounds. The nontrivial nature and intrinsic tunability of the gap opening at …
We theoretically propose a second-order topological magnon insulator by stacking the van der Waals honeycomb ferromagnets with antiferromagnetic interlayer coupling. The system exhibits Z$_{2}$ topological phase, protected by pseudo-time-reversal symmetry (PTRS). An easy-plane anisotropy term breaks PTRS and destroys the topological phase. Nevertheless, it respects a magnetic two-fold rotational symmetry which protects a second-order topological phase with corner modes in bilayer and hinge modes along stacking direction. Moreover, an introduced staggered interlayer coupling establishes a Z$_{2…
Two-dimensional (2D) van der Waals (vdW) magnets have been a fertile playground for the discovery and exploration of physical phenomena and new physics. In this Letter, we report the observation of an anomalous thermal Hall effect (THE) with \k{appa}_xy ~ 1x10^(-2) W K^(-1) m^(-1) in an insulating van der Waals ferromagnet VI3. The thermal Hall signal persists in the absence of an external magnetic field and flips sign upon the switching of the magnetization. In combination with theoretical calculations, we show that VI3 exhibits a dual nature of the THE, i.e., dominated by topological magnons…
Two dimensional van der Waals ferromagnets with honeycomb structures are expected to host the bosonic version of Dirac particles in their magnon excitation spectra. Using inelastic neutron scattering, we study spin wave excitations in polycrystalline CrCl$_3$, which exhibits ferromagnetic honeycomb layers with antiferromagnetic stackings along the $c$-axis. For comparison, polycrystal samples of CrI$_3$ with different grain sizes are also studied. We find that the powder-averaged spin wave spectrum of CrCl$_3$ at $T$ = 2 K can be adequately explained by the two dimensional spin Hamiltonian inc…
Thermal transport is a pivotal probe for studying low-energy, charge-neutral quasi-particles in insulating magnets. In this Letter, we report an observation of large magneto-thermal conductivity and thermal Hall effect (THE) in a van der Waals antiferromagnet FeCl2. The magneto-thermal conductivity reaches over ~700%, indicating strong magnon-phonon coupling. Furthermore, we find an appreciable thermal Hall signal which changes sign concurrently with the spin-flip transition from the antiferromagnetic state to the polarized ferromagnetic state. Our theoretical calculations suggest that, in add…
Optical pump-probe experiments carried out in the time domain reveal both the intrinsic low energy dynamics and its connections to higher energy excitations in correlated electron systems. In this work, we propose two microscopic mechanisms for the optical generation of coherent magnetic modes in van der Waals magnets, and derive the corresponding effective light-spin interactions: either through pumping atomic orbital excitations resonantly or via a light-induced Floquet spin Hamiltonian, the ground state of the system is driven out of equilibrium. The subsequent long-time relaxational dynami…
The quasi-two-dimensional antiferromagnet Ni$_2$P$_2$S$_6$ belongs to the family of magnetic van der Waals compounds that provides a rich material base for the realization of fundamental models of quantum magnetism in low dimensions. Here, we report high-frequency/high-magnetic field electron spin resonance measurements on single crystals of Ni$_2$P$_2$S$_6$. The results enable one to reliably determine the positive, "easy"-plane type of the single ion anisotropy of the Ni$^{2+}$ ions with the upper limit of its magnitude $\lesssim 0.7$ meV. The resonance response reveals strongly anisotropic …
Thermal and Magnetoelastic Properties of the van der Waals Ferromagnet Fe$_{3-δ}$GeTe$_2$: Anisotropic Spontaneous Magnetostriction and Ferromagnetic Magnon Excitations
Magnetic anisotropy in the near-stoichiometric van der Waals ferromagnet Fe$_3$GeTe$_2$
Leibniz Institute for Solid State and Materials Research（莱布尼茨固体与材料研究所）；Institute for Solid State and Materials Physics, TU Dresden（德累斯顿工业大学固体与材料物理研究所）；Department of Condensed Matter and Materials Physics, S. N. Bose National Centre for Basic Sciences（S.N. 玻色基础科学国家中心凝聚态与材料物理系）；School of Physical Sciences, Indian Association for the Cultivation of Science（印度科学促进协会物理科学学院）
We report on the temperature evolution of the polarization-dependent Raman spectrum of exfoliated MoI$_3$, a van der Waals material with a "true one-dimensional" crystal structure that can be exfoliated to individual atomic chains. The temperature evolution of several Raman features reveals anomalous behavior suggesting a phase transition of a magnetic origin. Theoretical considerations indicate that MoI$_3$ is an easy-plane antiferromagnet with alternating spins along the dimerized chains and with inter-chain helical spin ordering. The calculated frequencies of the phonons and magnons are con…
Despite serious effort, the nature of the magnetic interactions and the role of electron-correlation effects in magnetic two-dimensional (2D) van der Waals materials remain elusive. Using CrI$_3$ as a model system, we show that the calculated electronic structure including nonlocal electron correlations yields spin excitations consistent with inelastic neutron scattering measurements. Remarkably, this approach identifies an unreported correlation-enhanced interlayer super-superexchange, which rotates the magnon Dirac lines off, and introduces a gap along, the high-symmetry $Γ$-$K$-$M$ path. Th…
We demonstrate theoretically that the thermal Hall effect of magnons in collinear antiferromagnetic insulators is an indicator of magnetic and topological phase transitions in the magnon spectrum. The transversal heat current of magnons caused by a thermal gradient is calculated for an antiferromagnet on a honeycomb lattice. An applied magnetic field drives the system from the antiferromagnetic phase via a spin-flop phase into the field-polarized phase. Besides these magnetic phase transitions we find topological phase transitions within the spin-flop phase. Both types of transitions manifest …
In this work, we report the theoretical possibility of generating magnon polaron excitations through a space-varying magnetic field. The spatial dependence of the magnetic field in the Zeeman interaction gives rise to a magnon-phonon coupling when a magnetic field gradient is applied, and such a coupling depends directly on the strength of the gradient. It is also predicted that the direction of the magnetic field gradient allows control over which phonon polarization couples to the magnons in the material. Here we develop the calculations of the magnon-phonon coupling for an arbitrary (anti)f…
We report the observation of the $A_{\rm g}$-symmetric one-magnon Raman peak in the magnon Bose-Einstein condensation phase of TlCuCl$_{3}$. Its Raman shift traces the one-magnon energy at the magnetic $Γ$ point, and its intensity is proportional to the squared transverse magnetization. The appearance of the one-magnon Raman scattering originates from the exchange magnon Raman process and reflects the change of the magnetic-state symmetry. Using the bond-operator representation, we theoretically clarify the Raman selection rules, being consistent with the experimental results.
Spin and lattice are two fundamental degrees of freedom in a solid, and their fluctuations about the equilibrium values in a magnetic ordered crystalline lattice form quasiparticles termed magnons (spin waves) and phonons (lattice waves), respectively. In most materials with strong spin-lattice coupling (SLC), the interaction of spin and lattice induces energy gaps in the spin wave dispersion at the nominal intersections of magnon and phonon modes. Here we use neutron scattering to show that in the two-dimensional (2D) van der Waals honeycomb lattice ferromagnetic CrGeTe3, spin waves propagati…
Topological magnon insulators are a new class of magnetic materials that possess topologically nontrivial magnon bands. As a result, magnons in these materials display properties analogous to those of electrons in topological insulators. Here, we present magnetization, specific heat, and neutron scattering measurements of the ferromagnetic kagome magnet Cu(1,3-bdc). Our measurements provide a detailed description of the magnetic structure and interactions in this material, and confirm that it is an ideal prototype for topological magnon physics in a system with a simple spin Hamiltonian.
We compare the ground-state features of alternating ferrimagnetic chains $(1/2, S)$ with $S=1,3/2,2,5/2$ in a magnetic field and the corresponding Holstein-Primakoff bosonic models up to order $\sqrt{s/S}$, with $s=1/2$, considering the fully polarized magnetization as the boson vacuum. {The single-particle Hamiltonian is a Rice-Mele model with uniform hopping and modified boundaries, while the interactions have a correlated (density-dependent) hopping term and magnon-magnon repulsion.} The magnon-magnon repulsion increases the many-magnon energy and the density-dependent hopping decreases the…
In spite of flourishing studies on the topology of spin waves, a generic framework to classify and compute magnon band topology in non-collinear magnets is still missing. In this work we provide such a theory framework, by mapping an arbitrary linear spin wave into a local free-fermion Hamiltonian with exactly the same spectrum, symmetry implementation and band topology, which allows for a full classification and calculation on any topological properties of magnon bands. We apply this fermionization approach to honeycomb Kitaev magnet $α$-RuCl$_3$, and show the existence of topologically prote…
We report our density matrix renormalization-group and analytical work on S=1 antiferromagnetic Heisenberg spin chains. We study the finite size behavior within the framework of the non-linear sigma model. We study the effect of magnon-magnon interactions on the finite size spectrum and on the magnetization curve close to the critical magnetic field, determine the magnon scattering length and compare it to the prediction from the non-linear $σ$ model.
In three-dimensional (3D) quantum magnets, magnonic Weyl points (WPs) featuring linear band crossing of two non-degenerate magnon branches can emerge in certain lattice geometry when time-reversal symmetry is broken macroscopically. Unfortunately, there are very limited 3D quantum magnets that host magnonic WPs, and they are yet to be observed experimentally because the intrinsic perturbative interactions that break time-reversal symmetry macroscopically can be very negligible. Here, we present an alternative means via photo-irradiation, in which magnonic WPs can emerge in 3D quantum magnets w…
The magnetic properties of the interacting dimer system TlCuCl3 are investigated within a bond-operator formulation. The observed field-induced staggered magnetic order perpendicular to the field is described as a Bose condensation of magnons which are linear combinations of dimer singlet and triplet modes. This technique accounts for the magnetization curve and for the field dependence of the magnon dispersion curves observed by high-field neutron scattering measurements.
Magnonic excitations in the two-dimensional (2D) van der Waals (vdW) ferromagnet CrI3 are studied. We find that bulk magnons exhibit a non-trivial topological band structure without the need for Dzyaloshinskii-Moriya (DM) interaction. This is shown in vdW heterostructures, consisting of single-layer CrI3 on top of different 2D materials as MoTe2, HfS2 and WSe2. We find numerically that the proposed substrates modify substantially the out-of-plane magnetic anisotropy on each sublattice of the CrI3 subsystem. The induced staggered anisotropy, combined with a proper band inversion, leads to the o…
Motivated by the fact that many bilayer quantum magnets occur in nature, we generalize the study of thermal Hall transports of spin excitations to bilayer magnetic systems. It is shown that bilayer magnetic systems can be coupled either ferromagnetically or antiferromagnetically. We study both scenarios on the honeycomb lattice and show that the system realizes topologically nontrivial magnon bands induced by alternating next-nearest-neighbour Dzyaloshinsky-Moriya interaction (DMI). As a result, the bilayer system realizes both magnon Hall effect and magnon spin Nernst effect. We show that ant…
The magnon pumping effect in ferromagnetic insulators under an external time-dependent transverse magnetic field is theoretically studied. Generation of a magnon current is discussed by calculating the magnon source term in the spin continuity equation. This term represents the non-conservation of magnons arising from an applied transverse magnetic field. The magnon source term has a resonance structure as a function of the angular frequency of the transverse field, and this fact is useful to enhance the pumping effect.
Magnetization measurements were performed to investigate the critical behavior of the field-induced magnetic ordering in gapped spin system TlCuCl$_3$. The critical density of the magnons was obtained as a function of temperature and the magnon-magnon interaction constant was evaluated. The experimental phase boundary for $T < 5$ K agrees almost perfectly with the magnon BEC theory based on the Hartree-Fock approximation with realistic dispersion relations. The phase boundary can be described by the power law $[H_{N}(T)-H_{c}] propto T^{phi}$. With decreasing fitting temperature range, the cri…
We study theoretically the dynamics of magnons in the presence of a single skyrmion in chiral magnets featuring Dzyaloshinskii-Moriya interaction. We show by micromagnetic simulations that the scattering process of magnons by a skyrmion can be clearly defined although both originate in the common spins. We find that (i) the magnons are deflected by a skyrmion, with the angle strongly dependent on the magnon wavenumber due to the effective magnetic field of the topological texture, and (ii) the skyrmion motion is driven by magnon scattering through exchange of the momenta between the magnons an…
We propose that non-collinear magnetic order in quantum magnets can harbor a novel higher-order topological magnon phase with non-Hermitian topology and hinge magnon modes. We consider a three-dimensional system of interacting local moments on stacked-layers of honeycomb lattice. It initially favors a collinear magnetic order along an in-plane direction, which turns into a non-collinear order upon applying an external magnetic field perpendicular to the easy axis. We exploit the non-Hermitian nature of the magnon Hamiltonian to show that this field-induced transition corresponds to the transfo…
We theoretically study the interaction of magnons, quanta of spin waves, and a domain wall in a one-dimensional easy-axis antiferromagnet in the presence of an external magnetic field applied along the easy axis. To this end, we begin by obtaining the exact solution for spin waves in the background of a domain wall magnetized by an external field. The finite magnetization inside the domain wall is shown to give rise to reflection of magnons scattering off the domain wall, deviating from the well-known result of reflection-free magnons in the absence of a magnetic field. For practical applicati…
In experiments and applications usually the spin magnetic moment of magnons is considered. In this Paper we identify an additional degree of freedom of magnons: an \emph{orbital} magnetic moment brought about by spin-orbit coupling.Our microscopic theory uncovers that spin magnetization $\vec{M}^\mathrm{S}$ and orbital magnetization $\vec{M}^\mathrm{O}$ are independent quantities. They are not necessarily collinear; thus, even when the total spin moment is compensated due to antiferromagnetism ($\vec{M}^\mathrm{S} = \vec{0}$), $\vec{M}^\mathrm{O}$ may be nonzero. This scenario of orbital weak …
Achieving control over magnon spin currents in insulating magnets - where dissipation due to Joule heating is highly suppressed - is an active area of research that could lead to energy-efficient spintronics applications. However, magnon spin currents supported by conventional systems with uniform magnetic order have proven hard to control. An alternative approach that relies on topologically protected magnonic edge states of spatially periodic magnetic textures has recently emerged. A prime example of such textures is the ferromagnetic skyrmion crystal which hosts chiral edge states providing…
