The search for new elementary particles is one of the most basic pursuits in physics, spanning from subatomic physics to quantum materials. Magnons are the ubiquitous elementary quasiparticle to describe the excitations of fully-ordered magnetic syst
ems. But other possibilities exist, including fractional and multipolar excitations. Here, we demonstrate that strong quantum interactions exist between three flavors of elementary quasiparticles in the uniaxial spin-one magnet FeI2. Using neutron scattering in an applied magnetic field, we observe spontaneous decay between conventional and heavy magnons and the recombination of these quasiparticles into a super-heavy bound-state. Akin to other contemporary problems in quantum materials, the microscopic origin for new physics in FeI2 is the quasi-flat nature of excitation bands and the presence of Kitaev anisotropic magnetic exchange interactions.
Spin-waves e.g. magnons are the conventional elementary excitations of ordered magnets. However, other possibilities exist. For instance, magnon bound-states can arise due to attractive magnon-magnon interactions and drastically impact the static and
dynamic properties of materials. Here, we demonstrate a zoo of distinct multi-magnon quasiparticles in the frustrated spin-1 triangular antiferromagnet FeI$_2$ using time-domain terahertz spectroscopy. The energy-magnetic field excitation spectrum contains signatures of one-, two-, four- and six-magnon bound-states, which we analyze using an exact diagonalization approach for a dilute gas of interacting magnons. The two-magnon single-ion bound states occur due to strong anisotropy and the preponderance of even higher order excitations arises from the tendency of the single-ion bound states to themselves form bound states due to their very flat dispersion. This menagerie of tunable interacting quasiparticles provides a unique platform in a condensed matter setting that is reminiscent of the few-body quantum phenomena central to cold-atom, nuclear, and particle physics experiments.
We report a comprehensive inelastic neutron scattering study of the hybrid molecule-based multiferroic compound (ND4)2FeCl5D2O in the zero-field incommensurate cycloidal phase and the high-field quasi-collinear phase. The spontaneous electric polariz
ation changes its direction concurrently with the field-induced magnetic transition, from mostly aligned with the crystallographic a-axis to the c-axis. To account for such change of polarization direction, the underlying multiferroic mechanism was proposed to switch from the spin-current model induced via the inverse Dzyalloshinskii-Moriya interaction to the p-d hybridization model. We perform a detailed analysis of the inelastic neutron data of (ND4)2FeCl5D2O using linear spin-wave theory to quantify magnetic interaction strengths and investigate possible impact of different multiferroic mechanisms on the magnetic couplings. Our result reveals that the spin dynamics of both multiferroic phases can be well-described by a Heisenberg Hamiltonian with an easy-plane anisotropy. We do not find notable differences between the optimal model parameters of the two phases. The hierarchy of exchange couplings and the balance among frustrated interactions remain the same between two phases, suggesting that magnetic interactions in (ND4)2FeCl5D2O are much more robust than the electric polarization in response to delicate reorganizations of the electronic degrees of freedom in an applied magnetic field.
An indispensable step to understand collective magnetic phenomena in rare-earth compounds is the determination of spatially-anisotropic single-ion properties resulting from spin-orbit coupling and crystal field (CF). The CF Hamiltonian has a discrete
energy spectrum -- accessible to spectroscopic probes such as neutron scattering -- controlled by a number of independent parameters reflecting the point-symmetry of the magnetic sites. Determining these parameters in low-symmetry systems is often challenging. Here, we describe a general method to analyze CF excitation spectra using adjustable effective point-charges. We benchmark our method to existing neutron-scattering measurements on pyrochlore rare-earth oxides and obtain a universal point-charge model that describes a large family of related materials. We adapt this model to the newly discovered tripod Kagome magnets ($R_{3}$Mg$_2$Sb$_{3}$O$_{14}$, $R$ = Tb, Ho, Er, Yb) for which we report broadband inelastic neutron-scattering spectra. Analysis of these data using adjustable point-charges yields the CF wave-functions for each compound. From this, we calculate thermomagnetic properties that accurately reflect our measurements on powder samples, and predict the effective gyromagnetic tensor for pseudo-spin degrees of freedom -- a crucial step to understand the exotic collective properties of these kagome magnets at low temperature. We present further applications of our method to other tripod kagome materials and triangular rare-earth compounds $R$MgGaO$_4$ ($R$ =Yb, Tm). Overall, this study establishes a widely applicable methodology to predict CF and single-ion properties of rare-earth compounds based on interpretable and adjustable models of effective point-charges.
A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-bod
y model of quantum tunneling. Here, we show that the tripod kagome lattice material Ho${_3}$Mg${_2}$Sb${_3}$O${_{14}}$ unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho$^{3+}$ ground-state doublet, which is further coupled to a nuclear spin bath. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at $T^{ast}approx0.32$ K to a remarkable state with three peculiarities: a concurrent recovery of magnetic entropy associated with the strongly coupled electronic and nuclear degrees of freedom; a fragmentation of the spin into periodic and ice-like components; and persistent inelastic magnetic excitations down to $Tapprox0.12$ K. These observations deviate from expectations of classical spin fragmentation on a kagome lattice, but can be understood within a model of dipolar kagome ice under a homogeneous transverse magnetic field, which we survey with exact diagonalization on small clusters and mean-field calculations. In Ho${_3}$Mg${_2}$Sb${_3}$O${_{14}}$, hyperfine interactions dramatically alter the single-ion and collective properties, and suppress possible quantum correlations, rendering the fragmentation with predominantly single-ion quantum fluctuations. Our results highlight the crucial role played by hyperfine interactions in frustrated quantum magnets, and motivate further investigations of the role of quantum fluctuations on partially-ordered magnetic states.
Materials containing non-Kramers magnetic ions can show unusual quantum excitations because of the exact mapping of the two-singlet crystal-field ground state to a quantum model of Ising spins in a transverse magnetic field. Here, we model the magnet
ic excitation spectrum of garnet-structured Ho3Ga5O12, which has a two-singlet crystal-field ground state. We use a reaction-field approximation to explain published inelastic neutron-scattering data [Zhou et al., Phys. Rev. B 78, 140406(R) (2008)] using a three-parameter model containing the magnetic dipolar interaction, the two-singlet crystal-field splitting, and the nuclear hyperfine coupling. Our study clarifies the magnetic Hamiltonian of Ho3Ga5O12, reveals that the nuclear hyperfine interaction drives magnetic ordering in this system, and provides a framework for quantitative analysis of magnetic excitation spectra of materials with singlet crystal-field ground states.
A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-bod
y model of quantum tunneling. Here, we show that the tripod kagome lattice material Ho3Mg2Sb3O14 unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho3+ ground-state doublet, realizing a frustrated transverse Ising model. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at T*~0.32 K to a remarkable quantum state with three peculiarities: a continuous magnetic excitation spectrum down to T~0.12K; a macroscopic degeneracy of ice-like states; and a fragmentation of the spin into periodic and aperiodic components strongly affected by quantum fluctuations. Our results establish that Ho3Mg2Sb3O14 realizes a spin-fragmented state on the kagome lattice, with intrinsic quantum dynamics generated by a homogeneous transverse field.
