Spin-nematic Phase Research Articles

Magnetoelastic study on the frustrated quasi-one-dimensional spin- 12 magnet LiCuVO4

We investigated the magnetoelastic properties of the quasi-one-dimensional spin-1/2 frustrated magnet LiCuVO$_4$. Longitudinal-magnetostriction experiments were performed at 1.5 K in high magnetic fields of up to 60 T applied along the $b$ axis, i.e., the spin-chain direction. The magnetostriction data qualitatively resemble the magnetization results, and saturate at $H_{\text{sat}} \approx 54$ T, with a relative change in sample length of $\Delta L/L \approx 1.8\times10^{-4}$. Remarkably, both the magnetostriction and the magnetization evolve gradually between $H_{\text{c3}} \approx 48$ T and $H_{\text{sat}}$, indicating that the two quantities consistently detect the spin-nematic phase just below the saturation. Numerical analyses for a weakly coupled spin-chain model reveal that the observed magnetostriction can overall be understood within an exchange-striction mechanism. Small deviations found may indicate nontrivial changes in local correlations associated with the field-induced phase transitions.

Quantum spin nematic liquid in the S = 1 antiferromagnetic chain with the biquadratic interaction

The magnetization process of the S = 1 antiferromagnetic chain with the biquadratic interaction is investigated using the numerical diagonalization. As a result, it is found that the quantum spin nematic liquid phase appears below the saturation magnetization for sufficiently large negative biquadratic interaction. The ground state phase diagram is also presented. This result is consistent with the previous density matrix renormalization group study. In addition the present study confirms that the two magnon excitation is gapless, while the single magnon one is gapped in the spin nematic liquid phase.

Ultrafast spin-nematic and ferroelectric phase transitions induced by femtosecond light pulses

Optically induced phase transitions of the manganite ${\mathrm{Pr}}_{1/3}{\mathrm{Ca}}_{2/3}\mathrm{Mn}{\mathrm{O}}_{3}$ have been simulated by using a model Hamiltonian that captures the dynamics of strongly correlated charge, orbital, lattice, and spin degrees of freedom. Its parameters have been extracted from first-principles calculations. Beyond a critical intensity of a femtosecond light pulse, the material undergoes an ultrafast and nonthermal magnetic phase transition from a noncollinear to collinear antiferromagnetic phase. The light-pulse excites selectively either a spin-nematic or a ferroelectric phase, depending on the light polarization. The behavior can be traced to an optically induced ferromagnetic coupling between Mn trimers, i.e., polarons which are delocalized over three Mn sites. The polarization guides the polymerization of the polaronic crystal into distinct patterns of ferromagnetic chains determining the target phase.

Finite-temperature thermodynamic properties of spin-1 nematics in an applied magnetic field

We study numerically the thermodynamic properties of the spin nematic phases in a magnetic field in the spin-1 bilinear-biquadratic model. When the field is applied, the phase transition temperature once goes up and then decreases rapidly toward zero, which is detected by the peak-shift in the specific heat. The underlying mechanism of the reentrant behavior is the entropic effect. In a weak field the high temperature paramagnetic phase rapidly loses its entropy while the ferroquadrupolar nematic phase remains robust by modifying the shape of the ferroquadrupolar moment. This feature serves as a fingerprint of generic ferroquadrupolar phases, while it is not observed for the case of antiferroquadrupoles.

Thermal effects versus spin nematicity in a frustrated spin- 12 chain

The spin-nematic phase is an intriguing state of matter that lacks usual long-range dipolar order, yet it exhibits higher multipolar order. This makes its detection extremely difficult and controversial. Recently, nuclear magnetic resonance (NMR) has been proposed as one of the most suitable techniques to confirm its existence. We report a $^{17}$O NMR observation of the reduction of the local magnetization in the polarized state of the frustrated spin-1/2 chain $\beta$-TeVO$_4$, which was previously proposed to be a fingerprint of the spin-nematic behavior. However, our detailed study shows that the detected missing fraction of the magnetization, probed by NMR frequency shift, is thermally activated, thus undermining the presence of the spin-nematic phase in the investigated compound. This highlights the importance of careful considerations of temperature-dependent NMR shift that has been overlooked in previous studies of spin nematicity.

Two-photon driven magnon-pair resonance as a signature of spin-nematic order

We theoretically study the nonlinear magnetic resonance driven by intense laser or electromagnetic wave in a fully polarized frustrated magnet near a less-visible spin-nematic ordered phase. In general, both magnons and magnon pairs (two-magnon bound state) appear as the low-energy excitation in the saturated state of spin-nematic magnets. Their excitation energies are usually in terahertz (THz) or gigahertz range. Magnon pairs with angular momentum 2$\hbar$ can be excited by the simultaneous absorption of two photons, and such multi-photon processes occur if the applied THz laser is strong enough. We compute laser-driven magnetic dynamics of a frustrated four-spin system with both magnon ($\hbar$) and magnon-pair (2$\hbar$) like excitations which is analogous to a macroscopic frustrated magnet with a spin nematic phase. We estimate the required strength of magnetic field of laser for the realization of two photon absorption, taking into account dissipation effects with the Lindblad equation. We show that intense THz laser with ac magnetic field of 0.1-1.0 Tesla is enough to observe magnon-pair resonance.

Spin-lattice Coupling and the Emergence of the Trimerized Phase in the S=1 Kagome Antiferromagnet Na2Ti3Cl8

Spin-1 antiferromagnets are abundant in nature, but few theories exist to understand their properties and behavior when geometric frustration is present. Here we study the S=1 kagome compound Na_{2}Ti_{3}Cl_{8} using a combination of density functional theory, exact diagonalization, and density matrix renormalization group approaches to achieve a first principles supported explanation of its exotic magnetic phases. We find that the effective magnetic Hamiltonian includes essential non-Heisenberg terms that do not stem from spin-orbit coupling, and both trimerized and spin-nematic magnetic phases are relevant. The experimentally observed structural transition to a breathing kagome phase is driven by spin-lattice coupling, which favors the trimerized magnetic phase against the quadrupolar one. We thus show that lattice effects can be necessary to understand the magnetism in frustrated magnetic compounds and surmise that Na_{2}Ti_{3}Cl_{8} is a compound that cannot be understood from only electronic or only lattice Hamiltonians, very much like VO_{2}.

Multiple quadrupolar or nematic phases driven by the Heisenberg interactions in a spin-1 dimer system forming a bilayer

We explore several classes of quadrupolar ordering in a system of antiferromagnetically coupled quantum spin-1 dimers, which are stacked in the triangular lattice geometry forming a bilayer. Low-energy properties of this model is described by an $\mathcal{S}=1$ hard-core bosonic degrees of freedom defined on each dimer-bond, where the singlet and triplet states of the dimerized spins are interpreted as the vacuum and the occupancy of boson, respectively. The number of bosons per dimer and the magnetic and density fluctuations of bosons are controlled by the inter-dimer Heisenberg interactions. In a solid phase where each dimer hosts one boson and the inter-dimer interaction is weak, a conventional spin nematic phase is realized by the pair-fluctuation of bosons. Larger inter-dimer interaction favors Bose Einstein condensates (BEC) carrying quadrupolar moments. Among them, we find one exotic phase where the quadrupoles develop a spatially modulated structure on the top of a uniform BEC, interpreted in the original dimerized spin-1 model as coexistent $p$-type nematic and 120$^\circ$-magnetic correlations. This may explain an intriguing nonmagnetic phase found in Ba$_{3}$ZnRu$_{2}$O$_{9}$.

Spin-nematic order induced superconductivity

We explore a spin-fermion model with fermion-spin-quadrupolar interaction. In a nematic phase, this interaction reduces to a four-fermion interaction that is the basis of superconductivity. When the coupling constant is positive the superconductivity is a p-wave with spin-parallel–paired fermions. When it is negative the superconductivity is a p-wave and fermions are spin-antiparallel paired. For a system with zero chemical potential, even a very small coupling can bind fermions into a bound state that leads to superconductivity. When the chemical potential is non-zero the system possesses quantum critical transition from the normal spin-nematic phase to the phase where superconductivity coexists with spin-nematicity. The value of the quantum critical fermion-spin-nematicity coupling constant depends on the chemical potential.

Spin nematics in frustrated spin-dimer systems with bilayer structure

We study frustrated spin-1/2 dimer systems in two dimensions with a bilayer structure, where spins are ferromagnetically coupled in dimers. Our model includes frustrated two-spin exchange interactions as well as four-spin interaction. We pay particular attention to the spin nematic phase, which does not exhibit any magnetic (spin-dipole) order but has a spin-quadrupolar long-range order. Employing a perturbation calculation, a mean-field approximation, and a numerical many-variable variational Monte Carlo method, we determine ground-state phase diagrams on various two-dimensional lattices. It is found that the model exhibits the spin nematic phase with ferro-quadrupolar order in a wide parameter region, in addition to conventional magnetically-ordered phases. In particular, it is shown that even when the four-spin interactions are absent, frustrated two-spin exchange interactions can realize the spin nematic phase as a result of strong interdimer correlations. It is also found that the phase transitions between the spin nematic phase and antiferromagnetic phases can be continuous. Furthermore, we present some exact arguments that various phases including the spin nematic phase and the vector chiral (p-type nematic) phase emerge from an SU(4) symmetric point in the model by the addition of appropriate perturbative interactions. The spin nematic phase generated from the SU(4) point is connected with the spin nematic phase found numerically in the system with only two-spin interactions.

Identification of emergent constraints and hidden order in frustrated magnets using tensorial kernel methods of machine learning

Machine-learning techniques have proved successful in identifying ordered phases of matter. However, it remains an open question how far they can contribute to the understanding of phases without broken symmetry, such as spin liquids. Here we demonstrate how a machine learning approach can automatically learn the intricate phase diagram of a classical frustrated spin model. The method we employ is a support vector machine equipped with a tensorial kernel and a spectral graph analysis which admits its applicability in an effectively unsupervised context. Thanks to the interpretability of the machine we are able to infer, in closed form, both order parameter tensors of phases with broken symmetry, and the local constraints which signal an emergent gauge structure, and so characterize classical spin liquids. The method is applied to the classical XXZ model on the pyrochlore lattice where it distinguishes---among others---between a hidden biaxial spin nematic phase and several different classical spin liquids. The results are in full agreement with a previous analysis by Taillefumier \emph{et al.} [Phys. Rev. X 7, 041057 (2017)], but go further by providing a systematic hierarchy between disordered regimes, and establishing the physical relevance of the susceptibilities associated with the local constraints. Our work paves the way for the search of new orders and spin liquids in generic frustrated magnets.

Magnetocaloric effect and spin-strain coupling in the spin-nematic state of LiCuVO4

The study explores the spin-quadrupole-strain coupling and the magnetic Grquotuneisen parameter in the spin-nematic phase of LiCuVO${}_{4}$ by the ultrasound and magnetocaloric experiments in high magnetic fields. The paper shows a strong involvement of a crystal lattice observed as anomalies in the acoustic properties and a divergence of the Grquotuneisen parameter at the transition to the spin-nematic state.

Magnetic ground state of the frustrated spin- 12 chain compound β–TeVO4 at high magnetic fields

Frustrated spin-1/2 chains, despite the apparent simplicity, exhibit remarkably rich phase diagram comprising vector-chiral (VC), spin-density-wave (SDW) and multipolar/spin-nematic phases as a function of the magnetic field. Here we report a study of $\beta$-TeVO$_4$, an archetype of such compounds, based on magnetization and neutron diffraction measurements up to 25 T. We find the transition from the helical VC ground state to the SDW state at $\sim$3 T for the magnetic field along the $a$ and $c$ crystal axes, and at $\sim$9 T for the field along the $b$ axis. The high-field (HF) state, existing above $\sim$18 T, i.e., above $\sim$1/2 of the saturated magnetization, is an incommensurate magnetically ordered state and not the spin-nematic state, as theoretically predicted for the isotropic frustrated spin-1/2 chain. The HF state is likely driven by sizable interchain interactions and symmetric intrachain anisotropies uncovered in previous studies. Consequently, the potential existence of the spin nematic phase in $\beta$-TeVO$_4$ is limited to a narrow field range, i.e., a few tenths of a tesla bellow the saturation of the magnetization, as also found in other frustrated spin-1/2 chain compounds.

Possible observation of quantum spin-nematic phase in a frustrated magnet

Water freezes into ice in winter and evaporates into vapor in summer. Scientifically, the transformations between solid, liquid, and gas are called phase transitions and can be classified through the changes in symmetry which occur in each case. A fourth phase of matter was discovered late in the 19th century: the liquid crystal nematic, in which rod- or disk-shaped molecules align like the atoms in a solid, while continuing to flow like a liquid. Here we report thermodynamic evidence of a quantum analog of the classical nematic phase, the quantum spin nematic (SN). In an SN, the spins of a quantum magnet select a common axis, like a nematic liquid crystal, while escaping conventional magnetic order. Our state-of-the-art thermal measurements in high pulsed magnetic fields up to 33 T on the copper mineral volborthite with spin 1/2 on a frustrated lattice provide thermodynamic evidence for SN order, half a century after the theoretical proposal [Blume M, Hsieh YY (1969) J Appl Phys 40:1249; Andreev AF, Grishchuk IA (1984) J Exp Theor Phys 97:467-475].

Dynamical structure factors in the nematic phase of frustrated ferromagnetic spin chains

Frustrated spin systems can show phases with spontaneous breaking of spin-rotational symmetry without the formation of local magnetic order. We study the dynamic response of the spin-nematic phase of one-dimensional spin-1/2 systems, characterized by slow large-distance decay of quadrupolar correlations, by numerically computing one-spin and two-spin dynamical structure factors at zero temperature using time-dependent density matrix renormalization group methods. We interpret the results in terms of an effective theory of gapped magnon excitations interacting with a quasi-condensate of bound magnon pairs. This employs an extension of the well-known Tomonaga-Luttinger liquid theory which includes the magnon states as a mobile impurity. A good qualitative understanding of the characteristic thresholds and their intensity in the structure factors is obtained this way. Our results are useful in the interpretation of inelastic neutron scattering and resonant inelastic x-ray scattering experiments.

Electron spin resonance for the detection of long-range spin nematic order

In this paper we propose that electron spin resonance (ESR) measurements enable us to detect the long-range spin nematic order. We show that the frequency of the paramagnetic resonance peak in the ESR spectrum is shifted by the ferroquadrupolar order parameter together with other quantities. The ferroquadrupolar order parameter is extractable from the angular dependence of the frequency shift. In contrast, the antiferroquadrupolar order parameter is usually invisible in the frequency shift. Instead, the long-range antiferroquadrupolar order yields a characteristic resonance peak in the ESR spectrum, which we call a magnon-pair resonance peak. This resonance corresponds to the excitation of the bound magnon pair at the wave vector $\bm k={\bm 0}$. Reflecting the condensation of bound magnon pairs, the field dependence of the magnon-pair resonance frequency shows a singular upturn at the saturation field. Moreover, the intensity of the magnon-pair resonance peak shows a characteristic angular dependence and it vanishes when the magnetic field is parallel to one of the axes that diagonalize the weak anisotropic interactions. We confirm these general properties of the magnon-pair resonance peak in the spin nematic phase by studying an $S=1$ bilinear-biquadratic model on the square lattice in the linear flavor-wave approximation. In addition, we argue applications to the $S=1/2$ frustrated ferromagnets and also the $S=1/2$ orthogonal dimer spin system SrCu$_2$(BO$_3$)$_2$, both of which are candidate materials of spin nematics. Our theory for the antiferroquadrupolar ordered phase is consistent with many features of the magnon-pair resonance peak experimentally observed in the low-magnetization regime of SrCu$_2$(BO$_3$)$_2$.

Synthesis, structure and magnetism of the new S = 1 kagome magnet NH4Ni2.5V2O7(OH)2⋅H2O

Kagome antiferromagnets (KAFMs) have long been known to host exotic electronic states due to their strong geometric frustration, including the quantum spin liquid state in systems. Away from that limit, S = 1 KAFMs are also predicted to host unconventional ground states such as spin nematic phases, but a paucity of studies on known model materials has restricted progress.Here, we present the crystal structure and preliminary magnetization measurements on the newly synthesized S = 1 KAFM, NH4Ni2.5V2O7(OH)H2O, which has the three-fold symmetry of the kagome lattice but significant site depletion, with ∼ site occupancy. Bulk magnetic data show clear evidence of frustration and competition between ferromagnetic and antiferromagnetic interactions. We propose that the magnetic Hamiltonian is frustrated and that anisotropic terms cause the formation of an unconventional ground state.

Nuclear magnetic resonance in high magnetic field: Application to condensed matter physics

In this review, we describe the potentialities offered by the nuclear magnetic resonance (NMR) technique to explore at a microscopic level new quantum states of condensed matter induced by high magnetic fields. We focus on experiments realised in resistive (up to 34 T) or hybrid (up to 45 T) magnets, which open a large access to these quantum phase transitions. After an introduction on NMR observables, we consider several topics: quantum spin systems (spin–Peierls transition, spin ladders, spin nematic phases, magnetisation plateaus, and Bose–Einstein condensation of triplet excitations), the field-induced charge density wave (CDW) in high-Tc superconductors, and exotic superconductivity including the Fulde–Ferrel–Larkin–Ovchinnikov superconducting state and the field-induced superconductivity due to the Jaccarino–Peter mechanism. Dans cette revue, nous décrivons les opportunités offertes par la résonance magnétique nucléaire (RMN) pour étudier les propriétés microscopiques des nouveaux états quantiques de la matière induits par les champs magnétiques intenses. Nous mettons l'accent sur les expériences réalisées dans des bobines résistives (jusqu'à 34 T) ou hybrides (jusqu'à 45 T), qui ouvrent un large accès à ce type de transitions quantiques. Après avoir introduit les quantités observables par RMN, nous considérons plusieurs domaines de recherche : les systèmes de spins quantiques (la transition de spin–Peierls, les échelles de spin, les phases nématiques de spin, les plateaux d'aimantation et la condensation de Bose–Einstein des excitations triplets), l'onde de densité de charge induite sous champ dans les supraconducteurs à haute Tc, et la supraconductivité exotique, avec la phase supraconductrice Fulde–Ferrel–Larkin–Ovchinnikov et la supraconductivité induite sous champ de type Jaccarino–Peter.

Angular dependence of electron spin resonance for detecting the quadrupolar liquid state of frustrated spin chains

Spin nematic phase is a phase of frustrated quantum magnets with a quadrupolar order of electron spins. Since the spin nematic order is usually masked in experimentally accessible quantities, it is important to develop a methodology for detecting the spin nematic order experimentally. In this paper we propose a convenient method for detecting quasi-long-range spin nematic correlations of a quadrupolar Tomonaga-Luttinger liquid state of $S=1/2$ frustrated ferromagnetic spin chain compounds, using electron spin resonance (ESR). We focus on linewidth of a so-called paramagnetic resonance peak in ESR absorption spectrum. We show that a characteristic angular dependence of the linewidth on the direction of magnetic field arises in the spin nematic phase. Measurments of the angular dependence give a signature of the quadrupolar Tomonaga-Luttinger liquid state. In our method we change only the direction of the magnetic field, keeping the magnitude of the magnetic field and the temperature. Therefore, our method is advantageous for investigating the one-dimensional quadrupolar liquid phase that usually occupies only a narrow region of the phase diagram.

Spin multiplole moments as collective quantum phenomena

In this paper we investigate the occurrence of multipole moments of a collection of spins in a quantum magnetic system. To get insights into the behaviour of such systems we start by considering small spin clusters composed of dimers, trimers, as well as mixed spin systems with four spins. We focus our attention on the quantum multipole states, that gave rise to the widely discussed spin nematic and spin liquid phases. The magnetic properties of these systems are computed and the main differences between bosonic and fermionic multipolar states are discussed.