Spin Jam: a quantum-fluctuation-induced glassy state of a frustrated magnet
Junjie Yang, Anjana Samarakoon, Sachith Dissanayake, Hiroaki Ueda, Israel Klich, Kazuki Iida, Daniel Pajerowski, Nicholas P. Butch, Q. Huang, John R. D. Copley, Seung-Hun Lee
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Published as Proc. Natl. Acad. Sci. USA, doi:10.1073/pnas.1503126112
Since the discovery of spin glasses in dilute magnetic systems, their study has been largely focused on understanding randomness and defects as the driving mechanism. The same paradigm has also been applied to explain glassy states found in dense frustrated systems. Recently, however, it has been theoretically suggested that different mechanisms, such as quantum fluctuations and topological features, may induce glassy states in defect-free spin systems, far from the conventional dilute limit. Here we report experimental evidence for the existence of a glassy state, that we call a spin jam, in the vicinity of the clean limit of a frustrated magnet, which is insensitive to a low concentration of defects. We have studied the effect of impurities on SrCr9pGa12-9pO19 (SCGO(p)), a highly frustrated magnet, in which the magnetic Cr3+ (s=3/2) ions form a quasi-two-dimensional triangular system of bi-pyramids. Our experimental data shows that as the nonmagnetic Ga3+ impurity concentration is changed, there are two distinct phases of glassiness: a distinct exotic glassy state, which we call a "spin jam", for high magnetic concentration region (p>0.8) and a cluster spin glass for lower magnetic concentration, (p<0.8). This observation indicates that a spin jam is a unique vantage point from which the class of glassy states in dense frustrated magnets can be understood.
We present an extensive numerical study of a new type of frustrated itinerant magnetism on the pyrochlore lattice. In this theory, the pyrochlore magnet can be viewed as a cross-linking network of Kondo or double-exchange chains. Contrary to models based on Mott insulators, this itinerant magnetism approach provides a natural explanation for several spin and orbital superstructures observed on the pyrochlore lattice. Through extensive Monte Carlo simulations, we obtain the phase diagrams at two representative electron filling fractions $n = 1/2$ and 2/3. In particular, we show that an intrigui…
The development of spin glass like state in a geometrically frustrated (GF) magnet is a matter of great debate. We investigated the effect of magnetic (Mn) and nonmagnetic (Ga) doping at the Cr site of the layered GF antiferromagnetic compound LiCrO2. 10% Ga doping at the Cr site does not invoke any metastability typical of a glassy magnetic state. However, similar amount of Mn doping certainly drives the system to a spin glass state which is particularly evident from the relaxation, magnetic memory and heat capacity studies. The onset of glassy state in 10% Mn doped sample is of reentrant typ…
We show that introducing long-range Coulomb interactions immediately lifts the massive ground state degeneracy induced by geometric frustration for electrons on quarter-filled triangular lattices in the classical limit. Important consequences include the stabilization of a stripe-ordered crystalline (global) ground state, but also the emergence of very many low-lying metastable states with amorphous "stripe-glass" spatial structures. Melting of the stripe order thus leads to a frustrated Coulomb liquid at intermediate temperatures, showing remarkably slow (viscous) dynamics, with very long rel…
Here, we report both ac and dc magnetization, thermodynamic and electric properties of hexagonal Ba$_3$NiIr$_2$O$_9$. The Ni$^{2+}$ (spin-1) forms layered triangular-lattice and interacts antiferromagnetically while Ir$^{5+}$ is believed to act as magnetic link between the layers. This complex magnetic interaction results in magnetic frustration leading to a spin-glass transition at $T_f$ $\sim$ 8.5 K. The observed magnetic relaxation and aging effect also confirms the nonequilibrium ground state. The system further shows large exchange bias which is tunable with cooling field. Below the Curie…
Highly frustrated systems have macroscopically degenerate ground states that lead to novel properties. In magnetism its consequences underpin exotic and technologically important effects, such as, high temperature superconductivity, colossal magnetoresistence, and the anomalous Hall effect. One of the enduring mysteries of frustrated magnetism is why certain experimental systems have a spin glass transition and its exact nature, given that it is not determined by the strength of the dominant magnetic interactions. There have been some suggestions that real systems possess disorder of the magne…
Topological spin freezing in frustrated quantum materials
Indian Institute of Technology Madras（印度马德拉斯理工学院）；Quantum Centre of Excellence for Diamond and Emergent Materials, Indian Institute of Technology Madras（印度马德拉斯理工学院钻石与新兴材料卓越量子中心）
Since the first observation of weak ferromagnetism in the charge-transfer salt kappa-(BEDT-TTF)2-Cu[N(CN)2]Cl [U. Welp et al., Phys. Rev. Lett. 69, 840 (1992)], no further evidence of ferromagnetism in this class of organic materials has been reported. Here we present static and dynamic spin susceptibility measurements on kappa-(BEDT-TTF)2Hg(SCN)2Br revealing weak ferromagnetism below about TWF = 20 K. We suggest that frustrated spins in the molecular dimers suppress long-range order, forming a spin-glass ground state in the insulating phase.
The anelastic spectra (elastic energy loss and dynamic modulus versus temperature) of La1-xCaxMnO3 have been measured for 0.33< x < 0.5. A peak in the imaginary part of the elastic susceptibility is found slightly below the Curie temperature, whose temperature and frequency dependences are typical of the dielectric and magnetic susceptibilities of relaxor ferroelectrics, spin glasses and other inhomogeneous frustrated systems. The fluctuations can be associated with the magnetic clusters which are observed by several techniques or with charge-ordered insulating domains in the low temperature i…
Fractons are topological quasiparticles with limited mobility. While there exists a variety of models hosting these excitations, typical fracton systems require rather complicated many-particle interactions. Here, we discuss fracton behavior in the more common physical setting of classical kagome spin models with frustrated two-body interactions only. We investigate systems with different types of elementary spin degrees of freedom (three-state Potts, XY, and Heisenberg spins) which all exhibit characteristic subsystem symmetries and fracton-like excitations. The mobility constraints of isolat…
We report neutron scattering studies of the spin correlations of the geometrically frustrated pyrochlore Tb2Mo2O7 using single crystal samples. This material undergoes a spin-freezing transition below Tg~24 K, similar to Y2Mo2O7, and has little apparent chemical disorder. Diffuse elastic peaks are observed at low temperatures, indicating short-range ordering of the Tb moments in an arrangement where the Tb moments are slightly rotated from the preferred directions of the spin ice structure. In addition, a Q-independent signal is observed which likely originates from frozen, but completely unco…
Geometric magnetic frustration (GMF) has attracted substantial interest due to the exotic physics and rich phase diagrams revealed by the cancellation of normally-dominant magnetic interactions, giving impetus for the search for novel frustrated systems, most often based on antiferromagnetic correlations between magnetic ions decorating triangular or tetrahedral lattices. We report here low-temperature magnetic susceptibility and muon spin relaxation results on Li4MgOsO6 and Li3Mg2OsO6, members of the A5BO6 "rock salt ordered" family of frustrated materials. In Li3Mg2OsO6 we find spin freezing…
We study a class of disordered continuous classical spin systems including the kagome Heisenberg magnet. While each term in its local Hamiltonian can be independently minimised, we find {\it discrete} degenerate ground states whose number grows exponentially with system size. These states do not exhibit zero-energy `excitations' characteristic of highly frustrated magnets but instead are local minima of the energy landscape, albeit with an anomalously soft excitation spectrum. This represents a spin liquid version of the phenomenon of jamming familiar from granular media and structural glasses…
We report the synthesis and characterization of a new quantum magnet [2-[Bis(2-hydroxybenzyl)aminomethyl]pyridine]Ni(II)-trimer (BHAP-Ni3) in single-crystalline form. Our combined experimental and theoretical investigations reveal an exotic spin state that stabilizes a robust 2/3 magnetization plateau between 7 and 20 T in an external magnetic field. AC-susceptibility measurements show the absence of any magnetic order/glassy state down to 60 mK. The magnetic ground state is disordered and specific-heat measurements reveal the gapped nature of the spin excitations. Most interestingly, our theo…
We study two dimensional frustrated but non-disordered systems applying a replica approach to a stripe forming model with competing interactions. The phenomenology of the model is representative of several well known systems, like high-Tc superconductors and ultrathin ferromagnetic films, which have been the subject of intense research. We establish the existence of a glass transition to a non-ergodic regime accompanied by an exponential number of long lived metastable states, responsible for slow dynamics and non-equilibrium effects.
The nature of the low temperature ground state of the pyrochlore compound Tb2Ti2O7 remains a puzzling issue. Dynamic fluctuations and short-range correlations persist down to 50 mK, as evidenced by microscopic probes. In parallel, magnetization measurements show irreversibilities and glassy behavior below 200 mK. We have performed magnetization and AC susceptibility measurements on four single crystals down to 57 mK. We did not observe a clear plateau in the magnetization as a function of field along the [111] direction, as suggested by the quantum spin ice model. In addition to a freezing aro…
We have investigated the magnetic, dielectric and magnetodielectric (MDE) behavior of a geometrically frustrated spin-chain system, Ca3Co1.4Rh0.6O6, in the single crystalline form for different orientations. The results bring out that the magnetic behavior of this compound is by itself interesting in the sense that this compound exhibits an anisotropic glassy-like magnetic behavior with a huge frequency dependence of ac susceptibility peak for an orientation along the spin-chain in the range 30-60 K; this behavior is robust to applications of large external magnetic fields (H) unlike in canoni…
We report a new peculiar effect of the interaction between a sublattice of frustrated quantum spin-1/2 chains and a sublattice of pseudospin-1/2 centers (quantum electric dipoles) uniquely co-existing in the complex oxide Li2ZrCuO4. 7Li nuclear magnetic-, Cu2+ electron spin resonance and a complex dielectric constant data reveal that the sublattice of Li+-derived electric dipoles orders glass like at Tg ~ 70 K yielding a spin site nonequivalency in the CuO2 chains. We suggest that such a remarkable interplay between electrical and spin degrees of freedom might strongly influence the properties…
We have systematically investigated the influence of gradual replacement of Ca by Gd on the magnetic and complex dielectric properties of the well-known geometrically frustrated spin-chain system, Ca3Co2O6 (T_N= 24 K with additional magnetic transitions below 12K), by studying the series, Ca3-xGdxCo2O6 (x less than 0.7), down to 1.8K. Heat capacity measurements establish that the reduction of T_N with Gd substitution is much less as compared to that by Y substitution. The magnetic moment data reveal that there are changes in the oxidation state of Co as well, unlike for Y-substitution, beyond …
Ba$_3$Mn$_2$O$_8$ is a geometrically frustrated spin dimer compound. We investigate the effect of site disorder on the zero field phase diagram of this material by considering the solid solution Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$, where nonmagnetic V$^{5+}$ ions partially substitute magnetic Mn$^{5+}$ ions. This substitution results in unpaired $S=1$ moments for half-substituted dimers, which are ungapped and therefore susceptible to types of magnetic order not present in the parent compound. AC susceptibility measurements of compositions between $x=0.046$ and $x=0.84$ show a sharp frequ…
Although most quantum systems thermalize locally on short time scales independent of initial conditions, recent developments have shown this is not always the case. Lattice geometry and quantum mechanics can conspire to produce constrained quantum dynamics and associated glassy behavior, a phenomenon that falls outside the rubric of the eigenstate thermalization hypothesis. Constraints "fragment" the many-body Hilbert space due to which some states remain insulated from others and the system fails to attain thermal equilibrium. Such fragmentation is a hallmark of geometrically frustrated magne…
