Properties Of Quantum Magnets Research Articles

An Air-Stable Carbon-Centered Triradical with a Well-Addressable Quartet Ground State.

Organic polyradicals with a high-spin ground state and quantum magnetic properties suitable for spin manipulation are valuable materials for diverse innovative technologies, including quantum devices. However, the typically high reactivity and low stability of conventional polyradicals present a major obstacle to such applications. In this study, a highly stable carbon-centered triradical TR with a quartet ground state and excellent stability (τ1/2 of ∼90 days in air-saturated toluene at room temperature) is achieved, which shows apposite magnetic anisotropy and Zeeman splitting partition with favorable addressability. By virtue of the optimal stability, thorough structural and magnetic characterizations are realized. With X-ray crystallography unambiguously proving the molecular structure, the quartet ground state (ΔED-Q = 0.78 kcal/mol) is confirmed by the SQUID measurements, while the cw- and pulsed EPR techniques offer additional supportive evidence for the high-spin nature. Remarkably, owing to the easily attained magnetic anisotropy, selective excitations between different Zeeman splitting levels are successfully demonstrated with TR in its frozen toluene solution without the requirement for special alignment, which is unprecedented for organic polyradicals. Along with the millisecond spin-lattice relaxation and microsecond coherence time manifested by TR, this triradical is promising for potential coherent spin manipulation applications as a multienergy-level quantum information carrier.

Magnetic properties and entanglement of the octanuclear nickel phosphonate-based cage

The main subject considered in this paper is the quantum magnetic properties and entanglement of an octanuclear nickel phosphonate-based cage. We measured the temperature-dependent magnetic susceptibility of this cage, which indicates the coexistence of both antiferromagnetic and ferromagnetic interactions between the magnetic centers, Ni ions with spin 1. This observation prompted us to theoretically investigate the magnetic properties of such compounds. Our theoretical calculations were compared with the experimental results for magnetic susceptibility. Additionally, we explored the magnetization plateaus and magnetic susceptibility from an external magnetic field at low temperatures. We determined the thermal entanglement (negativity) and the logarithmic negativity for the octanuclear nickel phosphonate-based cage. The observed correlation between magnetization plateau jumps and magnetic susceptibility peaks in relation to the external magnetic field suggests the need for further experimental measurements.

Quantum Magnetic Properties and Metal‐to‐Insulator Transition in Chemically Doped Calcium Ruthenate Perovskite

Ruthenates provide a comprehensive platform to study a plethora of novel properties, such as quantum magnetism, superconductivity, and magnetic fluctuation mediated metal–insulator transition (MIT). Herein, an overview of quantum mechanical phenomenology in calcium ruthenium oxide with varying compositions is provided. While the stoichiometric composition of exhibits non‐fermi liquid (FL) behavior with quasi‐criticality, chemically doped compounds depict prominent signatures of quantum magnetic fluctuations at low temperature that in some cases are argued to mediate in metal–insulator transition. In the case of cobalt‐doped , an unusual continuum fluctuation is found to persist deep inside the glassy phase of the material. These observations reflect the richness of the ruthenate research platform in the study of quantum magnetic phenomena of fundamental importance.

Effect of Oxygen on the Quantum, Magnetic, and Thermodynamic Properties of Co Nanowires on the Reconstructed Anisotropic (1 × 2)/Au(110) and (1 × 2)/Pt(110) Surfaces: Ab Initio Approach

Ab initio theoretical study of the quantum magnetic properties of Co nanowires on the pure and oxygen-reconstructed (1 × 2)/Au(110) and (1 × 2)/Pt(110) surfaces is performed. Their structures and electronic configurations are calculated using the electron density functional theory. High values of magnetic moment and magnetic anisotropy energies of Co atoms are found on both pure and oxygen-reconstructed (1 × 2)/Au(110) and (1 × 2)/Pt(110) surfaces. The adsorption of oxygen atoms on the (1 × 2)/Au(110) substrate is shown to affect the structural arrangement of Co nanowire atoms on this substrate and to increase the magnetic anisotropy energy (by 1.91 meV per nanowire atom). The adsorption of oxygen on the Pt(110) substrate substantially decreases the magnetic anisotropy energy of the Co nanowire on it (by 5.98 meV per atom). The origin of these changes is revealed by analyzing the local densities of states of the d electrons of nanowire atoms. The temperature ranges of the states with the lowest free surface energy are determined using the atomistic thermodynamics methods. These data and the available experimental data are used to predict the possibility of observing the structures under study in experiments.

Quantum Magnetic Properties in Perovskite with Anderson Localized Artificial Spin-1/2.

Quantum magnetic properties in a geometrically frustrated lattice of spin‐1/2 magnet, such as quantum spin liquid or solid and the associated spin fractionalization, are considered key in developing a new phase of matter. The feasibility of observing the quantum magnetic properties, usually found in geometrically frustrated lattice of spin‐1/2 magnet, in a perovskite material with controlled disorder is demonstrated. It is found that the controlled chemical disorder, due to the chemical substitution of Ru ions by Co‐ions, in a simple perovskite CaRuO3 creates a random prototype configuration of artificial spin‐1/2 that forms dimer pairs between the nearest and further away ions. The localization of the Co impurity in the Ru matrix is analyzed using the Anderson localization formulation. The dimers of artificial spin‐1/2, due to the localization of Co impurities, exhibit singlet‐to‐triplet excitation at low temperature without any ordered spin correlation. The localized gapped excitation evolves into a gapless quasi‐continuum as dimer pairs break and create freely fluctuating fractionalized spins at high temperature. Together, these properties hint at a new quantum magnetic state with strong resemblance to the resonance valence bond system.

Quasi-two-dimensional Bose-Einstein condensation of spin triplets in the dimerized quantum magnetBa2CuSi2O6Cl2

We synthesized single crystals of composition Ba$_2$CuSi$_2$O$_6$Cl$_2$ and investigated its quantum magnetic properties. The crystal structure is closely related to that of the quasi-two-dimensional (2D) dimerized magnet BaCuSi$_2$O$_6$ also known as Han purple. Ba$_2$CuSi$_2$O$_6$Cl$_2$ has a singlet ground state with an excitation gap of ${\Delta}/k_{\rm B}\,{=}\,20.8$ K. The magnetization curves for two different field directions almost perfectly coincide when normalized by the $g$-factor except for a small jump anomaly for a magnetic field perpendicular to the $c$ axis. The magnetization curve with a nonlinear slope above the critical field is in excellent agreement with exact-diagonalization calculations based on a 2D coupled spin-dimer model. Individual exchange constants are also evaluated using density functional theory (DFT). The DFT results demonstrate a 2D exchange network and weak frustration between interdimer exchange interactions, supported by weak spin-lattice coupling implied from our magnetostriction data. The magnetic-field-induced spin ordering in Ba$_2$CuSi$_2$O$_6$Cl$_2$ is described as the quasi-2D Bose-Einstein condensation of triplets.

Critical behavior of quantum magnets with long-range interactions in the thermodynamic limit

Quasiparticle properties of quantum magnets with long-range interactions are investigated by high-order linked-cluster expansions in the thermodynamic limit. It is established that perturbative continuous unitary transformations on white graphs are a promising and flexible approach to treat long-range interactions in quantum many-body systems. We exemplify this scheme for the one-dimensional transverse-field Ising chain with long-range interactions. For this model the elementary Quasiparticle gap is determined allowing to access the quantum-critical regime including critical exponents and multiplicative logarithmic corrections for the ferro- and antiferromagnetic case.

Almost Perfect Frustration in the Dimer Magnet Ba2CoSi2O6Cl2

We determined the crystal structure of Ba$_2$CoSi$_2$O$_6$Cl$_2$, which was synthesized in this work, and investigated its quantum magnetic properties using single crystals. This compound should be described as a two-dimensionally coupled spin-1/2 XY-like spin dimer system. Ba$_2$CoSi$_2$O$_6$Cl$_2$ exhibits a stepwise magnetization process with a plateau at half of the saturation magnetization, irrespective of the field direction, although all the Co$^{2+}$ sites are equivalent. This indicates that spin triplets are localized owing to the almost perfect frustration of interdimer exchange interactions. Thus, the spin states for the zero and 1/2 magnetization-plateau states are almost exactly given by the simple product of singlet dimers and the alternate product of singlet and triplet dimers, respectively.

Microscopic observation of magnon bound states and their dynamics

The existence of bound states of elementary spin waves (magnons) in one-dimensional quantum magnets was predicted almost 80 years ago. Identifying signatures of magnon bound states has so far remained the subject of intense theoretical research, and their detection has proved challenging for experiments. Ultracold atoms offer an ideal setting in which to find such bound states by tracking the spin dynamics with single-spin and single-site resolution following a local excitation. Here we use in situ correlation measurements to observe two-magnon bound states directly in a one-dimensional Heisenberg spin chain comprising ultracold bosonic atoms in an optical lattice. We observe the quantum dynamics of free and bound magnon states through time-resolved measurements of two spin impurities. The increased effective mass of the compound magnon state results in slower spin dynamics as compared to single-magnon excitations. We also determine the decay time of bound magnons, which is probably limited by scattering on thermal fluctuations in the system. Our results provide a new way of studying fundamental properties of quantum magnets and, more generally, properties of interacting impurities in quantum many-body systems.

Angle-resolved NMR: Quantitative theory of75AsT1relaxation rate in BaFe2As2

While NMR measurements of nuclear energy spectra are routinely used to characterize the static properties of quantum magnets, the dynamical information locked in NMR 1/T1 relaxation rates remains notoriously difficult to interpret. The difficulty arises from the fact that information about all possible low-energy spin excitations of the electrons, and their coupling to the nuclear moments, is folded into a single number, 1/T1. Here we develop a quantitative theory of the NMR 1/T1 relaxation rate in a collinear antiferromagnet, focusing on the specific example of BaFe2As2. One of the most striking features of magnetism in BaFe2As2 is a strong dependence of 1/T1 on the orientation of the applied magnetic field. By careful analysis of the coupling between the nuclear and electronic moments, we show how this anisotropy arises from the "filtering" of spin fluctuations by the form-factor for transferred hyperfine interactions. This allows us to make convincing, quantitative, fits to experimental 1/T1 data for BaFe2As2, for different field orientations. We go on to show how a quantitative, angle-dependent theory for the relaxation rate leads to new ways of measuring the dynamical parameters of magnetic systems, in particular the spin wave velocities.

Ab initiomodeling of Bose-Einstein condensation in Pb2V3O9

We apply density functional theory band structure calculations and quantum Monte Carlo simulations to investigate the Bose-Einstein condensation in the spin-1/2 quantum magnet Pb2V3O9. In contrast to previous conjectures on the one-dimensional nature of this compound, we present a quasi-two-dimensional model of spin dimers with ferromagnetic and antiferromagnetic interdimer couplings. Our model is well justified microscopically and provides a consistent description of the experimental data on the magnetic susceptibility, high-field magnetization, and field vs. temperature phase diagram. The Bose-Einstein condensation in the quasi-two-dimensional spin system of Pb2V3O9 is largely governed by intralayer interactions, whereas weak interlayer couplings have a moderate effect on the ordering temperature. The proposed computational approach is an efficient tool to analyze and predict high-field properties of quantum magnets.

Giant Modification of the Magnetocrystalline Anisotropy in Transition-Metal Monolayers by an External Electric Field

Controlling and designing quantum magnetic properties by an external electric field is a key challenge in modern magnetic physics. Here, from first principles, the effects of an external electric field on the magnetocrystalline anisotropy (MCA) in ferromagnetic transition-metal monolayers are demonstrated which show that the MCA in an Fe(001) monolayer [but not in Co(001) and Ni(001) monolayers] can be controlled by the electric field through a change in band structure, in which small components of the p orbitals near the Fermi level, which are coupled to the d states by the electric field, play a key role. This prediction obtained opens a way to control the MCA by the electric field and invites experiments.

The tuning of quantum magnetization for organic/inorganic hybrid materials composed of Mn 12-acetate and azobenzene casted into PMMA films on PVA films

In order to examine the effects of polymer matrix substituting crystalline solvents and photoisomerization of azobenzene in photo-modulation of AC susceptibility discovered recently, we have compared various quantum magnetic properties of new organic/inorganic hybrid materials composed of Mn 12-acetate (a typical single-molecule magnet, [Mn 12(CH 3COO) 16(H 2O) 4O 12]·2CH 3COOH·4H 2O) containing or not containing azobenzene casted into polymethylmethacrylate (PMMA) films on Polyvinylalchol (PVA) films. The M– H hysteresis loops below blocking temperature for both materials exhibited distinct differences of the d M/d H vs. H plots, which suggested azobenzene as well as crystalline solvents resulted in tuning of magnetic properties. Moreover, the AC susceptibility at 0.1–1000 Hz frequencies provided activation energy U eff=87 K from Arrhenius law for both materials, albeit Cole–Cole plots indicated perturbation of quantum magnetization for both hybrid materials in polymer matrix.

ODD AND EVEN BEHAVIOR WITH LSUBm APPROXIMATION LEVEL IN HIGH-ORDER COUPLED CLUSTER METHOD (CCM) CALCULATIONS

The coupled cluster method (CCM) is a powerful and widely applied technique of modern-day quantum many-body theory. It has been used with great success in order to understand the properties of quantum magnets at zero temperature. This is largely due to the application of computational techniques that allow the method to be applied to high orders of approximation using a localized scheme known as the LSUBm scheme. A hitherto unreported aspect of this scheme is that results for LSUBm expectation values behave in distinctly different ways with odd and even values of m. Here, we consider the behavior of ground-state expectation values of odd and even orders of the CCM LSUBm approximation for unfrustrated spin-half Heisenberg antiferromagnets on the square and honeycomb lattice and the frustrated spin-half Heisenberg antiferromagnet on the triangular lattice. We demonstrate that results for odd and even orders of approximation show qualitatively different behavior for both the ground-state energy and the sublattice magnetization. Indeed, the odd series consistently forms an upper branch of results, and the even series a lower branch with respect to both ground-state energy and sublattice magnetization, for all of the models considered here.

Liquid–gas and other unusual thermal phase transitions in some large- N magnets

Much insight into the low temperature properties of quantum magnets has been gained by generalizing them to symmetry groups of order N, and then studying the large- N limit. In this paper we consider an unusual aspect of their finite temperature behavior—their exhibiting a phase transition between a perfectly paramagnetic state and a paramagnetic state with a finite correlation length at N=∞. We analyze this phenomenon in some detail in the large “spin” (classical) limit of the SU( N) ferromagnet which is also a lattice discretization of the CP N−1 model. We show that at N=∞ the order of the transition is governed by lattice connectivity. At finite values of N, the transition goes away in one or less dimension but survives on many lattices in two dimensions and higher, for sufficiently large N. The latter conclusion contradicts a recent conjecture of Sokal and Starinets [Nucl. Phys. B 601 (2001) 425], yet is consistent with the known finite temperature behavior of the SU(2) case. We also report closely related first order paramagnet–ferromagnet transitions at large N and shed light on a violation of Elitzur's theorem at infinite N via the large- q limit of the q state Potts model, reformulated as an Ising gauge theory.