Master Equations for pulsed magnetic fields: Application to magnetic molecules

We extend spin-lattice relaxation theory to incorporate the use of pulsed magnetic fields for probing the hysteresis effects and magnetization steps and plateaus exhibited, at low temperatures, by the dynamical magnetization of magnetic molecules. The main assumption made is that the lattice degrees of freedom equilibrate in times much shorter than both the experimental time scale (determined by the sweep rate) and the typical spin-lattice relaxation time. We first consider the isotropic case (a magnetic molecule with a ground state of spin $S$ well separated from the excited levels and also the general isotropic Heisenberg Hamiltonian where all energy levels are relevant) and then we include small off-diagonal terms in the spin Hamiltonian to take into account the Landau-Zener-St\"{u}ckelberg (LZS) effect. In the first case, and for an $S=1/2$ magnetic molecule we arrive at the generalized Bloch equation recently used for the magnetic molecule \{V$_6$\} in Phys. Rev. Lett. 94, 147204 (2005). An analogous equation is derived for the magnetization, at low temperatures, of antiferromagnetic ring systems. The LZS effect is discussed for magnetic molecules with a low spin ground state, for which we arrive at a very convenient set of equations that take into account the combined effects of LZS and thermal transitions. In particular, these equations explain the deviation from exact magnetization reversal at $B\approx 0$ observed in \{V$_6$\}. They also account for the small magnetization plateaus (``magnetic Foehn effect''), following the LZS steps, that have been observed in several magnetic molecules. Finally, we discuss the role of the Phonon Bottleneck effect at low temperatures and specifically we indicate how this can give rise to a pronounced Foehn effect.Comment: 10 pages, 4 figure

Classical spin liquid instability driven by off-diagonal exchange in strong spin-orbit magnets

We show that the off-diagonal exchange anisotropy drives Mott insulators with strong spin-orbit coupling to a classical spin liquid regime, characterized by an infinite number of ground states and Ising variables living on closed or open strings. Depending on the sign of the anisotropy, quantum fluctuations either fail to lift the degeneracy down to very low temperatures, or select non-collinear magnetic states with unconventional spin correlations. The results apply to all 2D and 3D tri-coordinated materials with bond-directional anisotropy, and provide a consistent interpretation of the suppression of the x-ray magnetic circular dichroism signal reported recently for $\beta$-Li$_2$IrO$_3$ under pressure

Theoretical investigation of dynamic properties of magnetic molecule systems as probed by NMR and pulsed fields experiments

In this dissertation we theoretically investigate static and especially dynamic properties of magnetic molecules (MM\u27s), as probed by the nuclear spin lattice relaxation rate 1/T1 (first part) and pulsed fields measurements of the magnetization M( t) (second part). In the first part, we provide a general first-principles account for 1/T1, which incorporates the decay of spin fluctuations and the corresponding broadening of the discrete magnetic energy levels of MM\u27s. This is achieved by including the interaction of the electronic moments with the local deformation of the host lattice (phonons), in the Markovian regime and employing the quantum regression theorem. Within this framework, we provide a rigorous interpretation of a number of 1/ T1 experimental findings in MM\u27s. We also provide an extensive account of the model spin-1/2 tetramer V12 by analyzing magnetic susceptibility and 1/T1 data. The second part focuses on phenomena manifested in pulsed fields measurements of M(t), such as hysteresis loops and Landau-Zener-Stuckelberg (LZS) steps. First, we give a theoretical analysis of the low-T hysteresis loops and LZS steps at B ≈ 0 observed in the magnetic molecule V6. The loops are successfully reproduced by employing a generalization of the standard Bloch equation which in turn reveals the one-phonon acoustic processes as the dominant source of relaxation in this system. The origin of the US steps is attributed to the presence in V 6 of a weak intra-molecular anisotropic exchange. The small deviation from the quantum-mechanical prediction of exact magnetization reversals at B ≈ 0 is attributed to the role of the phonon heat bath (dissipative US problem). Second, we provide a general, first-principles account of all dynamic phenomena manifested in pulsed fields experiments, by extending the standard spin-lattice relaxation theory to include time-dependent (pulsed) fields. This theory accounts for: (i) hysteresis effects (including the generalized Bloch equation used for V6), (ii) the effects associated with the dissipative US problem, in the adiabatic regime and in particular, (iii) the so-called magnetic Foehn effect. We also discuss how the phonon bottleneck effect (typically occurring at T ≲ 1 K) can give rise to an enhanced Foehn effect

Microscopic theory of the nearest-neighbor valence bond sector of the spin-1/2 kagome antiferromagnet

The spin-1/2 Heisenberg model on the kagome lattice, which is closely realized in layered Mott insulators such as ZnCu$_3$(OH)$_6$Cl$_2$, is one of the oldest and most enigmatic spin-1/2 lattice model. While the numerical evidence has accumulated in favor of a quantum spin liquid, the debate is still open as to whether it is a $Z_2$ spin liquid with very short-range correlations (some kind of Resonating Valence Bond spin liquid), or an algebraic spin-liquid with power-law correlations. To address this issue, we have pushed the program started by Rokhsar and Kivelson in their derivation of the effective quantum dimer model description of Heisenberg models to unprecedented accuracy for the spin-1/2 kagome, by including all the most important virtual singlet contributions on top of the orthogonalization of the nearest-neighbor valence bond singlet basis. Quite remarkably, the resulting picture is a competition between a $Z_2$ spin liquid and a diamond valence bond crystal with a 12-site unit cell, as in the DMRG simulations of Yan, Huse and White. Furthermore, we found that, on cylinders of finite diameter $d$, there is a transition between the $Z_2$ spin liquid at small $d$ and the diamond valence bond crystal at large $d$, the prediction of the present microscopic description for the 2D lattice. These results show that, if the ground state of the spin-1/2 kagome antiferromagnet can be described by nearest-neighbor singlet dimers, it is a diamond valence bond crystal, and, a contrario, that, if the system is a quantum spin liquid, it has to involve long-range singlets, consistent with the algebraic spin liquid scenario.Comment: 11 pages, 14 figures. Revised and extended version. Results are untouched, implications have been clarified and better put in contex

Highly Frustrated Magnetic Clusters: The kagome on a sphere

We present a detailed study of the low-energy excitations of two existing finite-size realizations of the planar kagome Heisenberg antiferromagnet on the sphere, the cuboctahedron and the icosidodecahedron. After highlighting a number of special spectral features (such as the presence of low-lying singlets below the first triplet and the existence of localized magnons) we focus on two major issues. The first concerns the nature of the excitations above the plateau phase at 1/3 of the saturation magnetization Ms. Our exact diagonalizations for the s=1/2 icosidodecahedron reveal that the low-lying plateau states are adiabatically connected to the degenerate collinear ``up-up-down'' ground states of the Ising point, at the same time being well isolated from higher excitations. A complementary physical picture emerges from the derivation of an effective quantum dimer model which reveals the central role of the topology and the intrinsic spin s. We also give a prediction for the low energy excitations and thermodynamic properties of the spin s=5/2 icosidodecahedron Mo72Fe30. In the second part we focus on the low-energy spectra of the s>1/2 Heisenberg model in view of interpreting the broad inelastic neutron scattering response reported for Mo72Fe30. To this end we demonstrate the simultaneous presence of several broadened low-energy ``towers of states'' or ``rotational bands'' which arise from the large discrete spatial degeneracy of the classical ground states, a generic feature of highly frustrated clusters. This semiclassical interpretation is further corroborated by their striking symmetry pattern which is shown, by an independent group theoretical analysis, to be a characteristic fingerprint of the classical coplanar ground states.Comment: 22 pages Added references Corrected typo

Quantum spin liquid in the semiclassical regime

Quantum spin liquids have been at the forefront of correlated electron research ever since their original proposal in 1973, and the realization that they belong to the broader class of intrinsic topological orders, along with the fractional quantum Hall states. According to received wisdom, quantum spin liquids can arise in frustrated magnets with low spin $S$, where strong quantum fluctuations act to destabilize conventional, magnetically ordered states. Here we present a magnet that has a $Z_2$ quantum spin liquid ground state already in the semiclassical, large-$S$ limit. The state has both topological and symmetry related ground state degeneracy, and two types of gaps, a `magnetic flux' gap that scales linearly with $S$ and an `electric charge' gap that drops exponentially in $S$. The magnet is described by the spin-$S$ version of the spin-1/2 Kitaev honeycomb model, which has been the subject of intense studies in correlated electron systems with strong spin-orbit coupling, and in optical lattice realizations with ultracold atoms. The results apply to both integer and half-integer spins

Quantum dimer model for the spin-1/2 kagome Z2 spin liquid

We revisit the description of the low-energy singlet sector of the spin-1/2 Heisenberg antiferromagnet on kagome in terms of an effective quantum dimer model. With the help of exact diagonalizations of appropriate finite-size clusters, we show that the embedding of a given process in its kagome environment leads to dramatic modifications of the amplitudes of the elementary loop processes, an effect not accessible to the standard approach based on the truncation of the Hamiltonian to the nearest-neighbour valence-bond basis. The resulting parameters are consistent with a Z$_2$ spin liquid rather than with a valence-bond crystal, in agreement with the last density matrix renormalization group results.Comment: Potential terms of the effective QDM include

Entangled tetrahedron ground state and excitations of the magneto-electric skyrmion material Cu2_2OSeO3_3

The strongly correlated cuprate Cu$_2$OSeO$_3$ has recently been identified as the first insulating system exhibiting a skyrmion lattice phase. Using a microscopic multi-boson theory for its magnetic ground state and excitations, we establish the presence of two distinct types of modes: a low energy manifold that includes a gapless Goldstone mode and a set of weakly dispersive high-energy magnons. These spectral features are the most direct signatures of the fact that the essential magnetic building blocks of Cu$_2$OSeO$_3$ are not individual Cu spins, but rather weakly-coupled Cu$_4$ tetrahedra. Several of the calculated excitation energies are in nearly perfect agreement with reported Raman and far-infrared absorption data, while the magneto-electric effect determined within the present quantum-mechanical framework is also fully consistent with experiments, giving strong evidence in the entangled Cu$_4$ tetrahedra picture of Cu$_2$OSeO$_3$. The predicted dispersions along with the dynamical dipole and quadrupole spin structure factors call for further experimental tests of this picture.Comment: 4 pages main text + 5 pages supplementary material, 3 figure

Frustration and Dzyaloshinsky-Moriya anisotropy in the kagome francisites Cu3_3Bi(SeO3)2_3)_2O2_2X

We investigate the antiferromagnetic canting instability of the spin-1/2 kagome ferromagnet, as realized in the layered cuprates Cu$_3$Bi(SeO$_3)_2$O$_2$X (X=Br, Cl, and I). While the local canting can be explained in terms of competing exchange interactions, the direction of the ferrimagnetic order parameter fluctuates strongly even at short distances on account of frustration which gives rise to an infinite ground state degeneracy at the classical level. In analogy with the kagome antiferromagnet, the accidental degeneracy is fully lifted only by non-linear 1/S corrections, rendering the selected uniform canted phase very fragile even for spins-1/2, as shown explicitly by coupled-cluster calculations. To account for the observed ordering, we show that the minimal description of these systems must include the microscopic Dzyaloshinsky-Moriya interactions, which we obtain from density-functional band-structure calculations. The model explains all qualitative properties of the kagome francisites, including the detailed nature of the ground state and the anisotropic response under a magnetic field. The predicted magnon excitation spectrum and quantitative features of the magnetization process call for further experimental investigations of these compounds.Comment: 21 pages, 6 figure