The LiHo_xY_{1-x}F_4 magnetic material in a transverse magnetic \nfield B_x perpendicular to the Ising spin direction has long been used \nto study tunable quantum phase transitions in pure and random disordered systems. \nWe first present analytical and numerical evidences for the validity of an effective spin-1/2 \napproach to the description of a general dipolar spin \nglass model with strong uniaxial Ising anisotropy and subject to weak \nB_x. \n We relate this toy model to the LiHo_xY_{1-x}F_4 transverse field Ising material. \n We show that an effective spin-1/2 \n model is able to capture both the qualitative and quantitative aspects of the \nphysics at small B_x. \nAfter confirming the validity of the effective spin-1/2 approach, we show that the field-induced magnetization along the \nx direction, \ncombined with the local random dilution-induced \ndestruction of crystalline mirror symmetries \ngenerates, via the predominant dipolar interactions between Ho^{3+} ions, \n random fields along the Ising z direction. \nThis identifies LiHo_xY_{1-x}F_4 in B_x as a new \nrandom field Ising system. \nWe show that the random fields explain the smearing \nof the nonlinear susceptibility at the spin glass transition \nwith increasing B_x. \nIn this thesis, we also investigate the phase diagram of non-diluted LiHoF_4 in the presence of B_x, by performing \nMonte-Carlo simulations. A previous quantum Monte Carlo (QMC) simulation found that even for small B_x where quantum fluctuations are small, close to the classical critical \npoint, there is a discrepancy between experiment and the QMC results. We revisit this problem, focusing on \nweak B_x close to the classical T_c, using an alternative approach. For small B_x, by applying a so-called cumulant \nexpansion, the quantum fluctuations around the classical T_c are taken into account perturbatively. We derived an effective \nperturbative classical Hamiltonian, on which MC simulations are performed. With this method we \ninvestigate different proposed sources of uncertainty which can affect the numerical results. \n We fully reproduce the previous QMC results at small B_x. Unfortunately, we find that \n none of the modifications to the microscopic Hamiltonian that we explore are able to provide a B_x-T phase diagram compatible with the experiments in the small \nsemi-classical B_x regime.
The LiHo_xY_{1-x}F_4 magnetic material in a transverse magnetic \nfield B_x perpendicular to the Ising spin direction has long been used \nto study tunable quantum phase transitions in pure and random disordered systems. \nWe first present analytical and numerical evidences for the validity of an effective spin-1/2 \napproach to the description of a general dipolar spin \nglass model with strong uniaxial Ising anisotropy and subject to weak \nB_x. \n We relate this toy model to the LiHo_xY_{1-x}F_4 transverse field Ising material. \n We show that an effective spin-1/2 \n model is able to capture both the qualitative and quantitative aspects of the \nphysics at small B_x. \nAfter confirming the validity of the effective spin-1/2 approach, we show that the field-induced magnetization along the \nx direction, \ncombined with the local random dilution-induced \ndestruction of crystalline mirror symmetries \ngenerates, via the predominant dipolar interactions between Ho^{3+} ions, \n random fields along the Ising z direction. \nThis identifies LiHo_xY_{1-x}F_4 in B_x as a new \nrandom field Ising system. \nWe show that the random fields explain the smearing \nof the nonlinear susceptibility at the spin glass transition \nwith increasing B_x. \nIn this thesis, we also investigate the phase diagram of non-diluted LiHoF_4 in the presence of B_x, by performing \nMonte-Carlo simulations. A previous quantum Monte Carlo (QMC) simulation found that even for small B_x where quantum fluctuations are small, close to the classical critical \npoint, there is a discrepancy between experiment and the QMC results. We revisit this problem, focusing on \nweak B_x close to the classical T_c, using an alternative approach. For small B_x, by applying a so-called cumulant \nexpansion, the quantum fluctuations around the classical T_c are taken into account perturbatively. We derived an effective \nperturbative classical Hamiltonian, on which MC simulations are performed. With this method we \ninvestigate different proposed sources of uncertainty which can affect the numerical results. \n We fully reproduce the previous QMC results at small B_x. Unfortunately, we find that \n none of the modifications to the microscopic Hamiltonian that we explore are able to provide a B_x-T phase diagram compatible with the experiments in the small \nsemi-classical B_x regime.
Several magnetic materials, in the first approximation, can be described by idealised theoretical models, such as classical Ising or Heisenberg spin systems, and, to some extent, such models are able to qualitatively expose many experimentally observed phenomena. But often, to account for complex behavior of magnetic matter, such models have to be refined by including more terms in Hamiltonian. The compound LiHo_xY_{1-x}F_4, by increasing concentration of nonmagnetic yttrium can be tuned from a diluted ferromagnet to a spin glass. LiHoF_4 is a good realisation of the transverse field Ising model, the simplest model exhibiting a quantum phase transition. In the pure case the magnetic behaviour of this material is well described by mean-field theory. It was believed that when diluted, LiHo_xY_{1-x}F_4 would also manifest itself as a diluted transverse field Ising model which continue to be well described by mean-field theory, and, at sufficient dilution, at zero temperature, exhibit a quantum spin-glass transition. The experimental data did not support such a scenario, and it was pointed out that, to explain physics of LiHo_xY_{1-x}F_4 in transverse magnetic field, the effect of a transverse-field-generated longitudinal random field has to be considered. We explore this idea further in local mean-field studies in which all three parameters: temperature, transverse field and concentration can be consistently surveyed, and where the transverse-field-generated longitudinal random field is explicitly present in the effective spin-1/2 Hamiltonian. We suggest other materials that are possible candidates for studying quantum criticality in the transverse field Ising model, and in the diluted case, for studying the effects of transverse and longitudinal random fields. The compounds we consider are RE(OH)_3, where RE are the rare earth ions Tb^{3+}, Dy^{3+} and Ho^{3+}. Using mean-field theory, we estimate the values of the transverse magnetic field that, at zero temperature, destroy ferromagnetic order to be B_x^c=4.35 T, B_x^c=5.03 T and B_x^c=54.81 T for Ho(OH)_3, Dy(OH)_3 and Tb(OH)_3, respectively. We confirm that Ho(OH)_3 and Tb(OH)_3, similarly to LiHoF_4, can be described by an effective spin-1/2 Hamiltonian. In the case of Dy(OH)_3 there is a possibility of a first order phase transition at transverse field close to B_x^c, and Dy(OH)_3 cannot be described by a spin-1/2 effective Hamiltonian. While diluted dipolar Ising spin glass has been studied experimentally in LiHo_xY_{1-x}F_4 and in numerical simulations, there are no studies of the Heisenberg case. Example materials that are likely candidates to be realisations of the diluted dipolar Heisenberg spin glass are (Gd_xY_{1-x})_2Ti_2O_7, (Gd_xY_{1-x})_2Sn_2O_7 and (Gd_xY_{1-x})_3Ga_5O_{12}. To stimulate interest in experimental studies of these systems we present results of Monte of Carlo simulations of the diluted dipolar Heisenberg spin glass. By performing finite-size scaling analysis of the spin-glass correlation length and the spin-glass susceptibility, we provide a compelling evidence of a thermodynamical spin-glass transition in the model. Frustrated pyrochlore magnets, depending on the character of single ion anisotropy and interplay of different types of interaction over a broad range of energy scales, exhibit a large spectrum of exotic phases and novel phenomena. The pyrochlore antiferromagnet Er_2Ti_2O_7 is characterised by a strong planar anisotropy. Experimental studies reveal that Er_2Ti_2O_7 undergoes a continuous phase transition to a long-range ordered phase with a spin configuration that, in this thesis, is referred to as the Champion-Holdsworth state. Such results are not in agreement with the theoretical prediction that the ground state of the pyrochlore easy-plane antiferromagnet with dipolar interactions complementing the nearest neighbour exchange interactions, is not the Champion-Holdsworth state but the so-called Palmer-Chalker state. On the other hand, Monte Carlo simulations of the easy-plane pyrochlore antiferromagnet indicate a thermal order-by-disorder selection of the Champion-Holdsworth state. To answer the question of whether order-by-disorder selection can be the mechanism at play in Er_2Ti_2O_7, we performed Monte Carlo simulations of the easy-plane pyrochlore antiferromagnet with weak dipolar interactions. We estimate the range strengths of the dipolar interaction such that order-by-disorder selection of the Champion-Holdsworth state is not suppressed. The estimated value of the allowed strength of the dipolar interactions indicates that the model studied is likely insufficient to explain the physics of Er_2Ti_2O_7 and other types of interactions or quantum effects should be considered.
The random-field Ising model (RFIM) is central to the study of disordered systems. Yet, for a long time it eluded realization in ferromagnetic systems because of the difficulty to produce locally random magnetic fields. Recently, it was shown that in anisotropic dipolar magnetic insulators, the archetype of which is the ${\text{LiHo}}_{x}{\text{Y}}_{1\ensuremath{-}x}{\text{F}}_{4}$ system, the RFIM can be realized in both ferromagnetic and spin-glass phases. The interplay between an applied transverse field and the off-diagonal terms of the dipolar interaction produce effective longitudinal fields, which are random in sign and magnitude as a result of spatial dilution. In this paper, we use exact numerical diagonalization of the full Hamiltonian of Ho pairs in ${\text{LiHo}}_{x}{\text{Y}}_{1\ensuremath{-}x}{\text{F}}_{4}$ to calculate the effective longitudinal field beyond the perturbative regime. In particular, we find that nearby spins can experience an effective field larger than the intrinsic dipolar broadening (of quantum states in zero field) which can therefore be evidenced in experiments. We then calculate the magnetization and susceptibility under several experimental protocols, and show how these protocols can produce direct measurement of the effective longitudinal field.
The rare-earth material LiHoF4 is believed to be an experimental realization of the celebrated (dipolar) Ising model and, upon the inclusion of a transverse field Bx, an archetypal quantum Ising model. Moreover, by substituting the magnetic Ho ions by nonmagnetic Y ions, disorder can be introduced into the system, giving rise to a dipolar disordered magnet and at high disorders to a spin glass. Indeed, this material has been scrutinized experimentally, numerically, and theoretically over many decades with the aim of understanding various collective magnetic phenomena. One of the to-date open questions is the discrepancy between the experimental and theoretical ${B}_{x}\ensuremath{-}T$ phase diagram at low fields and high temperatures. Here we propose a mechanism, backed by numerical results, that highlights the importance of quantum fluctuations induced by the off-diagonal dipolar terms, in determining the critical temperature of anisotropic dipolar magnets in the presence and in the absence of a transverse field. We thus show that the description as a simple Ising system is insufficient to quantitatively describe the full phase diagram of LiHoF4, for the pure as well as for the dilute system.
The quantum Ising model is perhaps the simplest possible model of a quantum magnetic material. Despite its simplicity, its versatility and wide range of applications, from quantum computation, to combinatorial optimization, to biophysics, make it one of the most important models of modern physics. In this thesis, we develop a general framework for studying quantum Ising systems with an arbitrary single ion Hamiltonian, with emphasis on the effects of quantum fluctuations, and the quantum phase transition between paramagnetic and ferromagnetic states that occurs when a magnetic field is applied transverse to the easy axis of the system. The magnetic insulating crystal LiHoF₄ is a physical realization of the quantum Ising model, with the additional features that the dominant coupling between spins is the long range dipolar interaction, and each electronic spin is strongly coupled to a nuclear degree of freedom. These nuclear degrees of freedom constitute a spin bath environment acting on the system. In this thesis, we present an effective low temperature Hamiltonian for LiHoF₄ that incorporates both these features, and we analyze the effects of the nuclear spin bath on the system. We find the lowest energy crystal field excitation in the system is gapped at the quantum critical point by the presence of the nuclear spins, with spectral weight being transferred down to a lower energy electronuclear mode that fully softens to zero at the quantum critical point. Furthermore, we present a toy model, the spin half spin half model, that illustrates the effects of an anisotropic hyperfine interaction on a quantum Ising system. We find the critical transverse field is increased when the longitudinal hyperfine coupling is dominant, as well as an enhancement of both the longitudinal electronic susceptibility and an applied longitudinal field. In addition, we present a field theoretic formalism for incorporating the effects of fluctuations beyond the random phase approximation in general quantum Ising systems. We find that any regular on site interaction, such as a nuclear spin bath, does not fundamentally alter the critical properties of a quantum Ising system. This formalism is used to calculate corrections to the magnetization of LiHoF₄.
We consider a long-range Ising antiferromagnet put in a transverse field (LRTIAF) with disorder. We have obtained the phase diagrams for both the classical and quantum cases. For the pure case applying quantum Monte Carlo method, we study the variation in order parameter (spin correlation in the Trotter direction), susceptibility, and average energy of the system for various values of the transverse field at different temperatures. The antiferromagnetic order is seen to get immediately broken as soon as the thermal or quantum fluctuations are added. We discuss generally the phase diagram for the same LRTIAF model with perturbative Sherrington-Kirkpatrick-type disorder. We find that while the antiferromagnetic order is immediately broken as one adds an infinitesimal transverse field or thermal fluctuation to the pure LRTIAF system, an infinitesimal SK spin-glass disorder is enough to induce a stable glass order in the LRTIAF. This glass order eventually gets destroyed as the thermal or quantum fluctuations are increased beyond their threshold values and the transition to paramagnetic phase occurs. Analytical studies for the phase transitions are discussed in details in each case. These transitions have been confirmed by applying classical and quantum Monte Carlo methods. We show here that the disordered LRTIAF has a surrogate incubation property of the SK spin glass phase.
The Ising model in transverse magnetic field is perhaps the simplest quantum spin model, yet the elements of site disorder, random magnetic fields, and tunable quantum fluctuations permit a rich array of ground states, and the rare ability to emphasize their classical or quantum character. We briefly review in this chapter experimental results from chains to crystals of spins, with magnetic, glassy, and spin liquid ground states. Singlet Ground State Magnets In a crystalline lattice, the crystal fields often take a form such that the ground states of magnetic ions are singlets separated from the higher lying spin multiplets. Sufficiently strong magnetic dipolar or exchange couplings between different sites can mix the singlets with the multiplets enough so as to induce non-zero expectation values for the magnetic dipoles at individual sites. Examples of this phenomenon are generally found among metals and insulators based on rare earths. Such metals were a subject of extensive research in the 1960's and 1970's, and the book by MacKintosh and Jensen [408] gives an excellent account of both the data as well as mean field approaches. With respect to insulating materials, LiTbF 4 emerged as a model system in the 1970's. It is an example of an ideal Ising dipolar coupled ferromagnet; here the long-range nature of the dipolar interactions leads to an upper critical dimension [149] (at which mean field theory with logarithmic corrections calculable using RG methods becomes an exact description of thermal phase transitions) of three rather than four. LiTbF 4 belongs to the LiREF 4 isostructural series of ionic salts. Li and F carry valences +1 and −1 respectively, leaving RE, which can be any rare earth atom or the nonmagnetic element Y, with a valence of +3. Figure 14.1 shows the body-centered tetragonal crystal structure for the family.