The langasites are a class of geometrically frustrated compounds with the formula A3XY3Z2O14 where A,X,Y,Z are cationic sites and site A is occupied by a magnetic ion. The interactions of the magnetic ions form a star shaped pattern called the Kagomé lattice. The langasites have been widely studied by the solid state community because of their functional properties such as piezoelectricity, multiferroicity, ferroelectricity, dielectricity and for use in the telecommunication industry. It was also realized that some langasite materials exhibit exotic magnetic ground states at low temperatures. A thorough understanding of their ground state is limited by the difficulty in synthesizing new members belonging to this series due to the formation of competing phases such as the garnets. In this study, four new magnetic langasites A3Ga3Ge2BeO14 (A= Pr, Nd, Sm and Eu) and a non-magnetic lattice standard La3Ga3Ge2BeO14 were synthesized. These were further structurally characterized by powder X-ray diffraction, Rietveld refinement and bond valence analysis. Further characterization of the low-temperature magnetism was done by performing magnetization, magnetic susceptibility (field cooled and zero field cooled) and heat capacity measurements. The low temperature spin dynamics were probed using muon spin resonance performed at TRIUMF (Vancouver) and elastic and inelastic neutron scattering measurements performed at the DCS (NIST) and D7 (ILL). From all the above measurements it can be concluded that the new Be langasites exhibit net antiferromagnetic interactions at low-temperatures with clear signs of diffuse scattering for Nd3Ga3Ge2BeO14 using inelastic neutron scattering measurements. There was no evidence of magnetic long-range ordering down to as low as 0.025 K. Based on the obtained measurements these new Be-langasite compounds can be classified as potential spin liquid candidates. / February 2017

Thesis advisor: Stephen D. Wilson / Spin-orbit intertwined order gives rise to many novel phenomena with a broad phase space spanned by the competing energy scales within a system. This dissertation synthesized and studied two such systems demonstrating different manifestations of spin-orbit interactions, originating from orbital degeneracy effects, on geometrically frustrated magnetic lattices. Firstly, strong spin-orbit coupling in the hyperkagome lattice, Na4Ir3O8, and secondly, the layered material, α-NaMnO2, where single-ion anisotropy and a cooperative Jahn-Teller distortion drive magnetism to the quasi-1D limit. The magnetic ground state of the Jeff = 1/2 spin-liquid candidate, Na4Ir3O8, is explored via combined bulk magnetization, muon spin relaxation, and neutron scattering measurements. A short-range, frozen, state comprised of quasi-static moments develops below a characteristic temperature of TF = 6 K, revealing an inhomogeneous distribution of spins occupying the entirety of the sample volume. Quasi-static, short-range, spin correlations persist until at least 20 mK and differ substantially from the nominally dynamic response of a quantum spin liquid. Much of this dissertation focuses on the second spin-orbit intertwined system, α-NaMnO2, where a cooperative Jahn-Teller distortion of the MnO6 octahedra arising from an orbital degeneracy in the Mn3+ cations directly affects the electronic (ferro-orbital) and magnetic (antiferromagnetic) order, which results in an intriguing study of low-dimensional magnetism. Intricacies of the structure, static magnetic order, and magnon dynamics are presented, which heavily relied on neutron scattering techniques. In particular, a longitudinally polarized bound magnon mode is characterized through the use of polarized neutron scattering. / Thesis (PhD) — Boston College, 2018. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.

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.

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.

This thesis will present research that studies the role of disorder, geometric frustration and the long range dipolar interaction on the collective behaviour of several insulating, rare earth magnets. Experiments were performed at low temperatures to measure the specific heat and magnetic susceptibility of several materials. Susceptibility was measured with a SQUID magnetometer that has been designed and constructed primarily for the study of slow dynamics in glassy systems. Specifically, this thesis will discuss three distinct topics. The first is the series of materials LiHo(x)Y(1-x)F(4), which are manifestations of the dilute, dipolar coupled Ising model. The low-x portion of the phase diagram has become a rather contentious issue in recent years with both theoretical and experimental groups disagreeing on the existence of a spin glass freezing transition and one experimental group arguing for the existence of an exotic "antiglass'' or spin liquid state resulting from quantum entanglement at x=0.045. We present specific heat and dynamical susceptibility measurements on four stoichiometries in this series: x = 0.018, 0.045, 0.080 and 0.012. No evidence of an unusual antiglass state is observed. Instead, our results show evidence, at all dilution levels studied, of a spin glass freezing transition. Interpretation of experimental data is found to be complicated by the anomalously slow dynamics in these materials. The relaxation time scales are found to increase as the concentration of Ho(3+) ions is reduced, an effect which can be attributed to single-ion physics and the importance of the nuclear hyperfine coupling in this system. A second set of materials studied here is a series of several Gd garnet materials, the most famous of which is Gd(3)Ga(5)O(12) (GGG), a material previously argued to be a disorder-free spin glass. Our specific heat experiments reproduce previous experiments on GGG and show that the homologous Gd garnets Gd(3)Te(2)Li(3)O(12) and Ga(3)Al(5)O(12) do not share the same glassy physics but exhibit sharp ordering features. By experimenting with the introduction of random site dilution, it is concluded that a 1-2% off-stoichiometry inherent in GGG is likely a special kind of disorder that is particularly effective in inducing random frustration and the formation of a spin glass. Finally, specific heat measurements on the pyrochlore antiferromagnet Gd(2)Sn(2)O(7) (GSO) are presented. While GSO has generally been found to be a well behaved and well understood model magnet, with long range order developing at around 1 K, like many other geometrically frustrated magnets, it has been discovered to possess persistent spin dynamics down to very low temperatures as measured by μSR and Mössbauer spectroscopy. Measurement of the low temperature limit of the specific heat when compared with linear spin-wave theory, however, presents a consistent picture of gapped magnon excitations that freeze out at low temperatures and make the existence of the proposed dynamic ground state unlikely.

This thesis will present research that studies the role of disorder, geometric frustration and the long range dipolar interaction on the collective behaviour of several insulating, rare earth magnets. Experiments were performed at low temperatures to measure the specific heat and magnetic susceptibility of several materials. Susceptibility was measured with a SQUID magnetometer that has been designed and constructed primarily for the study of slow dynamics in glassy systems. Specifically, this thesis will discuss three distinct topics. The first is the series of materials LiHo(x)Y(1-x)F(4), which are manifestations of the dilute, dipolar coupled Ising model. The low-x portion of the phase diagram has become a rather contentious issue in recent years with both theoretical and experimental groups disagreeing on the existence of a spin glass freezing transition and one experimental group arguing for the existence of an exotic "antiglass'' or spin liquid state resulting from quantum entanglement at x=0.045. We present specific heat and dynamical susceptibility measurements on four stoichiometries in this series: x = 0.018, 0.045, 0.080 and 0.012. No evidence of an unusual antiglass state is observed. Instead, our results show evidence, at all dilution levels studied, of a spin glass freezing transition. Interpretation of experimental data is found to be complicated by the anomalously slow dynamics in these materials. The relaxation time scales are found to increase as the concentration of Ho(3+) ions is reduced, an effect which can be attributed to single-ion physics and the importance of the nuclear hyperfine coupling in this system. A second set of materials studied here is a series of several Gd garnet materials, the most famous of which is Gd(3)Ga(5)O(12) (GGG), a material previously argued to be a disorder-free spin glass. Our specific heat experiments reproduce previous experiments on GGG and show that the homologous Gd garnets Gd(3)Te(2)Li(3)O(12) and Ga(3)Al(5)O(12) do not share the same glassy physics but exhibit sharp ordering features. By experimenting with the introduction of random site dilution, it is concluded that a 1-2% off-stoichiometry inherent in GGG is likely a special kind of disorder that is particularly effective in inducing random frustration and the formation of a spin glass. Finally, specific heat measurements on the pyrochlore antiferromagnet Gd(2)Sn(2)O(7) (GSO) are presented. While GSO has generally been found to be a well behaved and well understood model magnet, with long range order developing at around 1 K, like many other geometrically frustrated magnets, it has been discovered to possess persistent spin dynamics down to very low temperatures as measured by μSR and Mössbauer spectroscopy. Measurement of the low temperature limit of the specific heat when compared with linear spin-wave theory, however, presents a consistent picture of gapped magnon excitations that freeze out at low temperatures and make the existence of the proposed dynamic ground state unlikely.

LnBaCo2O5+δ (Ln-112) where Ln = lanthanide element; 0 ≤ δ ≤1 and LnBaCo4O7+δ (Ln-114) are highly correlated cobalt oxides. Synchrotron photoemission spectroscopy of LnBaCo2O5+δ (Ln = Gd, Dy, Dy1-xTbx) and LnBaCo4O7 (Ln = Yb) has been undertaken at the UK Synchrotron Radiation Source (Daresbury Laboratory).During the photoemission experiments, the samples were observed to be contaminated due to residual gases inside the main vacuum chamber. The surface degradation of the samples is studied using the difference spectra generated from the valence band spectra of freshly scraped and contaminated samples and the nature of contaminated species on these samples is identified in the light of the reviewed literature. High-resolution photoemission is carried out to study the metal-insulator (MI) transition in double perovskites LnBaCo2O5+δ (Ln = Gd, Dy, Dy1-xTbx - Ln-112; 0 ≤ δ ≤ 1) as a function of temperature. The high-resolution photoemission results of single crystal samples of GdBaCo2O5.5, DyBaCo2O5.5 and Dy1-xTbxBaCo2O5+δ show that the temperature-based MI transitions in these compounds occur in the 300-400 K temperature range. A post-growth oxygen annealing treatment for as-grown single crystals of Ln-112 is necessary, achieving oxygen contents close to 5.50, to observe a marked nonmetal-to-metal transition. Resonant photoemission is used to identify the atomic parentage of the valence band states. A comparison of the electronic structure of LnBaCo2O5+δ (Ln = Gd, Dy, Dy1-xTbx - Ln-112; 0 ≤ δ ≤ 1) and LnBaCo4O7 (Ln = Yb - Ln-114) single-crystal surfaces is made using synchrotron photoemission spectroscopy. In both cases, the states close to the Fermi energy are found to be of mixed Co 3d/O 2p character, and the comparison allows identification of states due to low spin Co³⁺ in octahedral environments. The contributions from Ln elements to the valence band are found at higher binding energies.

The thermodynamics of disorder have been studied for hundreds of years, with physicists using entropy to quantitatively connect the macroscopic properties of a system to its microscopic multiplicity (disorder). Here, we consider the effect of disorder in magnetic materials. The pyrochlore oxides (A2B2O7), comprised of a bipartite lattice of corner-sharing tetrahedra, have been central to the study of geometric frustration for the past several decades. Pyrochlores, in which the A-site is occupied by the magnetic cation dysprosium, tend to exhibit spin ice ordering down to low temperatures, in spite of chemical perturbations to the B-site lattice. With the motivation of this study being the investigation of how adding B-site disorder to the traditional Dy2ScNbO7 form of Dy-pyrochlores, a stoichiometric mixture of Sc-3+ and Nb-5+ was used to synthesize Dy2ScNbO7, the pyrochlore material that is central to this thesis work. We show using magnetometry, heat capacity, muon spin relaxation, and inelastic neutron scattering that the mixed B-site pyrochlore Dy2ScNbO7, does not adopt the spin ice ground state. The low temperature spin dynamics are much faster than other analogous dysprosium pyrochlores, the residual entropy is significantly smaller than that predicted for a spin ice and there are low-lying crystal field excitations. These results all indicate that the B-site disorder appears to destroy the predicted Ising anisotropy of dysprosium. / Thesis / Master of Science (MSc)

<p>Yb2Ti2O7 is one member of a series of magnetic compounds with the pyrochlore lattice structure. For specific types of single-ion anisotropy and exchange interactions, the geometry of the pyrochlore lattice frustrates near-neighbor interactions and coaxes a wide variety of unusual magnetic ground states from such compounds. Yb2Ti2O7 is unique among these compounds in that the source of the frustration is not immediately obvious when one considers the combination of single-ion anisotropy (XY-like) and the nature of the exchange interactions (ferromagnetic) present therein. A conventional magnetic transition was indeed initially expected based on the observation of specific heat anomaly near 200mK. However, many studies produced no signs of long-range magnetic order below this temperature. Intriguingly, above the transition, evidence for unusual two-dimensional correlations came in the form of rods of magnetic diffuse neutron scattering. This thesis contains four articles that detail the results of several neutron scattering studies on Yb2Ti2O7. The goal of these studies was to determine the nature of the static and dynamic spin correlations throughout the magnetic field vs. temperature phase diagram of Yb2Ti2O7.</p> <p>We first performed a time-of-flight neutron scattering experiment on a single crystal of Yb2Ti2O7, which we prepared using the optical floating zone method. This initial study provided a comprehensive survey of the phase diagram, including the previously unexplored response to a magnetic field. We found that the rods of diffuse scattering change qualitatively upon cooling below the temperature of the reported specific heat anomaly, showing signs for the development of short-range three-dimensional correlations. Additionally, we discovered that a relatively small magnetic field applied along the [110] direction could remove the diffuse scattering entirely, and produce sharp spin wave excitations in the inelastic channel, indicating long range spin correlations.</p> <p>We further quantified the temperature dependence of the diffuse scattering in zero-field using a triple-axis neutron spectrometer. The crossover from two-dimensional correlations to short-range three-dimensional correlations was found to begin at 400mK and reach completion near the temperature of the specific heat anomaly, ∼200mK. Our measurements of the low temperature specific heat of several single crystal samples, as well as a powder sample, revealed that significant sample-dependence of the magnetic properties exists. The single crystal samples were shown to have broader features in the specific heat at relatively low temperatures compared to the powder samples, pointing to some amount of structural disorder in the single crystals.</p> <p>To understand the nature of the structural defects in the single crystals, we compared the structure of a crushed single crystal of Yb2Ti2O7 to that of a powder sample using neutron powder diffraction. The major conclusion of that work was that the single crystal is non-stoichiometric, containing 2.3% excess ytterbium on the (non-magnetic) titanium sublattice. The introduction of additional magnetic moments into the system is expected to be the cause of the sample-dependence of the specific heat anomaly.</p> <p>Finally, we fit the spin wave dispersions in the field-polarized state, as measured by time-of-flight inelastic neutron scattering, to an effective spin-1/2 anisotropic exchange Hamiltonian. The microscopic parameters extracted from these fits place Yb2Ti2O7 close to exotic Quantum Spin Liquid phases predicted for the anisotropic spin-1/2 pryochlore model. The exchange parameters also reveal that the source of the frustration in Yb2Ti2O7 comes from the “quantum spin ice” nature of its exchange interactions.</p> / Doctor of Philosophy (PhD)

<p>The following dissertation presents neutron scattering studies on three specific magnetic insulating oxide materials whose lattice is based on triangular structural motifs. Each of the three materials studied, LuCoGaO₄, Co₃V₂O₈ and Tb₂Ti₂O₇, displays an interesting disordered ground state that is reached by different mechanisms: site disorder, geometric frustration, and quantum fluctuations induced by a transverse magnetic field. The main focus of this work is the characterization of the resulting magnetic ground states and magnetic excitations within these systems.</p> <p>Chapters 3, 4 and 5 contain original work in the form of six research articles that have either been published or have been prepared for publication in peer-reviewed journals.</p> <p>Chapter 3 describes studies of the quasi two-dimensional triangular layered antiferromagnet LuCoGaO₄. This material is found to exhibit a spin glass ground state as a result of geometrical frustration and site disorder inherent in this system. Below the freezing temperature, this system exhibits static, two-dimensional correlations consistent with frozen short-range correlated regions in the plane of the bilayers that extend over roughly five unit cells. The dynamic correlations reveal typical spin glass behavior upon cooling. Furthermore, a resonant gapped spin-wave-like excitation is observed, that can be related to the anisotropy in the system. Such an excitation is relatively uncommon in spin glasses and has been studied for the first time in such detail.</p> <p>Chapter 4 is concerned with the study of the kagome staircase system Co₃V₂O₈. While prone to geometrical frustration due to its underlying kagome structural motif, this material is characterized by predominantly ferromagnetic interactions that lead to an unfrustrated, ferromagnetic ground state. In this chapter, departures from this conventional ground state by different disordering mechanisms are investigated. The first part focuses on the effects of site disorder by introducing quenched nonmagnetic impurities into the system. The growth of single crystals of (Co_1-xMg_x)₃V₂O₈ is reported. These crystals reveal that the ferromagnetic ground state is very sensitive to doping, and show that a low doping concentration of 19% leads to a suppression of the ferromagnetic ground state below 1.5 K. This could be understood as percolation problem on the quasi two-dimensional kagome lattice including site and bond percolation. The second part focuses on the influence of a transverse magnetic field on the ground state of Ising spins, introducing quantum fluctuations that lead to quantum phase transitions at ~6.25, 7 and 13 T. The observed quantum phase transitions are characterized by distinct changes in the magnetic structure and their associated spin excitation spectra.</p> <p>Chapter 5 presents studies on the pyrochlore antiferromagnet Tb₂Ti₂O₇, which is a proposed spin liquid candidate but whose actual ground state is still the topic of current debate. The ground state of Tb₂Ti₂O₇ was revisited by neutron scattering measurements, revealing a new phase in the low temperature low field phase diagram that can be described as a frozen antiferromagnetic spin ice that exhibits distinct elastic and inelastic scattering features.</p> / Doctor of Philosophy (PhD)