Minimizing the energy of a many body system tends to favor order, but classical frustration and quantum fluctuations destabilize that order. The tension between these effects can produce exotic quantum states of matter. Quantum spin liquid (QSL) states emerge in models of localized magnetic moments where the crystal lattice connectivity frustrates ordering, and the exchange interaction of neighboring spins strengthens quantum fluctuations. Experimentally identifying a QSL in a real material is challenging from the lack of an order parameter. Piecing together evidence from varied techniques is necessary for diagnosing the nature of the ground state -- QSL or otherwise -- of a frustrated spin system. In this work, we use coplanar superconducting resonators to probe magnetic excitations in epitaxially grown thin films of a spin liquid candidate TbInO3. Adapting microwave techniques from the field of circuit quantum electrodynamics, we measure responses of these thin films whose volume is too low for applying conventional bulk techniques. In-plane susceptibility extracted from the spin resonance signal indicates extreme frustration of magnetic order down to 20 mK, over two orders of magnitude lower than the Curie-Weiss energy scale. Through a crystal field analysis, we identify the doublet eigenstates comprising the ground state. As a consequence of improper ferroelectricity, Tb moments split into two flavors with distinct g-factors reflecting the local crystal field environment of each site. Spin-orbit coupling, crystal fields, magnetic frustration and improper ferroelectricity distinctively combine to shape the magnetic ground state of TbInO3. This work establishes a measurement technique using superconducting resonators to probe thin films of frustrated magnets, and applies this technique towards building a coherent understanding of the magnetic properties of TbInO3.
Minimizing the energy of a many body system tends to favor order, but classical frustration and quantum fluctuations destabilize that order. The tension between these effects can produce exotic quantum states of matter. Quantum spin liquid (QSL) states emerge in models of localized magnetic moments where the crystal lattice connectivity frustrates ordering, and the exchange interaction of neighboring spins strengthens quantum fluctuations. Experimentally identifying a QSL in a real material is challenging from the lack of an order parameter. Piecing together evidence from varied techniques is necessary for diagnosing the nature of the ground state -- QSL or otherwise -- of a frustrated spin system. In this work, we use coplanar superconducting resonators to probe magnetic excitations in epitaxially grown thin films of a spin liquid candidate TbInO3. Adapting microwave techniques from the field of circuit quantum electrodynamics, we measure responses of these thin films whose volume is too low for applying conventional bulk techniques. In-plane susceptibility extracted from the spin resonance signal indicates extreme frustration of magnetic order down to 20 mK, over two orders of magnitude lower than the Curie-Weiss energy scale. Through a crystal field analysis, we identify the doublet eigenstates comprising the ground state. As a consequence of improper ferroelectricity, Tb moments split into two flavors with distinct g-factors reflecting the local crystal field environment of each site. Spin-orbit coupling, crystal fields, magnetic frustration and improper ferroelectricity distinctively combine to shape the magnetic ground state of TbInO3. This work establishes a measurement technique using superconducting resonators to probe thin films of frustrated magnets, and applies this technique towards building a coherent understanding of the magnetic properties of TbInO3.
The quantum nature of electrons emerges in various exotic ways when they are put together with quantum many-body interactions. In Mott insulating systems with strong electron correlation, frustration and strong quantum fluctuations promote localized electron spins to form nontrivial quantum paramagnetic phases such as quantum spin liquid and valence bond solid preventing the development of conventional magnetic orders. In this thesis, we study such exotic quantum phases in various different frustrated quantum magnets. First, encouraged by the spin liquid phenomenology observed in Ba3XSb2O9 (X=Cu, Ni), we investigate Z2 spin liquids on a three dimensional triangular lattice by employing the Schwinger boson mean-field theory with projective symmetry group analysis. It is found that a nematic spin liquid is energetically favorable on this lattice structure rather than symmetric spin liquids. Next, we study various valence bond solid phases that can appear in kagome lattice antiferromagnets by generalizing the recently proposed phenomenological Z2 gauge theory for the topological Z2 spin liquid state found in the nearest-neighbor kagome lattice Heisenberg model. This work provides a bridge between the topological spin liquid and valence bond solid phases previously proposed for kagome lattice antiferromagnets via vison condensation in the gauge theory. Then, we consider optical conductivity in Mott insulators as an experimental probe to detect quantum paramagnetic phases like valence bond solid. Applying this idea to deformed kagome lattice antiferromagnet Rb2Cu3SnF12 with a 12-site valence bond solid state, we estimate the size of optical conductivity in this quantum magnet. After this, another quantum paramagnet BiCu2PO6 is carefully investigated to clarify its puzzling ground state nature and quasiparticle excitations. Utilizing recent high resolution neutron scattering data, we construct a microscopic spin model and also an effective theory for the low energy spin excitations in the compound. We find significant influences of magnetic anisotropies on the ground state and quasiparticle dynamics. Lastly, we investigate emergent quantum phases in the thin film geometries of the pyrochlore iridates, where a number of exotic quantum ground states are proposed to occur in bulk materials as a result of the interplay between electron correlation and strong spin-orbit coupling. The fate of these bulk phases, as well as the novel quantum states that may arise only in a thin film setting, are studied via a theoretical model that allows layer-dependent magnetic structures.
Frustrated magnetism provides a rich platform for realizing exotic quantum phases in condensed matter systems. Among these, quantum spin liquids (QSLs) are a particularly intriguing class of states that exhibit no magnetic ordering and preserve all symmetries down to zero temperature. Just as conventional magnets can be thought of as spin crystals,QSLs represent their liquid analogs. This thesis explores two broad types of QSLs in two-dimensional magnets, with a focus on their dynamic properties and the nature of transitions from conventional magnetic states into QSL phases. QSLs are topological phases that host fractionalized excitations known as spinons. In these states, mobile spinons are coupled to an emergent gauge field, forming a highly entangled phase of matter. The first part of this thesis focuses on Dirac spin liquids (DSLs), a class of QSLs where spinons exhibit a gapless Dirac dispersion. To study the dynamicsof these spin liquids beyond leading-order mean-field theory, we develop a novel large-N fermionic limit of gapless spinons. In this limit, all gauge excitations are suppressed, and the leading-order corrections instead arise from order parameter fluctuations, which may condense and drive transitions into symmetry-broken phases from the parent DSL. Incorporating random phase approximation (RPA) corrections to the spin susceptibility, we find that sharp, spin-wave–like modes are recovered in the excitation spectrum. This methodology successfully captures characteristic features of the dynamics near phase transitions and in weakly symmetry-broken phases proximate to a DSL. We apply this approach to microscopic models, including the J1-J2 XXZ model on the triangular lattice and the J1-J3 XXZ model on the honeycomb lattice. These models closely represent a wide range of frustrated materials, such as triangular and honeycomb cobaltates and triangular ytterbium compounds. Our theoretical predictions show excellent agreement with experimentally measured inelastic neutron scattering spectra from these materials. Gapless spinons can also sometimes become gapped through chiral symmetry breaking, leading to the formation of a chiral spin liquid (CSL). The CSL is an archetypal bosonic realization of a fractional quantum Hall (FQH) state at half-filling, and has been proposed as a time-reversal–breaking ground state in a variety of frustrated spin models. The second part of this thesis addresses the intriguing possibility of realizing a CSL through the "melting" of a chiral spin crystal—a conventional magnet with non-coplanar ordering. Such a transition offers a physically appealing analogue to the melting of a Wigner crystal into a fermionic FQH liquid. Focusing on the kagome lattice, where chiral interactions are knownto stabilize a CSL ground state, we study the effects of additional long-range Heisenberg interactions and demonstrate a phase transition into a non-coplanar octahedral magnetic order. To describe the universal class of transition between a CSL and a non-coplanar anti-ferromagnetic order, we then develop a novel Chern-Simons–matter field theory framework, constrained by symmetry principles and symmetry fractionalization patterns. This thesis thus provides new insights into the dynamical signatures and phase transitions of quantum spin liquids, offering a bridge between theoretical models and experimental observations in frustrated magnetic systems.
In frustrated magnets, the experimental realization of a quantum disordered ground state (QDGS), especially quantum spin liquid (QSL) ground state, is a central topic in condensed matter physics.Several promising candidates were reported, and a number of QSL-like behavior, such as excitation continuum, Tlinear specific heat, and so on, were observed.However, whether the QSL-like behavior is owing to the synergy between spin frustration and quantum fluctuation or bond randomness effects has not been clarified yet.Several theoretical studies have demonstrated that the synergy effect between the magnetic frustration and the bond randomness suppresses magnetic ordering and induces a QSL-like state.This QSL-like state was proposed to be a random-singlet (RS) state, where not only nearest-neighbor spins but also distant spins form singlet pairs with random coupling energy.Since thermodynamic properties of RS and QSL are predicted to be similar to each other, it is important to elucidate the microscopic nature of randomness-induced QDGSs.However, its experimental verifications are still insufficient due to a lack of model materials.In this work, I synthesized polycrystalline samples of SrLaCuSbO 6 (SLCSO) and SrLaCuNbO 6 (SLCNO) by a solid-state reaction.Magnetic Cu 2+ ions with S = 1/2 Heisenberg spins form a square lattice with nearest-neighbor (J 1 ) and next-nearest-neighbor (J 2 ) exchange interaction.Thus, SLCSO and SLCNO were magnetically described as quasi-two-dimensional S = 1/2 J 1 -J 2 square lattice Heisenberg antiferromagnet (SLHAF).The temperature dependence of the magnetic susceptibilities of both compounds shows a broad maximum characteristic of an S = 1/2 SLHAF.However, both compounds undergo magnetic phase transitions at T N = 13.6 and 15.7 K for SLCSO and SLCNO, respectively, due to weak inter-layer interactions.Neutron powder diffraction measurements reveal contrasting spin structures in both compounds.The spin structures of SLCSO and SLCNO below T N are Néel antiferromagnetic and collinear antiferromagnetic, respectively.This result demonstrates that the nearest-neighbor interaction is dominant in SLCSO, whereas the next-nearest-neighbor interaction is dominant in SLCNO.The magnitude of the ordered moment was evaluated at 3.5 K to be m = 0.39(3) µ B for SLCSO and 0.37(1) µ B for SLCNO, which are significantly reduced from 1µ B expected in the classical spin case.The shrink of the ordered magnetic moment was caused by not only magnetic frustration effects but also bond randomness effects arising from the site disorder of Sr 2+ and La 3+ ions.Next, I synthesized the mixed system SrLaCuSb 1-x Nb x O 6 with 0.1 ≤ x ≤
The search for exotic states of matter continues to be a central theme in condensed matter physics. Among these, quantum spin liquids (QSLs) represent a profound challenge and opportunity, characterized by long-range entanglement and fractionalized excitations without conventional magnetic order even at absolute zero temperature. Frustrated quantum magnets are prime candidates for hosting such states, where competing interactions prevent classical ground states. This paper reports the theoretical and experimental signatures that would lead to the discovery of a chiral bosonic liquid (CBL) in a novel frustrated quantum magnet. A CBL is a particularly elusive type of QSL characterized by elementary excitations that behave as bosons and exhibit a distinct chirality, manifesting as a non-zero thermal Hall effect in the absence of a magnetic field. We outline a comprehensive strategy involving advanced material synthesis, precise low-temperature thermodynamic measurements, inelastic neutron scattering, and numerical simulations to identify the unique fingerprints of this novel state. Key indicators include a gapless or nearly gapless excitation spectrum, a specific heat scaling characteristic of bosonic excitations, and, most critically, a quantized or near-quantized thermal Hall conductivity directly reflecting the chiral nature of the bosonic fractional excitations. The implications of this discovery extend to fundamental understanding of quantum entanglement, topological states of matter, and potential applications in robust quantum information processing.
Quantum spin liquids (QSLs) host emergent, fractionalized fermionic excitations that are charge-neutral. Identifying clear experimental signatures of these excitations remains a central challenge in the field of strongly correlated systems, as they do not couple to conventional electromagnetic probes. Here, we propose lattice strain as a powerful and tunable probe: Mechanical deformation of the lattice generates large pseudomagnetic fields, inducing pseudo-Landau levels that serve as distinctive spectroscopic signatures of these excitations. Using the Kitaev model on the honeycomb lattice, we show that distinct QSL phases exhibit strikingly different strain responses. The semimetallic Kitaev spin liquid and the gapped chiral spin liquid display pronounced Landau quantization and a diamagnetic-like response to strain, whereas the Majorana metal phase shows a paramagnetic-like response without forming Landau levels. These contrasting behaviors provide a direct route to experimentally identifying and distinguishing QSL phases hosting fractionalized excitations. We further outline how local resonant ultrasound spectroscopy can detect the strain-induced resonances associated with these responses, offering a practical pathway towards identifying fractionalized excitations in candidate materials.
Quantum spin liquids (QSLs) host exotic fractionalized magnetic and gauge-field excitations whose microscopic origins and experimental verification remain frustratingly elusive. In the absence of static magnetic order, the spin excitation spectrum constitutes the crucial probe of QSL behavior, but its theoretical computation is a serious challenge. Here we employ state-of-the-art tensor-network methods to obtain the full dynamical spectral function of the J1-J2 kagome Heisenberg model and benchmark our results by tracking their evolution across the magnetically ordered and QSL phases. Reducing ∣J2∣/J1 causes increasingly strong spin-wave renormalization, flattening these modes then merging them into a continuum characteristic of deconfined spinons at all finite energies in the QSL. The low-energy continuum and the occurrence of gap closure at multiple high-symmetry points identify this gapless QSL as the U(1) Dirac spin liquid. These results establish a unified understanding of spin excitations in highly frustrated quantum magnets and provide clear spectral fingerprints for experimental detection in candidate kagome QSL materials.