We study how sharp signatures of fractionalization emerge in nonlinear spectroscopy experiments on spin liquids with separated energy scales. Our model is that of dipolar-octupolar rare earth pyrochlore materials, prime candidates for realizing quantum spin ice. This family of three-dimensional quantum spin liquids exhibits fractionalization of spin degrees of freedom into spinons charged under an emergent U(1) gauge field. We show that the technique of two-dimensional coherent spectroscopy can identify clear signatures of fractionalized spinon dynamics in dipolar-octupolar quantum spin ices. However, at intermediate temperatures, spinon dynamics are heavily constrained in the presence of an incoherent spin background, leading to a broad two-dimensional coherent spectroscopy response. At lower temperatures, a sharp signal emerges as the system enters a coherent spin liquid state. This lower temperature signal can in turn distinguish between zero-flux and π-flux forms of quantum spin ice.
The presence of multiple competing interactions in spin systems can lead to novel phases known as quantum spin liquids (QSLs). QSLs are disordered spin systems with long-range entanglement that realize the deconfined phase of emergent lattice gauge theories and host fractional excitations. A notable example of great experimental interest is quantum spin ice (QSI), a three-dimensional QSL that realizes an analog of quantum electrodynamics with emergent photons and interacting electric and magnetic charges. The current leading candidate materials for realizing QSI are dipolar-octupolar (DO) cerium-based pyrochlore compounds. These are believed to stabilize a
U(1) QSL known as
π-flux QSI, where translation symmetry acting on spinon excitations fractionalizes. In this thesis, we explore the physics of QSI, relying heavily on parton constructions, to make experimentally relevant predictions for DO materials. First, we explore the physics of symmetry fractionalization in QSI, whereby lattice symmetries are realized projectively when acting on fractional quasiparticles. Symmetry fractionalization is examined within the framework of gauge mean-field theory (GMFT), a parton construction designed explicitly for application to QSI. This study shows that the pyrochlore lattice space group strongly constrains possible symmetry fractionalization classes. It systematically explains how all space group transformations, beyond translation, fractionalize in
π-flux QSI. Next, we apply this framework to DO materials and show how the equal-time structure factor predicted for
π-flux QSI is consistent with recent energy-integrated inelastic neutron scattering experiments on certain candidate materials. We also predict that the dynamical spin structure factor of
π-flux QSI is characterized by a broad continuum with three distinctive peaks of decreasing intensity that are approximately equally spaced. We argue that these peaks should be accessible with currently available experimental apparatus and offer a smoking-gun signature of
π-flux QSI. We confirm those predictions by extending the exclusive boson representation and speculate on the thermodynamic behavior of cerium candidates. We close by commenting on recent experimental breakthroughs and possible future directions.
Motivated by the rapid experimental progress of quantum spin ice materials, we study the dynamical properties of pyrochlore spin ice in the U(1) spin liquid phases. In particular, we focus on the spinon excitations that appear at high energies and show up as an excitation continuum in the dynamic spin structure factor. The keen connection between the crystal symmetry fractionalization of the spinons and the spectral periodicity of the spinon continuum is emphasized and explicitly demonstrated. When the spinon experiences a background $\ensuremath{\pi}$ flux and the spinon continuum exhibits an enhanced spectral periodicity with a folded Brillouin zone, this spectral property can then be used to detect the spin quantum number fractionalization and U(1) spin liquid. Our prediction can be immediately examined by inelastic neutron-scattering experiments among quantum spin ice materials with Kramers' doublets. Further application to the non-Kramers' doublets is discussed.
We study the uniform
U(1) quantum spin liquid (QSL) with low-energy fermionic quasiparticles for pyrochlore magnets with dipolar-octupolar symmetry, employing a fermionic parton mean-field theory approach. Self-consistent calculations stabilize 12 fully symmetric uniform
U(1) QSLs, of which four mean-field states are ``monopole-flux'' states. Several of these mean-field states show a linear temperature dependence of specific heat at low temperatures, the other phases show a power-law temperature dependence of specific heat $C\ensuremath{\sim}{T}^{\ensuremath{\alpha}}$. The linear temperature dependence of specific heat at low temperatures is reminiscent of the observations in
Nd2ScNbO7. We further compute the dynamic spin structure factors and discuss the possible signature of these fermionic spinons in neutron-scattering experiments.
Unambiguous identification of fractionalized excitations in quantum spin liquids has been a long-standing issue in correlated topological phases. Conventional spectroscopic probes, such as the dynamical spin structure factor, can only detect composites of fractionalized excitations, leading to a broad continuum in energy. Lacking a clear signature in conventional probes has been the biggest obstacle in the field. In this work, we theoretically investigate what kinds of distinctive signatures of fractionalized excitations can be probed in two-dimensional nonlinear spectroscopy by considering the exactly solvable Kitaev spin liquids. We demonstrate the existence of a number of salient features of the Majorana fermions and fluxes in two-dimensional nonlinear spectroscopy, which provide crucial information about such excitations.
We study the quantum spin dynamics of a frustrated XXZ model on a pyrochlore lattice by using large-scale quantum Monte Carlo simulation and stochastic analytic continuation. In the low-temperature quantum spin ice regime, we observe signatures of coherent photon and spinon excitations in the dynamic spin structure factor. As the temperature rises to the classical spin ice regime, the photon disappears from the dynamic spin structure factor, whereas the dynamics of the spinon remain coherent in a broad temperature window. Our results provide experimentally relevant, quantitative information for the ongoing pursuit of quantum spin ice materials.
Frustrated spin-ice systems support emergent gauge fields and fractionalized quasiparticles that act as magnetic monopoles. Although artificial platforms have enabled their direct visualization, access to their quantum-coherent dynamics has remained limited. Here we realize a programmable dipolar square spin-ice model using a superconducting-qubit quantum annealer, providing access to a previously unexplored quantum-coherent regime of artificial spin ice. By implementing a direct one-to-one mapping between lattice spins and physical qubits, together with engineered extended couplings, we realize effective dipolar interactions on frustrated lattices comprising more than 400 vertices. Tuning transverse-field fluctuations enables us to probe the real-time dynamics of Dirac-string defects and interacting monopole plasmas. We observe super-diffusive monopole transport, with scaling exponents intermediate between classical diffusion and ballistic motion, indicating dynamics beyond classical stochastic relaxation and consistent with coherent propagation within an emergent gauge manifold. These results establish programmable quantum spin ice as a scalable platform for investigating fractionalized excitations and emergent gauge dynamics in engineered quantum matter.