arXiv subjects

T. F. Rosenbaum

Publications and source records attributed to T. F. Rosenbaum.

At least 19 recordsLinked to original sources

arXiv2026

Raman magnon spectroscopy of local interactions and ground state selection in $\mathrm{Sr_2IrO_4}$

Competing and coupled spin and charge interactions in quantum materials lead to a variety of ordered states where local configurations preferentially influence the long-range order. When these interactions are finely balanced in energy, disorder and fluctuations play an outsized role. Raman scattering is particularly well-suited to revealing the underlying physics in such situations because of its sensitivity to local environments and ability to reveal overall symmetries. We perform angle-resolved Raman polarization measurements on single crystals of the correlated, layered magnet, \ce{Sr2IrO4}, where the Mott insulating ground state arises from strong spin-orbit coupling. We characterize the symmetries of both the phonon and magnon modes through comprehensive measurements in both the $ab$-plane and out-of-plane geometries from 10 to 700 cm$^{-1}$, and trace the evolution of these modes in both configurations to 12 GPa in a diamond anvil cell with perforated diamonds. Pressure does not significantly alter the lattice as the phonon modes shift linearly under compression, but at the same time the magnon modes become position dependent and spread over a range of wavenumbers. We attribute this magnetic heterogeneity to pressure-enhanced variations in the weak interlayer interactions, which may locally favor competing magnetic stacking configurations, and compare our experimental results to the predictions of linear spin wave calculations. Our results demonstrate that Raman-active magnons amplify $μ$eV-scale interactions responsible for ground-state selection into easily measurable spectral changes.

cond-mat.other↗

arXiv2026

Many-body quantum geometric effects and entanglement at the 3D metal-insulator quantum phase transition

Quantum geometry has emerged as a unifying concept across condensed matter physics, underlying phenomena from nonlinear topological response to flat-band superconductivity. While usually formulated within band theory, quantum geometry remains meaningful in disordered interacting systems~\cite{resta1999electron}. Here we show that the first negative moment of the optical conductivity -- proportional to the zero temperature quantum Fisher information as a bound on the multipartite entanglement -- provides an experimental probe of quantum geometry across the three-dimensional metal-insulator quantum phase transition in phosphorus-doped silicon. We extract a quantum geometric length $\ell$ that characterizes the local wavefunctions. Far from the transition, this length is almost coincident with the Bohr radius of the hydrogenic phosphorus donors, reflecting their atomic-scale quantum geometry. Approaching the transition, $\ell$ is enhanced, but does not diverge continuously like a correlation length; it jumps discontinuously to infinity at the critical point. This reflects the UV domination of the sum rule in three dimensions that renders it insensitive to the critical fluctuations driving the diverging dielectric constant and correlation length. Its enhancement demonstrates a ``puffing" of the donor polarizability volume of quantum geometric origin, which yields a quantum geometric corrected Clausius-Mossotti description in closer agreement with the diverging dielectric response and provides a quantum mechanical foundation for the century-old Herzfeld metallization criterion.

cond-mat.str-el↗

arXiv2025

Fermi surface origin of the low-temperature magnetoresistance anomaly

A magnetoresistance (MR) anomaly at low temperatures has been observed in a variety of systems, ranging from low-dimensional chalcogenides to spin and charge density wave (SDW/CDW) metals and, most recently, topological semimetals. In some systems parabolic magnetoresistance can rise to hundreds of thousands of times its low-temperature, zero-field value. While the origin of such a dramatic effect remains unresolved, these systems are often low-carrier-density compensated metals, and the physics is expected to be quasi-classical. Here we demonstrate that this MR anomaly in temperature also exists in high conductivity good metals with large Fermi surfaces, namely Cr, Mo, and W, for both linear and quadratic field-dependent regimes with their non-saturation attributed to open orbit and electron-hole compensation, respectively. We provide evidence that quantum transport across sharp Fermi surface arcs, but not necessarily the full cyclotron orbit, governs this low-temperature MR anomaly. In Cr, extremely sharp curvatures are induced by superposed lattice and SDW band structures. One observes an overlay of the temperature dependence of three phenomena: namely, MR at a constant high field, linear MR in the low-field limit, and Shubnikov-de Haas (SdH) oscillations of the lightest orbit. In Mo, the temperature dependence of low-T MR anomaly extends beyond those of its SdH oscillations but disappears at temperatures where Kohler's scaling reemerges. In the low-temperature and high-field limit, large magnetoresistance from carriers circling quantum orbits is the three-dimensional analogy to the zero-conductance state of carrier localization in the integer quantum Hall effect, especially with regard to the adverse effect of disorder.

cond-mat.mtrl-sci↗

arXiv2024

Four-Wave Mixing at peV Energy Scales

We measure the non-linear magnetic susceptibility $χ^{(3)}$ of the disordered quantum Ising magnet, \lihofour, and demonstrate four-wave mixing due to coherent (anti-)Stokes Raman scattering at $\sim$ 100 Hz (p$e$V) energy scales. The temperature dependence of $χ^{(3)}$ approximately follows a $\frac{1}{T}$ form, with a high-$T$ cutoff that can be linked to dissipation in the coherent spin clusters. $χ^{(3)}$ also decreases monotonically with a transverse field, approaching a constant offset above a few kOe, suggesting the presence of both coherent, and spontaneous Raman scattering.

cond-mat.str-el↗

arXiv2024

A Gallery of Soft Modes: Theory and Experiment at a Ferromagnetic Quantum Phase Transition

We examine the low-energy excitations in the vicinity of the quantum critical point in LiHoF$_4$, a physical realization of the Transverse Field Ising Model, focusing on the long-range fluctuations which soften to zero energy at the ferromagnetic quantum phase transition. Microwave spectroscopy in tunable loop-gap resonator structures identifies and characterizes the soft mode and higher-energy electronuclear states. We study these modes as a function of frequency and magnetic fields applied transverse and parallel to the Ising axis. These are understood in the context of a theoretical model of a soft electronuclear mode that interacts with soft photons as well as soft phonons. We identify competing infrared divergences at the quantum critical point, coming from the photons and the electronuclear soft mode. It is an incomplete cancellation of these divergences that leads to the muted but distinct signatures observed in the experiments. The application of a longitudinal magnetic field gaps the soft mode. Measurements well away from the quantum critical point reveal a set of ``Walker'' modes associated with ferromagnetic domain dynamics.

cond-mat.str-el↗

arXiv2023

Quantum interference in superposed lattices

Charge transport in solids at low temperature reveals a material's mesoscopic properties and structure. Under a magnetic field, Shubnikov-de Haas (SdH) oscillations inform complex quantum transport phenomena that are not limited by the ground state characteristics. Here, in elemental metal Cr with two incommensurately superposed lattices of ions and a spin-density-wave ground state, we reveal that the phases of several low-frequency SdH oscillations in sigma_xx (rho_xx) and sigma_yy (rho_yy) are opposite, contrast with oscillations from normal cyclotron orbits that maintain identical phases. We trace the origin of the low frequency SdH oscillations to quantum interference effects arising from the incommensurate orbits of Cr's superposed reciprocal lattices, and explain the observed pi-phase shift by the reconnection of anisotropic joint open and closed orbits.

cond-mat.str-el↗

arXiv2023

Quantum Barkhausen Noise Induced by Domain Wall Co-Tunneling

Most macroscopic magnetic phenomena (including magnetic hysteresis) are typically understood classically. Here, we examine the dynamics of a uniaxial rare-earth ferromagnet deep within the quantum regime, so that domain wall motion, and the associated hysteresis, is dominated by large-scale quantum tunneling of spins, rather than classical thermal activation over a potential barrier. The domain wall motion is found to exhibit avalanche dynamics, observable as an unusual form of Barkhausen noise. We observe non-critical behavior in the avalanche dynamics that only can be explained by going beyond traditional renormalization group methods or classical domain wall models. We find that this ``quantum Barkhausen noise'' exhibits two distinct mechanisms for domain wall movement, each of which is quantum-mechanical, but with very different dependences on an external magnetic field applied transverse to the spin (Ising) axis. These observations can be understood in terms of the correlated motion of pairs of domain walls, nucleated by co-tunneling of plaquettes (sections of domain wall), with plaquette pairs correlated by dipolar interactions; this correlation is suppressed by the transverse field. Similar macroscopic correlations may be expected to appear in the hysteresis of other systems with long-range interactions.

cond-mat.dis-nn↗

arXiv2022

Theory of magnon-polaritons in quantum Ising materials

We present a theory of magnon-polaritons in quantum Ising materials, and develop a formalism describing the coupling between light and matter as an Ising system is tuned through its quantum critical point. The theory is applied to Ising materials having multilevel single-site Hamiltonians, in which multiple magnon modes are present, such as the insulating Ising magnet LiHoF$_4$ . We find that the magnon-photon coupling strengths may be tuned by the applied transverse field, with the coupling between the soft mode present in the quantum Ising material and a photonic resonator mode diverging at the quantum critical point of the material. A fixed system of spins will not exhibit the diamagnetic response expected when light is coupled to mobile spins or atoms. Without the diamagnetic response, one expects a divergent magnon-photon coupling strength to lead to a superradiant quantum phase transition. However, this neglects the effects of damping and decoherence present in any real system. We show that damping and decoherence may block the superradiant quantum phase transition, and lead to weak coupling between the soft magnon mode and the resonator mode. The results of the theory are applied to experimental data on the model system LiHoF$_4$ in a microwave resonator.

cond-mat.other↗

arXiv2022

High-pressure control of optical nonlinearity in the polar Weyl semimetal TaAs

The transition metal monopnictide family of Weyl semimetals recently has been shown to exhibit anomalously strong second-order optical nonlinearity, which is theoretically attributed to a highly asymmetric polarization distribution induced by their polar structure. We experimentally test this hypothesis by measuring optical second harmonic generation (SHG) from TaAs across a pressure-tuned polar-to-nonpolar structural phase transition. Despite the high-pressure structure remaining noncentrosymmetric, the SHG yield is reduced by more than 60 % by 20 GPa as compared to the ambient pressure value. By examining the pressure dependence of distinct groups of SHG susceptibility tensor elements, we find that the yield is primarily controlled by a single element that governs the response along the polar axis. Our results confirm a connection between the polar axis and the giant optical nonlinearity of Weyl semimetals and demonstrate pressure as a means to tune this effect $in$ $situ$.

cond-mat.str-el↗

arXiv2021

Magnetic order, disorder, and excitations under pressure in the Mott insulator Sr$_2$IrO$_4$

Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr$_2$IrO$_4$ at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr$_2$IrO$_4$ under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered state beyond 18 GPa. A strong first-order structural phase transition drives the magnetic evolution at $\sim$10 GPa with reduced structural anisotropy in the IrO$_6$ cages, leading to increasingly isotropic exchange interactions between the Heisenberg spins and a spin-flip transition to $c$-axis-aligned antiferromagnetic order. In the disordered phase of Heisenberg $J_\mathrm{eff}=1/2$ pseudospins, the spin excitations are quasi-elastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr$_2$IrO$_4$.

cond-mat.str-el↗

arXiv2021

Direct Observation of Collective Electronuclear Modes About a Quantum Critical Point

We directly measure the low energy excitation modes of the quantum Ising magnet LiHoF$_4$ using microwave spectroscopy. Instead of a single electronic mode, we find a set of collective electronuclear modes, in which the spin-$1/2$ Ising electronic spins hybridize with the bath of spin-$7/2$ Ho nuclear spins. The lowest-lying electronuclear mode softens at the approach to the quantum critical point, even in the presence of disorder. This softening is rapidly quenched by a longitudinal magnetic field. Similar electronuclear structures should exist in other spin-based quantum Ising systems.

cond-mat.str-el↗

arXiv2021

Phase diagram of the Shastry-Sutherland Compound SrCu2(BO3)2 under extreme combined conditions of field and pressure

Motivated by the intriguing properties of the Shastry-Sutherland compound SrCu2(BO3)2 under pressure, with a still debated intermediate plaquette phase appearing at around 20 kbar and a possible deconfined critical point at higher pressure upon entering the antiferromagnetic phase, we have investigated its high-field properties in this pressure range using tunnel diode oscillator (TDO) measurements. The two main new phases revealed by these measurements are fully consistent with those identified by infinite Projected Entangled Pair states (iPEPS) calculations of the Shastry-Sutherland model, a 1/5 plateau and a 10 x 2 supersolid. Remarkably, these phases are descendants of the full-plaquette phase, the prominent candidate for the intermediate phase of SrCu2(BO3)2. The emerging picture for SrCu2(BO3)2 is shown to be that of a system dominated by a tendency to an orthorhombic distortion at intermediate pressure, an important constraint on any realistic description of the transition into the antiferromagnetic phase.

cond-mat.str-el↗

arXiv2020

A continuous metal-insulator transition driven by spin correlations

Metal-insulator transitions involve a mix of charge, spin, and structural degrees of freedom, and when strongly-correlated, can underlay the emergence of exotic quantum states. Mott insulators induced by the opening of a Coulomb gap are an important and well-recognized class of transitions, but insulators purely driven by spin correlations are much less common, as the reduced energy scale often invites competition from other degrees of freedom. Here we demonstrate a clean example of a spin-correlation-driven metal-insulator transition in the all-in-all-out pyrochlore antiferromagnet Cd2Os2O7, where the lattice symmetry is fully preserved by the antiferromagnetism. After the antisymmetric linear magnetoresistance from conductive, ferromagnetic domain walls is carefully removed experimentally, the Hall coefficient of the bulk reveals four Fermi surfaces, two of electron type and two of hole type, sequentially departing the Fermi level with decreasing temperature below the Néel temperature, T_N. Contrary to the common belief of concurrent magnetic and metal-insulator transitions in Cd2Os2O7, the charge gap of a continuous metal-insulator transition opens only at T~10K, well below T_N=227K. The insulating mechanism resolved by the Hall coefficient parallels the Slater picture, but without a folded Brillouin zone, and contrasts sharply with the behavior of Mott insulators and spin density waves, where the electronic gap opens above and at T_N, respectively.

cond-mat.str-el↗

arXiv2020

Quantum dynamics in strongly driven random dipolar magnets

The random dipolar magnet LiHo$_x$Y$_{1-x}$F$_4$ enters a strongly frustrated regime for small Ho$^{3+}$ concentrations with $x<0.05$. In this regime, the magnetic moments of the Ho$^{3+}$ ions experience small quantum corrections to the common Ising approximation of LiHo$_x$Y$_{1-x}$F$_4$, which lead to a $Z_2$-symmetry breaking and small, degeneracy breaking energy shifts between different eigenstates. Here we show that destructive interference between two almost degenerate excitation pathways burns spectral holes in the magnetic susceptibility of strongly driven magnetic moments in LiHo$_x$Y$_{1-x}$F$_4$. Such spectral holes in the susceptibility, microscopically described in terms of Fano resonances, can already occur in setups of only two or three frustrated moments, for which the driven level scheme has the paradigmatic $Λ$-shape. For larger clusters of magnetic moments, the corresponding level schemes separate into almost isolated many-body $Λ$-schemes, in the sense that either the transition matrix elements between them are negligibly small or the energy difference of the transitions is strongly off-resonant to the drive. This enables the observation of Fano resonances, caused by many-body quantum corrections to the common Ising approximation also in the thermodynamic limit. We discuss its dependence on the driving strength and frequency as well as the crucial role that is played by lattice dissipation.

cond-mat.dis-nn↗

arXiv2019

Approaching the quantum critical point in a highly-correlated all-in-all-out antiferromagnet

Continuous quantum phase transitions involving all-in-all-out (AIAO) antiferromagnetic order in strongly spin-orbit-coupled 5d compounds could give rise to various exotic electronic phases and strongly-coupled quantum critical phenomena. Here we experimentally trace the AIAO spin order in Sm2Ir2O7 using direct resonant x-ray magnetic diffraction techniques under high pressure. The magnetic order is suppressed at a critical pressure Pc=6.30 GPa, while the lattice symmetry remains in the cubic Fd-3m space group across the quantum critical point. Comparing pressure tuning and the chemical series R2Ir2O7 reveals that the suppression of the AIAO order and the approach to the spin-disordered state is characterized by contrasting evolutions of both the pyrochlore lattice constant a and the trigonal distortion x. The former affects the 5d bandwidth, the latter the Ising anisotropy, and as such we posit that the opposite effects of pressure and chemical tuning lead to spin fluctuations with different Ising and Heisenberg character in the quantum critical region. Finally, the observed low-pressure scale of the AIAO quantum phase transition in Sm2Ir2O7 identifies a circumscribed region of P-T space for investigating the putative magnetic Weyl-semimetal state.

cond-mat.str-el↗

arXiv2019

Magnetic domain dynamics in an insulating quantum ferromagnet

The statistics and form of avalanches in a driven system reveal the nature of the underlying energy landscape and dynamics. In conventional metallic ferromagnets, eddy-current back action can dominate the dynamics. Here, we study Barkhausen noise in Li(Ho,Y)F4, an insulating Ising ferromagnet that cannot sustain eddy currents. For large avalanches at temperatures approaching the Curie point, we find a symmetric response free of drag effects. In the low temperature limit, drag effects contribute to the dynamics, which we link to enhanced pinning from local random fields that are enabled by the microscopic dipole-coupled Hamiltonian (the Ising model in transverse field).

cond-mat.other↗

arXiv2019

Odd-parity linear magnetoresistance and the planar Hall effect

The phenomena of odd-parity magnetoresistance and the planar Hall effect are deeply entwined with ferromagnetism. The intrinsic magnetization of the ordered state permits these unusual and rarely observed manifestations of Onsager's theorem when time reversal symmetry is broken at zero applied field. Here we study two classes of ferromagnetic materials, rare-earth magnets with high intrinsic coercivity and antiferromagnetic pyrochlores with strongly-pinned ferromagnetic layers at domain walls, which both exhibit odd-parity magnetoresistive behavior. The peculiar angular variation of the response with respect to the relative alignments of the magnetization, magnetic field, and current reveal the two underlying microscopic mechanisms: spin-polarization-dependent scattering of a Zeeman-shifted Fermi surface and magnetoresistance driven by the anomalous velocity physics usually associated with the anomalous Hall effect.

cond-mat.str-el↗

arXiv2019

Probing many-body localization in a disordered quantum magnet

Quantum states cohere and interfere. Quantum systems composed of many atoms arranged imperfectly rarely display these properties. Here we demonstrate an exception in a disordered quantum magnet that divides itself into nearly isolated subsystems. We probe these coherent clusters of spins by driving the system beyond its linear response regime at a single frequency and measuring the resulting "hole" in the overall linear spectral response. The Fano shape of the hole encodes the incoherent lifetime as well as coherent mixing of the localized excitations. For the disordered Ising magnet, $\mathrm{LiHo_{0.045}Y_{0.955}F_4}$, the quality factor $Q$ for spectral holes can be as high as 100,000. We tune the dynamics of the quantum degrees of freedom by sweeping the Fano mixing parameter $q$ through zero via the amplitude of the ac pump as well as a static external transverse field. The zero-crossing of $q$ is associated with a dissipationless response at the drive frequency, implying that the off-diagonal matrix element for the two-level system also undergoes a zero-crossing. The identification of localized two-level systems in a dense and disordered dipolar-coupled spin system represents a solid state implementation of many-body localization, pushing the search forward for qubits emerging from strongly-interacting, disordered, many-body systems.

cond-mat.dis-nn↗