arXiv subjects

P. M. Sarte

Publications and source records attributed to P. M. Sarte.

15 recordsLinked to original sources

arXiv2026

Influence of controlled disorder on the dipolar spin ice state of Ho-based pyrochlores

Pyrochlore magnets of the form $R_2B_2$O$_7$, in which rare-earth ions on the $R$-site form a three-dimensional network of corner-sharing tetrahedra, provide a canonical setting for geometrical frustration. Ho-based pyrochlores host a dipolar spin-ice ground state, characterized by Ising moments constrained by the ice rules and elementary excitations analogous to magnetic monopoles. Here we examine how controlled chemical disorder influences this state by introducing site mixing on the non-magnetic $B$-site in two compounds. Ho$_2$GaSbO$_7$ contains only Ga$^{3+}$/Sb$^{5+}$ charge disorder, whereas Ho$_2$ScSbO$_7$ exhibits both charge and substantial size disorder arising from the large ionic-radius mismatch between Sc$^{3+}$ and Sb$^{5+}$. Although both materials retain the pyrochlore structure, neutron scattering measurements reveal a reduced correlation length for the $R/B$-site cation ordering and enhanced local structural distortions in Ho$_2$ScSbO$_7$. Despite these structural differences, bulk thermodynamic measurements and magnetic diffuse scattering demonstrate that both systems exhibit the defining signatures of a dipolar spin-ice state. Low-energy inelastic neutron spectroscopy further uncovers broad magnetic excitations that develop within the dipolar spin-ice regime, a feature absent in pristine Ho pyrochlores and indicative of disorder-induced splitting of the non-Kramers ground-state doublet. Together, these results show that controlled disorder generates tunable transverse-field-driven quantum fluctuations in Ho-based pyrochlores, although the dipolar spin-ice state is remarkably robust to this disorder.

cond-mat.str-el↗

arXiv2023

Spin-orbital correlations from complex orbital order in MgV$_{2}$O$_{4}$

MgV$_{2}$O$_{4}$ is a spinel based on magnetic V$^{3+}$ ions which host both spin ($S=1$) and orbital ($l_{eff}=1$) moments. Owing to the underlying pyrochlore coordination of the magnetic sites, the spins in MgV$_{2}$O$_{4}$ only antiferromagnetically order once the frustrating interactions imposed by the $Fd\overline{3}m$ lattice are broken through an orbitally-driven structural distortion at T$_{S}$ $\simeq$ 60 K. Consequently, a Néel transition occurs at T$_{N}$ $\simeq$ 40 K. Low temperature spatial ordering of the electronic orbitals is fundamental to both the structural and magnetic properties, however considerable discussion on whether it can be described by complex or real orbital ordering is ambiguous. We apply neutron spectroscopy to resolve the nature of the orbital ground state and characterize hysteretic spin-orbital correlations using x-ray and neutron diffraction. Neutron spectroscopy finds multiple excitation bands and we parameterize these in terms of a multi-level (or excitonic) theory based on the orbitally degenerate ground state. Meaningful for the orbital ground state, we report an "optical-like" mode at high energies that we attribute to a crystal-field-like excitation from the spin-orbital $j_{eff}$=2 ground state manifold to an excited $j_{eff}$=1 energy level. We parameterize the magnetic excitations in terms of a Hamiltonian with spin-orbit coupling and local crystalline electric field distortions resulting from deviations from perfect octahedra surrounding the V$^{3+}$ ions. We suggest that this provides compelling evidence for complex orbital order in MgV$_{2}$O$_{4}$. We then apply the consequences of this model to understand hysteretic effects in the magnetic diffuse scattering where we propose that MgV$_{2}$O$_{4}$ displays a high temperature orbital memory of the low temperature spin order.

cond-mat.str-el↗

arXiv2023

Orbital character of the spin-reorientation transition in TbMn$_6$Sn$_6$

Ferromagnetic (FM) order in a two-dimensional kagome layer is predicted to generate a topological Chern insulator without an applied magnetic field. The Chern gap is largest when spin moments point perpendicular to the kagome layer, enabling the capability to switch topological transport properties, such as the quantum anomalous Hall effect, by controlling the spin orientation. In TbMn$_{6}$Sn$_{6}$, the uniaxial magnetic anisotropy of the Tb$^{3+}$ ion is effective at generating the Chern state within the FM Mn kagome layers while a spin-reorientation (SR) transition to easy-plane order above $T_{SR}=310$ K provides a mechanism for switching. Here, we use inelastic neutron scattering to provide key insights into the fundamental nature of the SR transition. The observation of two Tb excitations, which are split by the magnetic anisotropy energy, indicates an effective two-state orbital character for the Tb ion, with a uniaxial ground state and an isotropic excited state. The simultaneous observation of both modes below $T_{SR}$ confirms that orbital fluctuations are slow on magnetic and electronic time scales $<$ ps and act as a spatially-random orbital alloy. A thermally-driven critical concentration of isotropic Tb ions triggers the SR transition.

cond-mat.str-el↗

arXiv2021

Absence of moment fragmentation in the mixed $B$-site pyrochlore Nd$_{2}$GaSbO$_{7}$

Nd-based pyrochlore oxides of the form Nd$_{2}B_{2}$O$_{7}$ have garnered a significant amount of interest owing to the moment fragmentation physics observed in Nd$_{2}$Zr$_{2}$O$_{7}$ and speculated in Nd$_{2}$Hf$_{2}$O$_{7}$. Notably this phenomenon is not ubiquitous in this family, as it is absent in Nd$_{2}$Sn$_{2}$O$_{7}$, which features a smaller ionic radius on the $B$-site. Here, we explore the necessary conditions for moment fragmentation in the Nd pyrochlore family through a detailed study of the mixed $B$-site pyrochlore Nd$_{2}$GaSbO$_{7}$. The $B$-site of this system is characterized by significant disorder and an extremely small average ionic radius. Similarly to Nd$_{2}$Sn$_{2}$O$_{7}$, we find no evidence for moment fragmentation through our bulk characterization and neutron scattering experiments, indicating that chemical pressure (and not necessarily the $B$-site disorder) plays a key role in the presence or absence of this phenomenon in this material family. Surprisingly, the presence of significant $B$-site disorder in Nd$_{2}$GaSbO$_{7}$ does not generate a spin glass ground state and instead the same all-in-all-out magnetic order identified in other Nd pyrochlores is found here.

cond-mat.str-el↗

arXiv2020

Van Vleck excitons in Ca$_{2}$RuO$_{4}$

A framework is presented for modeling and understanding magnetic excitations in localized, intermediate coupling magnets where the interplay between spin-orbit coupling, magnetic exchange, and crystal field effects are known to create a complex landscape of unconventional magnetic behaviors and ground states. A spin-orbit exciton approach for modeling these excitations is developed based upon a Hamiltonian which explicitly incorporates single-ion crystalline electric field and spin exchange terms. This framework is then leveraged to understand a canonical Van Vleck $j\rm{_{eff}}=0$ singlet ground state whose excitations are coupled spin and crystalline electric field levels. Specifically, the anomalous Higgs mode [Jain et al. Nat. Phys. 13, 633 (2017)], spin-waves [S. Kunkemöller et al. Phys. Rev. Lett. 115, 247201 (2015)], and orbital excitations [L. Das et al. Phys. Rev. X 8, 011048 (2018)] in the multiorbital Mott insulator Ca$_2$RuO$_4$ are captured and good agreement is found with previous neutron and inelastic x-ray spectroscopic measurements. Furthermore, our results illustrate how a crystalline electric field-induced singlet ground state can support coherent longitudinal, or amplitude excitations, and transverse wavelike dynamics. We use this description to discuss mechanisms for accessing a nearby critical point.

cond-mat.str-el↗

arXiv2020

Spin excitations in the frustrated triangular lattice antiferromagnet NaYbO$_2$

Here we present a neutron scattering-based study of magnetic excitations and magnetic order in NaYbO$_2$ under the application of an external magnetic field. The crystal electric field-split $J = 7/2$ multiplet structure is determined, revealing a mixed $|m_z>$ ground state doublet and is consistent with a recent report Ding et al. [1]. Our measurements further suggest signatures of exchange effects in the crystal field spectrum, manifested by a small splitting in energy of the transition into the first excited doublet. The field-dependence of the low-energy magnetic excitations across the transition from the quantum disordered ground state into the fluctuation-driven ordered regime is analyzed. Signs of a first-order phase transition into a noncollinear ordered state are revealed at the upper-field phase boundary of the ordered regime, and higher order magnon scattering, suggestive of strong magnon-magnon interactions, is resolved within the previously reported $up-up-down$ phase. Our results reveal a complex phase diagram of field-induced order and spin excitations within NaYbO$_2$ and demonstrate the dominant role of quantum fluctuations cross a broad range of fields within its interlayer frustrated triangular lattice.

cond-mat.str-el↗

arXiv2020

Magnetic Fluctuations and the Spin-Orbit Interaction in Mott Insulating CoO

Motivated by the presence of an unquenched orbital angular momentum in CoO, a team at Chalk River, including a recently hired research officer Roger Cowley, performed the first inelastic neutron scattering experiments on the classic Mott insulator [Sakurai $\textit{et al.}$ 1968 Phys. Rev. $\mathbf{167}$ 510]. Despite identifying magnon modes at the zone boundary, the team was unable to parameterise the low energy magnetic excitation spectrum below $T\rm{_{N}}$ using conventional pseudo-bosonic approaches. It would not be for another 40 years that Roger, now at Oxford and motivated by the discovery of the high-$T_{c}$ cuprate superconductors [Bednorz & Muller 1986 Z. Phys. B $\mathbf{64}$ 189], would make another attempt at the parameterisation of the magnetic excitation spectrum that had previously alluded him. Upon his return to CoO, Roger found a system embroiled in controversy, with some of its most fundamental parameters still remaining undetermined. Faced with such a formidable task, Roger performed a series of inelastic neutron scattering experiments in the early 2010's on both CoO and a magnetically dilute structural analogue MgO. These experiments would prove instrumental in the determination of both single-ion [Cowley $\textit{et al.}$ 2013 Phys. Rev. B $\mathbf{88}$ 205117] and cooperative magnetic parameters [Sarte $\textit{et al.}$ 2018 Phys. Rev. B $\mathbf{98}$ 024415] for CoO. Both these sets of parameters would eventually be used in a spin-orbit exciton model [Sarte $\textit{et al.}$ 2019 Phys. Rev. B $\mathbf{100}$ 075143], developed by his longtime friend and collaborator Bill Buyers, to successfully parameterise the complex spectrum that both measured at Chalk River almost 50 years prior. The story of CoO is of one that has come full circle, one filled with both spectacular failures and intermittent, yet profound, little victories.

cond-mat.str-el↗

arXiv2019

Spin-Orbit Excitons in CoO

CoO has an odd number of electrons in its unit cell, and therefore is expected to be metallic. Yet, CoO is strongly insulating owing to significant electronic correlations, thus classifying it as a Mott insulator. We investigate the magnetic fluctuations in CoO using neutron spectroscopy. The strong and spatially far-reaching exchange constants reported in [Sarte et al. Phys. Rev. B 98 024415 (2018)], combined with the single-ion spin-orbit coupling of similar magnitude [Cowley et al. Phys. Rev. B 88, 205117 (2013)] results in significant mixing between $j_{eff}$ spin-orbit levels in the low temperature magnetically ordered phase. The high degree of entanglement, combined with the structural domains originating from the Jahn-Teller structural distortion at $\sim$ 300 K, make the magnetic excitation spectrum highly structured in both energy and momentum. We extend previous theoretical work on PrTl$_{3}$ [Buyers et al. Phys. Rev. B 11, 266 (1975)] to construct a mean-field and multi-level spin exciton model employing the aforementioned spin exchange and spin-orbit coupling parameters for coupled Co$^{2+}$ ions on a rocksalt lattice. This parameterization, based on a tetragonally distorted type-II antiferromagnetic unit cell, captures both the sharp low energy excitations at the magnetic zone center, and the energy broadened peaks at the zone boundary. However, the model fails to describe the momentum dependence of the excitations at high energy transfers, where the neutron response decays faster with momentum than the Co$^{2+}$ form factor. We discuss such a failure in terms of a possible breakdown of localized spin-orbit excitons at high energy transfers.

cond-mat.str-el↗

arXiv2019

Relaxing Kondo screened Kramers-doublets in CeRhSi$_{3}$

CeRhSi$_{3}$ is a superconductor under pressure coexisting with a weakly antiferromagnetic phase characterized by a Bragg peak at $\vec{q}_{0}$=($\sim$ 0.2, 0, 0.5) (N. Aso et al. J. Magn. Magn. Mater. 310, 602 (2007)). The compound is also a heavy fermion material with a large specific heat coefficient $γ$=110 mJ $\cdot$ mol$^{-1}$ $\cdot$ K$^{-2}$ and a high Kondo temperature of $T_{K}$=50 K indicative that CeRhSi$_{3}$ is in a strongly Kondo screened state. We apply high resolution neutron spectroscopy to investigate the magnetic fluctuations in the normal phase, at ambient pressures, and at low temperatures. We measure a commensurate dynamic response centered around the $\vec{Q}$=(0, 0, 2) position that gradually evolves to H$\sim$ 0.2 with decreasing temperature and/or energy transfers. The response is broadened both in momentum and energy and not reminiscent of sharp spin wave excitations found in insulating magnets where the electrons are localized. We parameterize the excitation spectrum and temperature dependence using a heuristic model utilizing the random phase approximation to couple relaxing Ce$^{3+}$ ground state Kramers doublets with a Kondo-like dynamic response. With a Ruderman-Kittel-Kasuya-Yosida (RKKY) exchange interaction within the $ab$ plane and an increasing single site susceptibility, we can qualitatively reproduce the neutron spectroscopic results in CeRhSi$_{3}$ and namely the trade-off between scattering at commensurate and incommensurate positions. We suggest that the antiferromagnetic phase in CeRhSi$_{3}$ is driven by weakly correlated relaxing localized Kramers doublets and that CeRhSi$_{3}$ at ambient pressures is on the border between a Rudderman-Kittel-Yosida antiferromagnetic state and a Kondo screened phase where static magnetism is predominately absent.

cond-mat.str-el↗

arXiv2018

Ordered magnetism in the intrinsically decorated $j\rm{_{eff}}$ = $\frac{1}{2}$ $α$-CoV$_{3}$O$_{8}$

The antiferromagnetic mixed valence ternary oxide $α$-CoV$_{3}$O$_{8}$ displays disorder on the Co$^{2+}$ site that is inherent to the $Ibam$ space group. The zero field structural and dynamic properties of $α$-CoV$_{3}$O$_{8}$~have been investigated using a combination of neutron and x-ray diffraction, DC susceptibility, and neutron spectroscopy. The low temperature magnetic and structural properties are consistent with a random macroscopic distribution of Co$^{2+}$ over the 16$k$ metal sites. However, by applying the sum rules of neutron scattering we observe the collective magnetic excitations are parameterized with an ordered Co$^{2+}$ arrangement and critical scattering consistent with a three dimensional Ising universality class. The low energy spectrum is well-described by Co$^{2+}$ cations coupled $via$ a three dimensional network composed of competing ferromagnetic and stronger antiferromagnetic superexchange within the $ab$ plane and along $c$, respectively. While the extrapolated Weiss temperature is near zero, the 3D dimensionality results in long range antiferromagnetic order at $T\rm{_{N}}\sim$ 19 K. A crystal field analysis finds two bands of excitations separated in energy at $\hbar ω$ $\sim$ 5 meV and 25 meV, consistent with a $j\rm{_{eff}}=\frac{1}{2}$ ground state with little mixing between spin-orbit split Kramers doublets. A comparison of our results to the random 3D Ising magnets and other compounds where spin-orbit coupling is present indicate that the presence of an orbital degree of freedom, in combination with strong crystal field effects and well-separated $j\rm{_{eff}}$ manifolds may play a key role in making the dynamics largely insensitive to disorder.

cond-mat.str-el↗

arXiv2018

Disentangling orbital and spin exchange interactions for Co$^{2+}$ on a rocksalt lattice

Neutron spectroscopy was applied to study the magnetic interactions of orbitally degenerate Co$^{2+}$ on a host MgO rocksalt lattice where no long range spin or orbital order exists. The paramagnetic nature of the substituted monoxide Co$_{0.03}$Mg$_{0.97}$O allows for the disentanglement of spin-exchange and spin-orbit interactions. By considering the prevalent excitations from Co$^{2+}$ spin pairs, we extract 7 exchange constants out to the fourth coordination shell. An antiferromagnetic next nearest neighbor 180$^{\circ}$ exchange interaction is dominant, however dual ferromagnetic and antiferromagnetic interactions are observed for pairings with other pathways. These interactions can be understood in terms of a combination of orbital degeneracy in the $t_{2g}$ channel and the Goodenough-Kanamori-Anderson (GKA) rules. Our work suggests that such a hierarchy of exchange interactions exists in transition metal-based oxides with a $t_{2g}$ orbital degeneracy.

cond-mat.str-el↗

arXiv2018

Dipolar-Octupolar Ising Antiferromagnetism in Sm$_2$Ti$_2$O$_7$: A Moment Fragmentation Candidate

Over the past two decades, the magnetic ground states of all rare earth titanate pyrochlores have been extensively studied, with the exception of Sm$_2$Ti$_2$O$_7$. This is, in large part, due to the very high absorption cross-section of naturally-occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically-enriched single crystal of Sm$_2$Ti$_2$O$_7$. Using inelastic neutron scattering, we determine that the crystal field ground state for Sm$^{3+}$ is a dipolar-octupolar doublet with Ising anisotropy. Neutron diffraction experiments reveal that Sm$_2$Ti$_2$O$_7$ orders into the all-in, all-out magnetic structure with an ordered moment of 0.44(7) $μ_B$ below $T_N=0.35$ K, consistent with expectations for antiferromagnetically-coupled Ising spins on the pyrochlore lattice. Zero-field muon spin relaxation measurements reveal an absence of spontaneous oscillations and persistent spin fluctuations down to 0.03 K. The combination of the dipolar-octupolar nature of the Sm$^{3+}$ moment, the all-in, all-out ordered state, and the low-temperature persistent spin dynamics make this material an intriguing candidate for moment fragmentation physics.

cond-mat.str-el↗

arXiv2018

Evidence for negative thermal expansion in the superconducting precursor phase SmFeAsO

The fluorine-doped rare-earth iron oxypnictide series SmFeAsO$_{1-x}$F$_x$ (0 $\leq x \leq$ 0.10) was investigated with high resolution powder x-ray scattering. In agreement with previous studies, the parent compound SmFeAsO exhibits a tetragonal-to-orthorhombic structural distortion at T$\rm{_{S}}$~=~130~K which is rapidly suppressed by $x \simeq$ 0.10 deep within the superconducting dome. The change in unit cell symmetry is followed by a previously unreported magnetoelastic distortion at 120~K. The temperature dependence of the thermal expansion coefficient $α_{V}$ reveals a rich phase diagram for SmFeAsO: (i) a global minimum at 125 K corresponds to the opening of a spin-density wave instability as measured by pump-probe femtosecond spectroscopy whilst (ii) a global maximum at 110 K corresponds to magnetic ordering of the Sm and Fe sublattices as measured by magnetic x-ray scattering. At much lower temperatures than T$\rm{_{N}}$, SmFeAsO exhibits a significant negative thermal expansion on the order of -40~ppm~$\cdot$~K$^{-1}$ in contrast to the behavior of other rare-earth oxypnictides such as PrFeAsO and the actinide oxypnictide NpFeAsO where the onset of $α<$ 0 only appears in the vicinity of magnetic ordering. Correlating this feature with the temperature and doping dependence of the resistivity and the unit cell parameters, we interpret the negative thermal expansion as being indicative of the possible condensation of itinerant electrons accompanying the opening of a SDW gap, consistent with transport measurements.

cond-mat.supr-con↗

arXiv2017

Evidence for the Confinement of Magnetic Monopoles in Quantum Spin Ice

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids. Despite decades of searches, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials. Here we report the detection of a hierarchy of unequally-spaced magnetic excitations \emph{via} high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$. These excitations are well-described by a simple model of monopole pairs bound by a linear potential with an effective tension of 0.642(8) K~$\cdot$Å$^{-1}$ at 1.65~K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$.

cond-mat.str-el↗

arXiv2014

Incipient Ferromagnetism in Tb2Ge2O7: Application of Chemical Pressure to the Enigmatic Spin Liquid, Tb2Ti2O7

The origin of the spin liquid state in Tb$_2$Ti$_2$O$_7$ has challenged experimentalists and theorists alike for nearly 20 years. To improve our understanding of the exotic magnetism in Tb$_2$Ti$_2$O$_7$, we have synthesized a chemical pressure analog, Tb$_2$Ge$_2$O$_7$. Germanium substitution results in a lattice contraction and enhanced exchange interactions. We have characterized the magnetic ground state of Tb$_2$Ge$_2$O$_7$ with specific heat, ac and dc magnetic susceptibility, and polarized neutron scattering measurements. Akin to Tb$_2$Ti$_2$O$_7$, there is no long-range order in Tb$_2$Ge$_2$O$_7$ down to 20 mK. The Weiss temperature of $-$19.2(1) K, which is more negative than that of Tb$_2$Ti$_2$O$_7$, supports the picture of stronger antiferromagnetic exchange. Polarized neutron scattering of Tb$_2$Ge$_2$O$_7$ reveals that at 3.5 K liquid-like correlations dominate in this system. However, below 1 K, the liquid-like correlations give way to intense short-range ferromagnetic correlations with a length scale related to the Tb-Tb nearest neighbor distance. Despite stronger antiferromagnetic exchange, the ground state of Tb$_2$Ge$_2$O$_7$ has ferromagnetic character, in stark contrast to the pressure-induced antiferromagnetic order observed in Tb$_2$Ti$_2$O$_7$.

cond-mat.str-el↗