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S. M. Koohpayeh

Publications and source records attributed to S. M. Koohpayeh.

At least 19 recordsLinked to original sources

Intrinsic quantum disorder in Yb2Ti2O7 and the quantum S=1/2 pyrochlore phase diagram

We present an experimental and theoretical study of the anisotropic pyrochlore phase diagram. Inelastic field-dependent neutron scattering on Yb$_2$Ti$_2$O$_7$ shows intrinsic broadening and a flat low-energy magnon mode which is partially captured by interacting magnon models. Exact diagonalization reveals the existence of an emergent quantum phase between ferromagnetism and antiferromagnetism, in which Yb$_2$Ti$_2$O$_7$ Hamiltonian potentially resides. This behavior matches the phenomenology of quantum criticality in heavy fermion systems, and shows Yb$_2$Ti$_2$O$_7$ is a clean system which can be field-tuned from well-defined magnons to a nontrivial quantum ground state. This suggests that quantum criticality is a generic feature of the dipolar phase diagram.

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Quenched Disorder in the Triangular Lattice Antiferromagnet YbZn$_2$GaO$_5$

We investigate the crystal electric field (CEF) excitations of Yb$^{3+}$ ions in powder samples of the triangular-lattice rare-earth-based antiferromagnet YbZn$_2$GaO$_5$ using inelastic neutron scattering (INS). Three CEF excitations from the ground-state Kramers doublet were observed, each exhibiting significant broadening beyond instrumental resolution. Combining temperature-dependent INS and neutron powder diffraction, we identify a significant static contribution to this broadening and attribute it to heterogeneous coordination of Yb$^{3+}$ ions due to Ga$^{3+}$/Zn$^{2+}$ site mixing. Rietveld refinement of neutron powder diffraction indicates that 35% of Ga occupies the Zn site and 60% of Zn occupies the Ga site. We show with a point charge model for the CEF Hamiltonian that heterogeneous coordination of Yb$^{3+}$ ions leads to broadened CEF peaks. First-principles calculations demonstrate that the random Ga$^{3+}$/Zn$^{2+}$ distribution can produce the distortions of the YbO$_6$ octahedra observed from neutron diffraction. Because the documented heterogeneity will extend to exchange interactions, our results suggest that disorder is a significant factor in the unusual magnetism previously reported in YbZn$_2$GaO$_5$, including broad low-energy magnetic excitations and the absence of magnetic ordering down to 0.3K.

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Pressure control of magnetic order and excitations in the pyrochlore antiferromagnet MgCr$_{2}$O$_{4}$

MgCr$_{2}$O$_{4}$ is one of the best-known realizations of the pyrochlore-lattice Heisenberg antiferromagnet. The strong antiferromagnetic exchange interactions are perturbed by small further-neighbor exchanges such that this compound may in principle realize a spiral spin liquid (SSL) phase in the zero-temperature limit. However, a spin Jahn-Teller transition below $T_{\rm N} \approx 13$ K yields a complicated long-range magnetic order with multiple coexisting propagation vectors. We present neutron scattering and thermo-magnetic measurements of MgCr$_{2}$O$_{4}$ samples under applied hydrostatic pressure up to $P=1.7$ GPa demonstrating the existence of multiple close-lying nearly degenerate magnetic ground states. We show that the application of hydrostatic pressure increases the ordering temperature by around 0.8 K per GPa and increases the bandwidth of the magnetic excitations by around 0.5 meV per GPa. We also evidence a strong tendency for the preferential occupation of a subset of magnetic domains under pressure. In particular, we show that the $\boldsymbol{k}=(0,0,1)$ magnetic phase, which is almost negligible at ambient pressure, dramatically increases in spectral weight under pressure. This modifies the spectrum of magnetic excitations, which we interpret unambiguously as spin waves from multiple magnetic domains. Moreover, we report that the application of pressure reveals a feature in the magnetic susceptibility above the magnetostructural transition. We interpret this as the onset of a short-range ordered phase associated with $\boldsymbol{k}=(0,0,1)$, previously not observed in magnetometry measurements.

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Quantum Critical Magnetic Excitations in Spin-1/2 and Spin-1 Chain Systems

The study of CoNb$_2$O$_6$ sits at the confluence of simplicity and complexity: on one hand, the model for Ising chains -- the building blocks of CoNb$_2$O$_6$ -- in a transverse field, can be exactly solved and, thus, serves as an archetype of quantum criticality; on the other hand, the weak but nonzero interchain coupling adds geometric frustration to the stage, substantially complicating the phase diagram. Here we utilize low-temperature specific heat and thermal conductivity measurements to study the low-lying magnetic excitations in CoNb$_2$O$_6$ and its spin-1 analogue NiNb$_2$O$_6$. The thermal conductivity is found to be suppressed around the quantum critical point, where the specific heat is enhanced due to gapless magnetic excitations, pointing to the localized nature of the latter. These results highlight the predominant role of frustration in determining the quantum critical magnetic excitations of spin chains, which may furthermore underlie the remarkable similarities between the phenomenology of these spin-1/2 and spin-1 systems.

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Topological nature of the Kondo insulator SmB$_6$ and its sensitiveness to Sm vacancy

The true topological nature of the Kondo insulator SmB$_6$ remains to be unveiled. Our previous tunneling study not only found evidence for the existence of surface Dirac fermions, but it also uncovered that they inherently interact with the spin excitons, collective excitations in the bulk. We have extended such a spectroscopic investigation into crystals containing a Sm deficiency. The bulk hybridization gap is found to be insensitive to the deficiency up to 1% studied here, but the surface states in Sm-deficient crystals exhibit quite different temperature evolutions from those in stoichiometric ones. We attribute this to the topological surface states remaining incoherent down to the lowest measurement temperature due to their continued interaction with the spin excitons that remain uncondensed. This result shows that the detailed topological nature of SmB$_6$ could vary drastically in the presence of disorder in the lattice. This sensitiveness to disorder is seemingly contradictory to the celebrated topological protection, but it can be understood as being due to the intimate interplay between strong correlations and topological effects.

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Monopolar and dipolar relaxation in spin ice Ho$_2$Ti$_2$O$_7$

When degenerate states are separated by large energy barriers, the approach to thermal equilibrium can be slow enough that physical properties are defined by the thermalization process rather than the equilibrium. The exploration of thermalization pushes experimental boundaries and provides refreshing insights into atomic scale correlations and processes that impact steady state dynamics and prospects for realizing solid state quantum entanglement. We present a comprehensive study of magnetic relaxation in Ho$_2$Ti$_2$O$_7$ based on frequency-dependent susceptibility measurements and neutron diffraction studies of the real-time atomic-scale response to field quenches. Covering nearly ten decades in time scales, these experiments uncover two distinct relaxation processes that dominate in different temperature regimes. At low temperatures (0.6K<T<1K) magnetic relaxation is associated with monopole motion along the applied field direction through the spin-ice vacuum. The increase of the relaxation time upon cooling indicates reduced monopole conductivity driven by decreasing monopole concentration and mobility as in a semiconductor. At higher temperatures (1K<T<2K) magnetic relaxation is associated with the reorientation of monopolar bound states as the system approaches the single-spin tunneling regime. Spin fractionalization is thus directly exposed in the relaxation dynamics.

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Duality and domain wall dynamics in a twisted Kitaev chain

The Ising chain in transverse field is a paradigmatic model for a host of physical phenomena, including spontaneous symmetry breaking, topological defects, quantum criticality, and duality. Although the quasi-1D ferromagnet CoNb$_2$O$_6$ has been put forward as the best material example of the transverse field Ising model, it exhibits significant deviations from ideality. Through a combination of THz spectroscopy and theory, we show that CoNb$_2$O$_6$ in fact is well described by a different model with strong bond dependent interactions, which we dub the {\it twisted Kitaev chain}, as these interactions share a close resemblance to a one-dimensional version of the intensely studied honeycomb Kitaev model. In this model the ferromagnetic ground state of CoNb$_2$O$_6$ arises from the compromise between two distinct alternating axes rather than a single easy axis. Due to this frustration, even at zero applied field domain-wall excitations have quantum motion that is described by the celebrated Su-Schriefer-Heeger model of polyacetylene. This leads to rich behavior as a function of field. Despite the anomalous domain wall dynamics, close to a critical transverse field the twisted Kitaev chain enters a universal regime in the Ising universality class. This is reflected by the observation that the excitation gap in CoNb$_2$O$_6$ in the ferromagnetic regime closes at a rate precisely twice that of the paramagnet. This originates in the duality between domain walls and spin-flips and the topological conservation of domain wall parity. We measure this universal ratio `2' to high accuracy -- the first direct evidence for the Kramers-Wannier duality in nature.

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Low Energy Magneto-optics of Tb$_{2}$Ti$_{2}$O$_{7}$ in [111] Magnetic Field

The pyrochlore magnet Tb$_{2}$Ti$_{2}$O$_{7}$ shows a lack of magnetic order to low temperatures and is considered to be a quantum spin liquid candidate. We perform time-domain THz spectroscopy on high quality Tb$_{2}$Ti$_{2}$O$_{7}$ crystal and study the low energy excitations as a function of [111] magnetic field with high energy resolution. The low energy crystal field excitations change their energies anomalously under magnetic field. Despite several sharp field dependent changes, we show that the material's spectrum can be described not by a phase transitions, but by field dependent hybridization between the low energy crystal field levels. We highlight the strong coupling between spin and lattice degrees of freedom in Tb$_{2}$Ti$_{2}$O$_{7}$ as evidenced by the magnetic field tunable crystal field environment. Calculations based on single ion physics with field induced symmetry reduction of the crystal field environment can reproduce our data.

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Orientation Dependence of the Magnetic Phase Diagram of Yb$_2$Ti$_2$O$_7$

In the quest to realize a quantum spin liquid (QSL), magnetic long-range order is hardly welcome. Yet it can offer deep insights into a complex world of strong correlations and fluctuations. Much hope was placed in the cubic pyrochlore Yb$_2$Ti$_2$O$_7$ as a putative U(1) QSL but a new class of ultra-pure single crystals make it abundantly clear the stoichiometric compound is a ferromagnet. Here we present a detailed experimental and theoretical study of the corresponding field-temperature phase diagram. We find it to be richly anisotropic with a critical endpoint for $\vec{B}\,\parallel\,\langle 100\rangle$, while field parallel to $\langle 110 \rangle$ and $\langle 111 \rangle$ enhances the critical temperature by up to a factor of two and shifts the onset of the field-polarized state to finite fields. Landau theory shows that Yb$_2$Ti$_2$O$_7$ in some ways is remarkably similar to pure iron. However, it also pinpoints anomalies that cannot be accounted for at the classical mean-field level including a dramatic enhancement of $T_{\mathrm{C}}$ and reentrant phase boundary by fields with a component transverse to the easy axes, as well as the anisotropy of the upper critical field in the quantum limit.

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Multiphase Magnetism in Yb2Ti2O7

We document the coexistence of ferro- and anti-ferromagnetism in pyrochlore $\rm Yb_2Ti_2O_7$ using three neutron scattering techniques on stoichiometric crystals: elastic neutron scattering shows a canted ferromagnetic ground state, neutron scattering shows spin wave excitations from both a ferro-and an antiferro-magnetic state, and field and temperature dependent small angle neutron scattering reveals the corresponding anisotropic magnetic domain structure. High-field $\langle 111 \rangle$ spin wave fits show that $\rm Yb_2Ti_2O_7$ is extremely close to an antiferromagnetic phase boundary. Classical Monte Carlo simulations based on the interactions inferrred from high field spin wave measurements confirm $ψ_2$ antiferromagnetism is metastable within the FM ground state.

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Enhanced thermal Hall conductivity below 1 Kelvin in the pyrochlore magnet Yb$_2$Ti$_2$O$_7$

In this letter, we report the gigantic thermal Hall effect $κ_{xy}$ in the low-field correlated-paramagnetic state of the frustrated pyrochlore Yb$_2$Ti$_2$O$_7$. We observed a record magnitude for the thermal Hall angle in an insulator, $\left|κ_{xy}\right|/κ_{xx}\sim 2\,\%$. The signal onsets at $T\sim 3\,$K and is severely weakened around the transition to canted ferromagnetic order at $T_\text{CFM}=0.275\,$K. Besides the large $κ_{xy}>0$ of the fluctuating regime, a sign change towards negative $κ_{xy}$ occurs at the lowest temperatures and in moderate field, where sharp magnon excitations appear in the inelastic neutron scattering spectra. We analyze the magnon-Hall signal and its suppression with field semi-quantitatively. A contribution of phonon skew scattering to $κ_{xy}$ is ruled out by a comparison of $κ_{xx}$ for Tb-, Yb-, and Y-based rare earth pyrochlore titanates. These results represent the first report of non-vanishing $κ_{xy}$ measured in a dilution refrigerator ($T < 0.29\,$K).

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Probing magnon dynamics and interactions in a ferromagnetic spin-1 chain

NiNb$_{2}$O$_{6}$ is an almost ideal realization of a 1D spin-1 ferromagnetic Heisenberg chain compound with weak unidirectional anisotropy. Using time-domain THz spectroscopy, we measure the low-energy electrodynamic response of NiNb$_{2}$O$_{6}$ as a function of temperature and external magnetic field. At low temperatures, we find a magnon-like spin-excitation, which corresponds to the lowest energy excitation at $q\sim0$. At higher temperatures, we unexpectedly observe a temperature-dependent renormalization of the spin-excitation energy, which has a strong dependence on field direction. Using theoretical arguments, exact diagonalizations and finite temperature dynamical Lanczos calculations, we construct a picture of magnon-magnon interactions that naturally explains the observed renormalization. This unique scenario is a consequence of the spin-1 nature and has no analog in the more widely studied spin-1/2 systems.

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Synthesis, crystal growth and characterization of the pyrochlore Er2Ti2O7

Pyrochlore erbium titanate samples in the form of powders (with nominal compositions of Er2Ti2+xO7) and bulk single crystals were prepared to elucidate the effect of synthesis and growth conditions on their composition, structure, and transition temperature. All samples were characterized using X-ray diffraction and specific heat measurements. Larger lattice parameters were measured for the Ti-deficient stuffed powders, Er2(Ti2-xErx)O7-δ, while Ti-rich anti-stuffed powders, (Er2-xTix)Ti2O7+δ, showed a decrease in lattice parameter. The lattice parameter for the stoichiometrically synthesized powder, Er2Ti2O7, was measured to be a = 10.07522(9) Å. Single crystals grown by the conventional floating zone (FZ) technique were Ti deficient (stuffed) and darker in color due to oxygen vacancies. Using the traveling solvent floating zone (TSFZ), a high structural quality, transparent and stoichiometric Er2Ti2O7 single crystal was grown at a lower temperature using the TiO2 solvent. Heat capacity measurements of the TSFZ grown Er2Ti2O7 crystal and stoichiometric powder exhibited a very close magnetic transition temperature TC ~1.23K that was suppressed in off-stoichiometric samples, demonstrating correlations between stoichiometry and ground state magnetism in Er2Ti2O7.

cond-mat.mtrl-sci↗

Magnetic excitations of the classical spin liquid MgCr2O4

We report a comprehensive inelastic neutron-scattering study of the frustrated pyrochlore antiferromagnet MgCr2O4 in its cooperative paramagnetic regime. Theoretical modeling yields a microscopic Heisenberg model with exchange interactions up to third-nearest neighbors, which quantitatively explains all the details of the dynamic magnetic response. Our work demonstrates that the magnetic excitations in paramagnetic MgCr2O4 are faithfully represented in the entire Brillouin zone by a theory of magnons propagating in a highly-correlated paramagnetic background. Our results also suggest that MgCr2O4 is proximate to a spiral spin-liquid phase distinct from the Coulomb phase, which has implications for the magneto-structural phase transition in MgCr2O4 .

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Field-dependent heat transport in the Kondo insulator SmB6 : phonons scattered by magnetic impurities

The thermal conductivity $κ$ of the Kondo insulator SmB$_6$ was measured at low temperature, down to 70 mK, in magnetic fields up to 15 T, on single crystals grown using both the floating-zone and the flux methods. The residual linear term $κ_0/T$ at $T \to 0$ is found to be zero in all samples, for all magnetic fields, in agreement with previous studies. There is therefore no clear evidence of fermionic heat carriers. In contrast to some prior data, we observe a large enhancement of $κ(T)$ with increasing field. The effect of field is anisotropic, depending on the relative orientation of field and heat current (parallel or perpendicular), and with respect to the cubic crystal structure. We interpret our data in terms of heat transport predominantly by phonons, which are scattered by magnetic impurities.

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Diamagnetic Sm$^{3+}$ in the topological Kondo insulator SmB$_6$

Samarium hexaboride is a topological Kondo insulator, with metallic surface states manifesting from its insulating band structure. Since the insulating bulk itself is driven by strong correlations, both the bulk and surface host compelling magnetic and electronic phenomena. We employed X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Sm M$_{4,5}$ edges to measure surface and bulk magnetic properties of Sm$^{2+}$ and Sm$^{3+}$ within SmB$_6$. We observed anti-alignment to the applied field of the Sm$^{3+}$ magnetic dipole moment below $T = 75$ K and of the total orbital moment of samarium below 30 K. The induced Sm$^{3+}$ moment at the cleaved surface at 8 K and 6 T implies 1.5% of the total Sm as magnetized Sm$^{3+}$. The field dependence of the Sm$^{3+}$ XMCD dichorism at 8 K is diamagnetic and approximately linear. The bulk magnetization at 2 K is however driven by Sm$^{2+}$ Van Vleck susceptibility as well as 1% paramagnetic impurities with $μ_{\rm Eff} = 5.2(1)~μ_{\rm B}$. This indicates diamagnetic Sm$^{3+}$ is compensated within the bulk. The XAS and XMCD spectra are weakly affected by Sm vacancies and carbon doping while XAS is strongly affected by polishing.

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Non-uniform carrier density in Cd$_3$As$_2$ evidenced by optical spectroscopy

We report the detailed optical properties of Cd$_3$As$_2$ crystals in a wide parameter space: temperature, magnetic field, carrier concentration and crystal orientation. We investigate high-quality crystals synthesized by three different techniques. In all the studied samples, independently of how they were prepared and how they were treated before the optical experiments, our data indicate conspicuous fluctuations in the carrier density (up to 30%). These charge puddles have a characteristic scale of 100 $μ$m, they become more pronounced at low temperatures, and possibly, they become enhanced by the presence of crystal twinning. The Drude response is characterized by very small scattering rates ($\sim 1$ meV) for as-grown samples. Mechanical treatment, such as cutting or polishing, influences the optical properties of single crystals, by increasing the Drude scattering rate and also modifying the high frequency optical response. Magneto-reflectivity and Kerr rotation are consistent with electron-like charge carriers and a spatially non-uniform carrier density.

cond-mat.mtrl-sci↗

Impurities or a neutral Fermi surface? A further examination of the low-energy ac optical conductivity of SmB$_6$

Recent experiments have uncovered evidence of low energy excitations in the bulk of SmB$_6$ that are perhaps associated with unconventional quasiparticles, bringing into question whether this Kondo "insulator" is truly insulating in the bulk. Recently, we demonstrated that SmB$_6$ possesses significant in-gap bulk ac conduction far in excess of typical disordered semiconductors. Whether such conduction is an intrinsic feature of SmB$_6$, suggesting the formation of an exotic state, or residual conduction from impurities continues to be a topic of debate. Here, we further examine the origin of the ac optical conductivity of SmB$_6$ in light of recent experimental and theoretical developments. The optical conductivity of SmB$_6$ is shown to possess distinct regimes of either dominant free carrier or $localized$ response contributions. The free carrier response is found to be in good qualitative agreement with previous literature, although quantitative differences are revealed and discussed. The localized response, which dominates at the lowest temperatures, is analyzed in the context of models of either in-gap impurity states or an exotic neutral Fermi surface. The charge density or effective mass of this low temperature in-gap conductivity is extracted through a conductivity sum rule analysis and found to be in general alignment with both models in the appropriate limits. Our results shed further light on the nature of the in-gap states of this remarkable material.

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