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A. P. Ramirez

Publications and source records attributed to A. P. Ramirez.

At least 19 recordsLinked to original sources

How Electrons Become Mobile in a Colossal Dielectric -- Fe$_2$TiO$_5$

We measure the colossal permittivity in single crystal Fe$_2$TiO$_5$ using broadband spectroscopy in the frequency range 20 Hz - 1 MHz. The relaxation response is analyzed using a Debye-like model with Arrhenius activation in two different ways and yields an energy barrier of 286.1 $\pm$ 2.8 meV. DC transport yields an activation energy of 288.8 $\pm$ 2.8 meV. These results strongly imply that the energy barrier for localized dipole motion and itinerant charge transport originate from the same atom-level forces. A further implication is that colossal dielectric behavior is a microscopic bulk phenomenon arising from a system on brink of metallicity.

cond-mat.mtrl-sci

Suppression of Thermal Conductivity via Singlet-Dominated Scattering in TmFeO$_3$

We measured the thermal conductivity of the rare-earth orthoferrites, $R$FeO$_3$, where $R$ = Eu, Gd, Tb, Dy, Ho, Er, Tm, and Yb from 3 K to 300 K and see an anomalous strong suppression for TmFeO$_3$ over most of the temperature range. Using a Debye thermal transport model, we demonstrate that this suppression is due to resonant scattering between phonons and the Tm$^{3+}$ $4f$ singlet crystal field levels. The implications of these results are discussed in context of thermal conductivity studies in quantum magnets.

cond-mat.mtrl-sci

Quantum Spin Relaxation with THz Attempt Frequency in the 1/3-Fire, 2/3-Ice Ferrimagnet SmMn$_2$Ge$_2$

Ferrimagnets in which half the spins are disordered and half ordered, so-called half-fire, half-ice state, have been advanced theoretically as a route towards realizing exotic magnetic ground states. Here we demonstrate novel single-spin resonance in SmMn$_2$Ge$_2$, a 1/3-fire, 2/3-ice material. Using ac-susceptibility in the frequency range 0.1 Hz - 1 kHz we find a Debye-like resonance with Orbach relaxation temperature dependence, yielding an energy barrier $E_B \approx 840$ $k_B$ and attempt frequencies in the THz range. These quantities strongly suggest single-spin relaxation among paramagnetic Sm spins where the flipping field is provided by the FM-ordered Mn spins at domain boundaries, a direct outcome of the 1/3-fire, 2/3-ice state.

cond-mat.mtrl-sci

Neutron Scattering Study of Fluctuating and Static Spin Correlations in the Anisotropic Spin Glass Fe$_2$TiO$_5$

The anisotropic spin glass transition, in which spin freezing is observed only along the c-axis in pseudobrookite Fe$_2$TiO$_5$, has long been perplexing because the Fe$^{3+}$ moments (d$^5$) are expected to be isotropic. Recently, neutron diffraction demonstrated that surfboard-shaped antiferromagnetic nanoregions coalesce above the glass transition temperature, T$_g$ $\approx$ 55 K, and a model was proposed in which the freezing of the fluctuations of the surfboards' magnetization leads to the anisotropic spin glass state. Given this new model, we have carried out high resolution inelastic neutron scattering measurements of the spin-spin correlations to understand the temperature dependence of the intra-surfboard spin dynamics on neutron (picosecond) time-scales. Here, we report on the temperature-dependence of the spin fluctuations measured from single crystal Fe$_2$TiO$_5$. Strong quasi-elastic magnetic scattering, arising from intra-surfboard correlations, is observed well above T$_g$. The spin fluctuations possess a steep energy-wave vector relation and are indicative of strong exchange interactions, consistent with the large Curie-Weiss temperature. As the temperature approaches T$_g$ from above, a shift in spectral weight from inelastic to elastic scattering is observed. At various temperatures between 4 K and 300 K, a characteristic relaxation rate of the fluctuations is determined. Despite the freezing of the majority of the spin correlations, an inelastic contribution remains even at base temperature, signifying the presence of fluctuating intra-surfboard spin correlations to at least T/T$_g$ $\approx$ 0.1 consistent with a description of Fe$_2$TiO$_5$ as a hybrid between conventional and geometrically frustrated spin glasses.

cond-mat.dis-nn

The Geometrically Frustrated Spin Glass (Fe1-pGap)2TiO5

The unusual anisotropy of the spin glass transition in the pseudobrookite system Fe$_2$TiO$_5$ has been interpreted as arising from an induced, van der Waals-like, interaction among magnetic clusters. Here we present susceptibility ($χ$) and specific heat data (C) for Fe2TiO5 diluted with non-magnetic Ga, (Fe$_{1-p}$Ga$_p$)$_2$TiO$_5$, for disorder parameter p = 0, 0.11, and 0.42, and elastic neutron scattering data for p = 0.20. A uniform suppression of T{_g} is observed upon increasing p, along with a value of $χ(T_g)$ that increases as T$_g$ decreases, i.e. $dχ(T_g)/dT_g< 0$. We also observe C(T) $\propto$ T$^2$ in the low temperature limit. The observed behavior places (Fe$_{1-p}$Ga$_p$)$_2$TiO$_5$ in the category of a strongly geometrically frustrated spin glass.

cond-mat.dis-nn

Eminuscent phase in frustrated magnets: a challenge to quantum spin liquids

A geometrically frustrated (GF) magnet consists of localised magnetic moments, spins, whose orientation cannot be arranged to simultaneously minimise their interaction energies. Such materials may host novel fascinating phases of matter, such as fluid-like states called quantum spin liquids. GF magnets have, like all solid-state systems, randomly located impurities whose magnetic moments may ``freeze'' at low temperatures, making the system enter a spin-glass state. We analyse the available data for spin-glass transitions in GF materials and find a surprising trend: the glass-transition temperature grows with decreasing impurity concentration and reaches a finite value in the impurity-free limit at a previously unidentified, ``hidden'', energy scale. We propose a scenario in which the interplay of interactions and entropy leads to a crossover in the permeability of the medium that assists glass freezing at low temperatures. This low-temperature, ``eminuscent'', phase may obscure or even destroy the widely-sought spin-liquid states in rather clean systems.

cond-mat.str-el

Magnetoquantum Oscillations in the Specific Heat of a Topological Kondo Insulator

Surprisingly, magnetoquantum oscillations (MQO) characteristic of a metal with a Fermi surface have been observed in measurements of the topological Kondo insulator SmB6. As these MQO have only been observed in measurements of magnetic torque (dHvA) and not in measurements of magnetoresistance (SdH), a debate has arisen as to whether the MQO are an extrinsic effect arising from rare-earth impurities, defects, and/or aluminum inclusions or an intrinsic effect revealing the existence of charge-neutral excitations. We report here the first observation of magnetoquantum oscillations in the low-temperature specific heat of SmB6. The observed frequencies and their angular dependence for these flux-grown samples are consistent with previous results based on magnetic torque for SmB6 but the inferred effective masses are significantly larger than previously reported. Such oscillations can only be observed if the MQO are of bulk thermodynamic origin; the measured magnetic-field dependent oscillation amplitude and effective mass allow us to rule out suggestions of an extrinsic, aluminium inclusion-based origin for the MQO.

cond-mat.str-el

Observation of Quantum Oscillations in The Low Temperature Specific Heat of SmB$_6$

We report measurements of the low-temperature specific heat of Al-flux-grown samples of SmB$_6$ in magnetic fields up to 32 T. Quantum oscillations periodic in $1/H$ are observed between 8 and 32 T at selected angles between [001] and [111]. The observed frequencies and their angular dependence are consistent with previous magnetic torque measurements of SmB$_6$ but the effective masses inferred from Lifshitz-Kosevich theory are significantly larger and closer to those inferred from zero-field specific heat. Our results are thus consistent with a bulk density of states origin for the oscillations.

cond-mat.str-el

Fluctuation-Induced Interactions and the Spin Glass Transition in $Fe_2TiO_5$

We investigate the spin-glass transition in the strongly frustrated well-known compound $Fe_2TiO_5$. A remarkable feature of this transition, widely discussed in the literature, is its anisotropic properties: the transition manifests itself in the magnetic susceptibly only along one axis, despite $Fe^{3+}$ $d^5$ spins having no orbital component. We demonstrate, using neutron scattering, that below the transition temperature $T_g = 55 K$, $Fe_2TiO_5$ develops nanoscale surfboard shaped antiferromagnetic regions in which the $Fe^{3+}$ spins are aligned perpendicular to the axis which exhibits freezing. We show that the glass transition may result from the freezing of transverse fluctuations of the magnetization of these regions and we develop a mean-field replica theory of such a transition, revealing a type of magnetic van der Waals effect.

cond-mat.dis-nn

Evidence for Undoped Weyl Semimetal Charge Transport in $Y_{2}Ir_{2}O_{7}$

Weyl fermions scattering from a random Coulomb potential are predicted to exhibit resistivity versus temperature $ρ\space α\space T^{-4}$ in a single particle model. Here we show that, in closed environment-grown polycrystalline samples of $Y_{2}Ir_{2}O_{7}$, $ρ= ρ_{0} T^{-4}$ over four orders of magnitude in $ρ$. While the measured prefactor, $ρ_{0}$, is obtained from the model using reasonable materials parameters, the $T^{-4}$ behavior extends far beyond the model's range of applicability. In particular, the behavior extends into the low-temperature, high-resistivity region where the Ioffe-Regel parameter, $k_{T} \ell \ll 2π$. Strong on-site Coulomb correlations, instrumental for predicting a Weyl semimetal state in $Y_{2}Ir_{2}O_{7}$, are the possible origin of such "bad" Weyl semimetal behavior.

cond-mat.str-el

Spin order and dynamics in the diamond-lattice Heisenberg antiferromagnets CuRh2O4 and CoRh2O4

Antiferromagnetic insulators on the diamond lattice are candidate materials to host exotic magnetic phenomena ranging from spin-orbital entanglement to degenerate spiral ground-states and topological paramagnetism. Compared to other three-dimensional networks of magnetic ions, such as the geometrically frustrated pyrochlore lattice, the investigation of diamond-lattice magnetism in real materials is less mature. In this work, we characterize the magnetic properties of model A-site spinels CoRh2O4 (cobalt rhodite) and CuRh2O4 (copper rhodite) by means of thermo-magnetic and neutron scattering measurements and perform group theory analysis, Rietveld refinement, mean-field theory, and spin wave theory calculations to analyze the experimental results. Our investigation reveals that cubic CoRh2O4 is a canonical S=3/2 diamond-lattice Heisenberg antiferromagnet with a nearest neighbor exchange J = 0.63 meV and a Neel ordered ground-state below a temperature of 25 K. In tetragonally distorted CuRh2O4, competiting exchange interactions between up to third nearest-neighbor spins lead to the development of an incommensurate spin helix at 24 K with a magnetic propagation vector k = (0,0,0.79). Strong reduction of the ordered moment is observed for the S=1/2 spins in CuRh2O4 and captured by our 1/S corrections to the staggered magnetization. Our work identifies CoRh2O4 and CuRh2O4 as reference materials to guide future work searching for exotic quantum behavior in diamond-lattice antiferromagnets.

cond-mat.str-el

Structural and magnetic properties of two branches of the Tripod Kagome Lattice family A$_{2}$RE$_{3}$Sb$_{3}$O$_{14}$ (A = Mg, Zn; RE = Pr, Nd, Gd, Tb, Dy, Ho, Er, Yb)

We present a systematic study of the structural and magnetic properties of two branches of the rare earth Tripod Kagome Lattice (TKL) family A$_{2}$RE$_{3}$Sb$_{3}$O$_{14}$ (A = Mg, Zn; RE = Pr, Nd, Gd, Tb, Dy, Ho, Er, Yb; here, we use abbreviation \textit{A-RE}, as in \textit{MgPr} for Mg$_{2}$Pr$_{3}$Sb$_{3}$O$_{14}$), which complements our previously reported work on \textit{MgDy}, \textit{MgGd}, and \textit{MgEr} \cite{TKL}. The present susceptibility ($χ_{dc}$, $χ_{ac}$) and specific heat measurements reveal various magnetic ground states, including the non-magnetic singlet state for \textit{MgPr}, \textit{ZnPr}; long range orderings (LROs) for \textit{MgGd}, \textit{ZnGd}, \textit{MgNd}, \textit{ZnNd}, and \textit{MgYb}; a long range magnetic charge ordered state for \textit{MgDy}, \textit{ZnDy}, and potentially for \textit{MgHo}; possible spin glass states for \textit{ZnEr}, \textit{ZnHo}; the absence of spin ordering down to 80 mK for \textit{MgEr}, \textit{MgTb}, \textit{ZnTb}, and \textit{ZnYb} compounds. The ground states observed here bear both similarities as well as striking differences from the states found in the parent pyrochlore systems. In particular, while the TKLs display a greater tendency towards LRO, the lack of LRO in \textit{MgHo}, \textit{MgTb} and \textit{ZnTb} can be viewed from the standpoint of a balance among spin-spin interactions, anisotropies and non-Kramers nature of single ion state. While substituting Zn for Mg changes the chemical pressure, and subtly modifies the interaction energies for compounds with larger RE ions, this substitution introduces structural disorder and modifies the ground states for compounds with smaller RE ions (Ho, Er, Yb).

cond-mat.str-el

Electron-phonon coupling in DyFeO3 revealed by infrared spectroscopy

We have investigated crystal field and phonon dynamics of the multiferroic orthoferrite DyFeO$_3$ via polarized infrared spectroscopy. Reflectance of single crystals was measured in the far- to mid-infrared spectral range at range of temperatures from 10-295 K. We observe a strongly anisotropic phonon spectrum which differs from earlier lattice dynamical calculations in its symmetry, as well as a mode with significant and unusual temperature dependence that we interpret as a coupled phonon-crystal-field excitation.

cond-mat.str-el

Spin Order and Excitations in Triangular Antiferromagnet La2Ca2MnO7

We report a spin S = 3/2 triangular antiferromagnet with nearest-neighbor coupling J = 0.29 meV in La2Ca2MnO7. A genuinely two-dimensional, three-sublattice order develops below 2.80 K << the Weiss constant (25 K). The spin excitations deviate substantially from linear spin-wave theory, suggesting that magnon breakdown occurs in the material. Such a breakdown has been anticipated in recent theoretical studies, although the excitation spectrum remains to be accounted for.

cond-mat.str-el

Magnetically tunable dielectric materials

The coupling between localized spins and phonons can lead to shifts in the dielectric constant of insulating materials at magnetic ordering transitions. Studies on isostructural SeCuO3 (ferromagnetic) and TeCuO3 (antiferromagnetic) illustrate how the q-dependent spin-spin correlation function couples to phonon frequencies leading to a shift in the dielectric constant. A model is discussed for this spin-phonon coupling. The magnetodielectric coupling in multiferroic materials can be very large at a ferroelectric transition temperature. This coupling is investigated in the recently identified multiferroic Ni3V2O8.

cond-mat.mtrl-sci

Morphology Effectively Controls Singlet-Triplet Exciton Relaxation and Charge Transport in Organic Semiconductors

We present a comparative study of ultrafast photo-conversion dynamics in tetracene (Tc) and pentacene (Pc) single crystals and Pc films using optical pump-probe spectroscopy. Photo-induced absorption in Tc and Pc crystals is activated and temperature-independent respectively, demonstrating dominant singlet-triplet exciton fission. In Pc films (as well as C$_{60}$-doped films) this decay channel is suppressed by electron trapping. These results demonstrate the central role of crystallinity and purity in photogeneration processes and will constrain the design of future photovoltaic devices.

cond-mat.other

Doping a semiconductor to create an unconventional metal

Landau Fermi liquid theory, with its pivotal assertion that electrons in metals can be simply understood as independent particles with effective masses replacing the free electron mass, has been astonishingly successful. This is true despite the Coulomb interactions an electron experiences from the host crystal lattice, its defects, and the other ~1022/cm3 electrons. An important extension to the theory accounts for the behaviour of doped semiconductors1,2. Because little in the vast literature on materials contradicts Fermi liquid theory and its extensions, exceptions have attracted great attention, and they include the high temperature superconductors3, silicon-based field effect transistors which host two-dimensional metals4, and certain rare earth compounds at the threshold of magnetism5-8. The origin of the non-Fermi liquid behaviour in all of these systems remains controversial. Here we report that an entirely different and exceedingly simple class of materials - doped small gap semiconductors near a metal-insulator transition - can also display a non-Fermi liquid state. Remarkably, a modest magnetic field functions as a switch which restores the ordinary disordered Fermi liquid. Our data suggest that we have finally found a physical realization of the only mathematically rigourous route to a non-Fermi liquid, namely the 'undercompensated Kondo effect', where there are too few mobile electrons to compensate for the spins of unpaired electrons localized on impurity atoms9-12.

cond-mat.str-el

Soft Manifold Dynamics Behind Negative Thermal Expansion

Minimal models are developed to examine the origin of large negative thermal expansion (NTE) in under-constrained systems. The dynamics of these models reveals how underconstraint can organize a thermodynamically extensive manifold of low-energy modes which not only drives NTE but extends across the Brillioun zone. Mixing of twist and translation in the eigenvectors of these modes, for which in ZrW2O8 there is evidence from infrared and neutron scattering measurements, emerges naturally in our model as a signature of the dynamics of underconstraint.

cond-mat.mtrl-sci