arXiv subjects

S. L. Cooper

Publications and source records attributed to S. L. Cooper.

At least 19 recordsLinked to original sources

arXiv2019

Emergent Vibronic Excitations in the Magnetodielectric Regime of $\text{Ce}_2\text{O}_3$: Raman Scattering Studies

The strong coupling between spin, lattice and electronic degrees of freedom in magnetic materials can produce interesting phenomena, including multiferroic and magnetodielectric (MD) behavior, and exotic coupled excitations, such as electromagnons. We present a temperature- and magnetic-field-dependent inelastic light (Raman) scattering study that reveals the emergence of vibronic modes, i.e., coupled vibrational and crystal-electric-field (CEF) electronic excitations, in the unconventional rare-earth MD material, $\text{Ce}_2\text{O}_3$. The energies and intensities of these emergent vibronic modes are indicative of enhanced vibronic coupling and increased modulation of the dielectric susceptibility in the Néel state ($T_\text{N} \approx 6.2\,\text{K}$). The field-dependences of the energies and intensities of these vibronic modes are consistent with a decrease of both the vibronic coupling and the dielectric fluctuations associated with these modes below $T_\text{N}$. These results suggest a distinctive mechanism for MD behavior in $\text{Ce}_2\text{O}_3$ that is associated with a field-tunable coupling between CEF and phonon states.

cond-mat.str-el↗

arXiv2018

Real-Space Magnetic Imaging of the Multiferroic Spinels MnV2O4 and Mn3O4

Controlling multiferroic behavior in materials will enable the development of a wide variety of technological applications. However, the exact mechanisms driving multiferroic behavior are not well understood in most materials. Two such materials are the spinels MnV2O4 and Mn3O4, where mechanical strain is thought to play a role in determining magnetic behavior. Bulk studies of MnV2O4 have yielded conflicting and inconclusive results, due in part to the presence of mesoscale magnetic inhomogeneity, which complicates the interpretation of bulk measurements. To study the sub-micron-scale magnetic properties of Mn-based spinel materials, we performed magnetic force microscopy (MFM) on MnV2O4 samples subject to different levels of mechanical strain. We also used a crystal grain mapping technique to perform spatially registered MFM on Mn3O4. These local investigations revealed 100-nm-scale "stripe" modulations in the magnetic structure of both materials. In MnV2O4, the magnetization of these stripes is estimated to be Mz $\approx$ 105 A/m, which is on the order of the saturation magnetization reported previously. Cooling in a strong magnetic field eliminated the stripe patterning only in the low-strain sample of MnV2O4. The discovery of nanoscale magnetostructural inhomogeneity that is highly susceptible to magnetic field control in these materials necessitates both a revision of theoretical proposals and a reinterpretation of experimental data regarding the low-temperature phases and magnetic-field-tunable properties of these Mn-based spinels.

cond-mat.mtrl-sci↗

arXiv2016

Magnons and Magnetodielectric Effects in CoCr$_2$O$_4$: Raman Scattering Studies

Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$_2$O$_4$, is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. This paper reports an inelastic light scattering study of the magnon and phonon spectrum of CoCr$_2$O$_4$ as simultaneous functions of temperature, pressure, and magnetic field. Below the Curie temperature ($T_C \sim 94$ K) of CoCr$_2$O$_4$ we observe a $ω\sim 16 \,\text{cm}^{-1}$ $\boldsymbol q=0$ magnon having T$_{1g}$-symmetry, which has the transformation properties of an axial vector. The anomalously large Raman intensity of the T$_{1g}$-symmetry magnon is characteristic of materials with a large magneto-optical response and likely arises from large magnetic fluctuations that strongly modulate the dielectric response in CoCr$_2$O$_4$. The Raman susceptibility of the T$_{1g}$-symmetry magnon exhibits a strong magnetic-field dependence that is consistent with the magnetodielectric response observed in CoCr$_2$O$_4$, suggesting that magnetodielectric behavior in CoCr$_2$O$_4$ primarily arises from the field-dependent suppression of magnetic fluctuations that are strongly coupled to long-wavelength phonons. Increasing the magnetic anisotropy in CoCr$_2$O$_4$ with applied pressure decreases the magnetic field-dependence of the T$_{1g}$-symmetry magnon Raman susceptibility in CoCr$_2$O$_4$, suggesting that strain can be used to control the magnetodielectric response in CoCr$_2$O$_4$.

cond-mat.mtrl-sci↗

arXiv2016

Effects of magnetic field and twin domains on magnetostructural phase mixture in Mn3O4: Raman scattering studies of untwinned crystals

The ferrimagnetic spinel Mn3O4 exhibits large and anisotropic changes in electronic and structural properties in response to an applied magnetic field. These changes are thought to result from the field-dependent tuning---via strong spin-lattice coupling---between two nearly degenerate magnetostructural phases. Recent variable-magnetic-field studies of Mn3O4 have been performed on melt-grown crystals, which can exhibit twin domains due to a Jahn-Teller structural transition below the melting temperature. Because of the near degeneracy of the magnetostructural phases, however, strain associated with the twin domains likely affects the magnetic responses of Mn3O4. In this report, we present a variable-magnetic-field Raman scattering study of untwinned Mn3O4 crystals grown out of a flux below the Jahn-Teller structural transition. We measure distinct q = 0 magnetic and vibrational excitation spectra for each isolated magnetostructural phase of untwinned Mn3O4 crystals and determine the symmetries of the observed excitations. We determine how the magnetostructural phase mixture changes in response to magnetic fields applied in the magnetic easy plane. Lastly, by comparing results on flux- and melt-grown Mn3O4 crystals, we show that the intrinsic mixture of the two magnetostructural phases is indeed strongly influenced by the presence of twin domains.

cond-mat.str-el↗

arXiv2015

Isotropic and Anisotropic Regimes of the Field-Dependent Spin Dynamics in Sr2IrO4: Raman Scattering Studies

A major focus of experimental interest in Sr2IrO4 has been to clarify how the magnetic excitations of this strongly spin-orbit coupled system differ from the predictions of anisotropic 2D spin-1/2 Heisenberg model and to explore the extent to which strong spin-orbit coupling affects the magnetic properties of iridates. Here, we present a high-resolution inelastic light (Raman) scattering study of the low energy magnetic excitation spectrum of Sr2IrO4 and doped Eu-doped Sr2IrO4 as functions of both temperature and applied magnetic field. We show that the high-field (H>1.5 T) in-plane spin dynamics of Sr2IrO4 are isotropic and governed by the interplay between the applied field and the small in-plane ferromagnetic spin components induced by the Dzyaloshinskii-Moriya interaction. However, the spin dynamics of Sr2IrO4 at lower fields (H<1.5 T) exhibit important effects associated with interlayer coupling and in-plane anisotropy, including a spin-flop transition at Hc in Sr2IrO4 that occurs either discontinuously or via a continuous rotation of the spins, depending upon the in-plane orientation of the applied field. These results show that in-plane anisotropy and interlayer coupling effects play important roles in the low-field magnetic and dynamical properties of Sr2IrO4.

cond-mat.str-el↗

arXiv2015

Influence of Ti doping on the incommensurate charge density wave in 1T-TaS2

We report temperature-dependent transport and x-ray diffraction measurements of the influence of Ti hole doping on the charge density wave (CDW) in 1T-Ta(1-x)Ti(x)S(2). Confirming past studies, we find that even trace impurities eliminate the low-temperature commensurate (C) phase in this system. Surprisingly, the magnitude of the in-plane component of the CDW wave vector in the nearly commensurate (NC) phase does not change significantly with Ti concentration, as might be expected from a changing Fermi surface volume. Instead, the angle of the CDW in the basal plane rotates, from 11.9 deg at x=0 to 16.4 deg at x=0.12. Ti substitution also leads to an extended region of coexistence between incommensurate (IC) and NC phases, indicating heterogeneous nucleation near the transition. Finally, we explain a resistive anomaly originally observed by DiSalvo [F. J. DiSalvo, et al., Phys. Rev. B {\bf 12}, 2220 (1975)] as arising from pinning of the CDW on the crystal lattice. Our study highlights the importance of commensuration effects in the NC phase, particularly at x ~ 0.08.

cond-mat.str-el↗

arXiv2015

Magnon spectra and strong spin-lattice coupling in magnetically frustrated MnB2O4 (B = Mn,V): Inelastic light scattering studies

The ferrimagnetic spinels MnB2O4 (B = Mn,V) exhibit a similar series of closely spaced magnetic and structural phase transitions at low temperatures, reflecting both magnetic frustration and a strong coupling between the spin and lattice degrees of freedom. Careful studies of excitations in MnB2O4 (B = Mn,V), and the evolution of these excitations with temperature, are important for obtaining a microscopic description of the role that magnetic excitations and spin-lattice coupling play in the low temperature phase transitions of these materials. We report an inelastic light (Raman) scattering study of the temperature and magnetic field dependences of one- and two-magnon excitations in MnV2O4 and Mn3O4. We observe a pair of q=0 one-magnon modes at 74 cm^{-1} and 81 cm^{-1} in MnV2O4, which is in contrast with the single 80 cm^{-1} q=0 magnon that has been reported for MnV2O4 based on previous neutron scattering measurements and spin wave calculations. Additionally, we find that the two-magnon energy of MnV2O4 decreases ("softens") with decreasing temperature below T_{N}, which we attribute to strong coupling between magnetic and vibrational excitations near the zone boundary.

cond-mat.str-el↗

arXiv2015

Structural contributions to the pressure-tuned charge-density-wave to superconductor transition in ZrTe3: Raman scattering studies

Superconductivity evolves as functions of pressure or doping from charge-ordered phases in a variety of strongly correlated systems, suggesting that there may be universal characteristics associated with the competition between superconductivity and charge order in these materials. We present an inelastic light (Raman) scattering study of the structural changes that precede the pressure-tuned charge-density-wave (CDW) to superconductor transition in one such system, ZrTe3. In certain phonon bands, we observe dramatic linewidth reductions that accompany CDW formation, indicating that these phonons couple strongly to the electronic degrees of freedom associated with the CDW. The same phonon bands, which represent internal vibrations of ZrTe3 prismatic chains, are suppressed at pressures above ~10 kbar, indicating a loss of long-range order within the chains, specifically amongst intrachain Zr-Te bonds. These results suggest a distinct structural mechanism for the observed pressure-induced suppression of CDW formation and provide insights into the origin of pressure-induced superconductivity in ZrTe3.

cond-mat.str-el↗

arXiv2013

Emergence of charge density wave domain walls above the superconducting dome in TiSe2

Superconductivity (SC) in so-called "unconventional superconductors" is nearly always found in the vicinity of another ordered state, such as antiferromagnetism, charge density wave (CDW), or stripe order. This suggests a fundamental connection between SC and fluctuations in some other order parameter. To better understand this connection, we used high-pressure x-ray scattering to directly study the CDW order in the layered dichalcogenide TiSe2, which was previously shown to exhibit SC when the CDW is suppressed by pressure [1] or intercalation of Cu atoms [2]. We succeeded in suppressing the CDW fully to zero temperature, establishing for the first time the existence of a quantum critical point (QCP) at Pc = 5.1 +/- 0.2 GPa, which is more than 1 GPa beyond the end of the SC region. Unexpectedly, at P = 3 GPa we observed a reentrant, weakly first order, incommensurate phase, indicating the presence of a Lifshitz tricritical point somewhere above the superconducting dome. Our study suggests that SC in TiSe2 may not be connected to the QCP itself, but to the formation of CDW domain walls.

cond-mat.supr-con↗

arXiv2012

Inelastic light scattering measurements of a pressure-induced quantum liquid in KCuF$_3$

Pressure-dependent, low temperature inelastic light (Raman) scattering measurements of KCuF$_3$ show that applied pressure above $P^{*} \sim$ 7 kbar suppresses a previously observed structural phase transition temperature to zero temperature in KCuF$_3$, resulting in the development of a $ω\sim$ 0 fluctuational (quasielastic) response near $T \sim$ 0 K. This pressure-induced fluctuational response --- which we associate with slow fluctuations of the CuF$_6$ octahedral orientation --- is temperature independent and exhibits a characteristic fluctuation rate that is much larger than the temperature, consistent with quantum fluctuations of the CuF$_6$ octahedra. A model of pseudospin-phonon coupling provides a qualitative description of both the temperature- and pressure-dependent evolution of the Raman spectra of KCuF$_3$.

cond-mat.str-el↗

arXiv2011

Pressure- and Field-Tuning the Magnetostructural Phases of Mn3O4: Raman Scattering and X-Ray Diffraction Studies

We present temperature-, magnetic-field-, and pressure-dependent Raman scattering studies of single crystal Mn3O4, combined with temperature- and field-dependent x-ray diffraction studies, revealing the novel magnetostructural phases in Mn3O4. Our temperature-dependent studies showed that the commensurate magnetic transition at T2=33K in the binary spinel Mn3O4 is associated with a structural transition from tetragonal to orthorhombic structures. Field-dependent studies showed that the onset and nature of this structural transition can be controlled with an applied magnetic field, and revealed evidence for a field-tuned quantum phase transition to a tetragonal spin-disordered phase for H||[1-10]. Pressure-dependent Raman measurements showed that the magnetic easy axis direction in Mn3O4 can be controlled---and the ferrimagnetic transition temperature increased---with applied pressure. Finally, combined pressure- and magnetic-field-tuned Raman measurements revealed a rich magnetostructural phase diagram---including a pressure- and field-induced magnetically frustrated tetragonal phase in the PH phase diagram---that can be generated in Mn3O4 with applied pressure and magnetic field.

cond-mat.str-el↗

arXiv2009

Mapping the magneto-structural quantum phases of Mn3O4

We present temperature-dependent x-ray diffraction and temperature- and field-dependent Raman scattering studies of single crystal Mn3O4, which reveal the novel magnetostructural phases that evolve in the spinels due to the interplay between strong spin-orbital coupling, geometric frustration, and applied magnetic field. We observe a structural transition from tetragonal to monoclinic structures at the commensurate magnetic transition at T2=33K, show that the onset and nature of this structural transition can be controlled with an applied magnetic field, and find evidence for a field-tuned quantum phase transition to a tetragonal incommensurate or spin glass phase.

cond-mat.str-el↗

arXiv2008

Raman scattering studies of temperature- and field-induced melting of charge order in (La,Pr,Ca)MnO$_{3}$

We present Raman scattering studies of the structural and magnetic phases that accompany temperature- and field-dependent melting of charge- and orbital-order (COO) in La0.5Ca0.5MnO3 and La0.25Pr0.375Ca0.375MnO3. Our results show that thermal and field-induced COO melting in La0.5Ca0.5MnO3 exhibits three stages in a heterogeneous melting process associated with a structural change: a long-range, strongly JT distorted/COO regime; a coexistence regime; and weakly JT distorted/PM or FM phase. We provide a complete structural phase diagram of La0.5Ca0.5MnO3 for the temperature and field ranges 6<=T<=170 K and 0<=H<=9 T. We also investigate thermal and field-induced melting in La0.25Pr0.375Ca0.375MnO3 to elucidate the role of disorder in melting of COO. We find that while thermal melting of COO in La0.25Pr0.375Ca0.375MnO3 is quite similar to that in La0.5Ca0.5MnO3, the field-induced transition from the COO phase to the weakly JT-distorted/FM phase in La0.25Pr0.375Ca0.375MnO3 is very abrupt, and occurs at significantly lower fields (H~2 T at T~0 K) than in La0.5Ca0.5MnO3 (H~30 T at T=0 K). Moreover, the critical field H_c increases with increasing temperature in La0.25Pr0.375Ca0.375MnO3 in contrast to La0.5Ca0.5MnO3. To explain these differences, we propose that field-induced melting of COO in La0.25Pr0.375Ca0.375MnO3 is best described as the field-induced percolation of FM domains, and we suggest that Griffiths phase physics may be an appropriate theoretical model for describing the unusual temperature- and field- dependent transitions observed in La0.25Pr0.375Ca0.375MnO3.

cond-mat.str-el↗

arXiv2007

Quantum and classical mode softening near the charge-density-wave/superconductor transition of Cu$_{x}$TiSe$_{2}$: Raman spectroscopic studies

Temperature- and x-dependent Raman scattering studies of the charge density wave (CDW) amplitude modes in CuxTiSe2 show that the amplitude mode frequency omega_o exhibits identical power-law scaling with the reduced temperature, T/T_CDW, and the reduced Cu content, x/x_c, i.e., omega_o ~ (1 - p)^0.15 for p = T/T_CDW or x/x_c, suggesting that mode softening is independent of the control parameter used to approach the CDW transition. We provide evidence that x-dependent mode softening in CuxTiSe2 is caused by the reduction of the electron-phonon coupling constant lambda due to expansion of the lattice, and that x-dependent `quantum' (T ~ 0) mode softening reveals a quantum critical point within the superconductor phase of CuxTiSe2.

cond-mat.str-el↗

arXiv2007

Metal to insulator transition in manganites - optical conductivity changes up to 24 eV

The electronic response of doped manganites at the transition from the paramagnetic insulating to the ferromagnetic metallic state in $\rm La_{1-x}Ca_{x}MnO_3$ for $\rm (x=0.3,0.2)$ was investigated by dc conductivity, ellipsometry, and VUV reflectance for energies between 0 and 24 eV. A stablized Kramers-Kronig transformation yields the optical conductivity and reveals changes in the optical spectral weight up to 24 eV at the metal to insulator transition. In the observed energy range, the spectral weight is conserved within $\rm 0.3 %$. The redistribution of spectral weight between low and high energies has important ramifications for the down-folding of low-energy Hamiltonians. We discuss the importance of the charge-transfer, Coulomb onsite, Jahn-Teller, and screening effects to the electronic structure.

cond-mat.str-el↗

arXiv2006

Field- and pressure-induced phases in Sr$_{4}$Ru$_{3}$O$_{10}$: A spectroscopic investigation

We have investigated the magnetic-field- and pressure-induced structural and magnetic phases of the triple-layer ruthenate - Sr$_{4}$Ru$_{3}$O$_{10}$. Magnetic-field-induced changes in the phonon spectra reveal dramatic spin-reorientation transitions and strong magneto-elastic coupling in this material. Additionally, pressure-dependent Raman measurements at different temperatures reveal an anomalous negative Gruneisen-parameter associated with the B$_{1g}$ mode ($\sim$ 380 cm$^{-1}$) at low temperatures (T $<$ 75K), which can be explained consistently with the field dependent Raman data.

cond-mat.str-el↗

arXiv2005

Optical sum rules that relate to the potential energy of strongly correlated systems

A class of sum rules for inelastic light scattering is developed. We show that the first moment of the non-resonant response provides information about the potential energy in strongly correlated systems. The polarization dependence of the sum rules provide information about the electronic excitations in different regions of the Brillouin zone. We determine the sum rule for the Falicov-Kimball model, which possesses a metal-insulator transition, and compare our results to the light scattering experiments in SmB_6.

cond-mat.str-el↗

arXiv2005

Lattice dynamics and the electron-phonon interaction in Ca$_2$RuO$_4$

We present a Raman scattering study of Ca$_2$RuO$_4$, in which we investigate the temperature-dependence of the lattice dynamics and the electron-phonon interaction below the metal-insulator transition temperature ({\it T}$_{\rm MI}$). Raman spectra obtained in a backscattering geometry with light polarized in the ab-plane reveal 9 B$_{1g}$ phonon modes (140, 215, 265, 269, 292, 388, 459, 534, and 683 cm$^{-1}$) and 9 A$_g$ phonon modes (126, 192, 204, 251, 304, 322, 356, 395, and 607 cm$^{-1}$) for the orthorhombic crystal structure (Pbca$-$D$_{2h}^{15}$). With increasing temperature toward {\it T}$_{\rm MI}$, the observed phonon modes shift to lower energies and exhibit reduced spectral weights, reflecting structural changes associated with the elongation of the RuO$_6$ octahedra. Interestingly, the phonons exhibit significant increases in linewidths and asymmetries for {\it T} $>$ {\it T}$_{\rm N}$. These results indicate that there is an increase in the effective number of electrons and the electron-phonon interaction strengths as the temperature is raised through {\it T}$_{\rm N}$, suggesting the presence of orbital fluctuations in the temperature regime {\it T}$_{\rm N}$ $<$ {\it T} $<$ {\it T}$_{\rm MI}$.

cond-mat.str-el↗