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Naween Anand

Publications and source records attributed to Naween Anand.

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Magnetic field tuning of crystal field levels and vibronic states in Spin-ice Ho$_2$Ti$_2$O$_7$ observed in far-infrared reflectometry

Low temperature optical spectroscopy in applied magnetic fields provides clear evidence of magnetoelastic coupling in the spin ice material Ho$_2$Ti$_2$O$_7$. In far-IR reflectometry measurements, we observe field dependent features around 30, 61, 72 and 78~meV, energies corresponding to crystal electronic field (CEF) doublets. The calculations of the crystal-field Hamiltonian model confirm that the observed features in IR spectra are consistent with magnetic-dipole-allowed excitations from the ground state to higher $^5$I$_8$ CEF levels. We present the CEF parameters that best describe our field-dependent IR reflectivity measurements. Additionally, we identify a weak field-dependent shoulder near one of the CEF doublets. This indicates that this level is split even in zero-field, which we associate with a vibronic bound state. Modeling of the observed splitting shows that the phonon resides at slightly lower energy compared to the CEF level that it couples to, which is in contrast with previously published inelastic neutron measurements. The magnetic field dependence of the vibronic state shows a gradual decoupling of the phonon with the CEF level as it shifts. This approach should work in pyrochlores and other systems that have magnetic dipole transitions in the IR spectroscopic range, which can elucidate the presence and the ability to tune the nature of vibronic states in a wide variety of materials.

cond-mat.str-el

Investigation of the monopole magneto-chemical potential in spin ices using capacitive torque magnetometry

The single-ion anisotropy and magnetic interactions in spin-ice systems give rise to unusual non-collinear spin textures, such as Pauling states and magnetic monopoles. The effective spin correlation strength ($J_{eff}$) determines the relative energies of the different spin-ice states. With this work, we display the capability of capacitive torque magnetometry in characterizing the magneto-chemical potential associated with monopole formation. We build a magnetic phase diagram of Ho$_2$Ti$_2$O$_7$, and show that the magneto-chemical potential depends on the spin-sublattice ($α$ or $β$), i.e., the Pauling state, involved in the transition. Monte-Carlo simulations using the dipolar-spin-ice Hamiltonian support our findings of a sublattice-dependent magneto-chemical potential, but the model underestimates the $J_{eff}$ for the $β$-sublattice. Additional simulations, including next-nearest neighbor interactions ($J_2$), show that long-range exchange terms in the Hamiltonian are needed to describe the measurements. This demonstrates that torque magnetometry provides a sensitive test for $J_{eff}$ and the spin-spin interactions that contribute to it.

cond-mat.str-el

High-throughput search for magnetic topological materials using spin-orbit spillage, machine-learning and experiments

Magnetic topological insulators and semi-metals have a variety of properties that make them attractive for applications including spintronics and quantum computation, but very few high-quality candidate materials are known. In this work, we use systematic high-throughput density functional theory calculations to identify magnetic topological materials from 40000 three-dimensional materials in the JARVIS-DFT database (https://jarvis.nist.gov/jarvisdft). First, we screen materials with net magnetic moment > 0.5 μB and spin-orbit spillage > 0.25, resulting in 25 insulating and 564 metallic candidates. The spillage acts as a signature of spin-orbit induced band-inversion. Then, we carry out calculations of Wannier charge centers, Chern numbers, anomalous Hall conductivities, surface bandstructures, and Fermi-surfaces to determine interesting topological characteristics of the screened compounds. We also train machine learning models for predicting the spillage, bandgaps, and magnetic moments of new compounds, to further accelerate the screening process. We experimentally synthesize and characterize a few candidate materials to support our theoretical predictions.

cond-mat.mtrl-sci

Large anomalous Nernst and inverse spin-Hall effects in epitaxial thin films of Kagome semimetal Mn$_3$Ge

Synthesis of crystallographically well-defined thin films of topological materials is important for unraveling their mesoscale quantum properties and for device applications. Mn$_3$Ge, an antiferromagnetic Weyl semimetal with a chiral magnetic structure on a Kagome lattice, is expected to have enhanced Berry curvature around Weyl nodes near the Fermi energy, leading to large anomalous Hall / Nernst effects and a large spin-Hall effect. Using magnetron sputtering, we have grown epitaxial thin films of hexagonal D0$_{19}$ Mn$_3$Ge that are flat and continuous. Large anomalous Nernst and inverse spin-Hall effects are observed in thermoelectric and spin-pumping devices. The anomalous Nernst signal in our Mn$_3$Ge films is estimated to be 0.1 $μ$V / K, and is comparable to that in ferromagnetic Fe, despite Mn$_3$Ge having a weak magnetization of ~3.5 m$μ_B$ at room temperature. The spin mixing conductance is 90.5 nm$^{-2}$ at the Py / Mn$_3$Ge interface, and the spin-Hall angle in Mn$_3$Ge is estimated to be about 8 times of that in Pt.

cond-mat.mtrl-sci

Modification of Spin Ice Physics in Ho$_2$Ti$_2$O$_7$ Thin Films

We present an extensive study on the effect of substrate orientation, strain, stoichiometry and defects on spin ice physics in Ho$_2$Ti$_2$O$_7$ thin films grown onto yttria-stabilized-zirconia substrates. We find that growth in different orientations produces different strain states in the films. All films exhibit similar c-axis lattice parameters for their relaxed portions, which are consistently larger than the bulk value of 10.10 Å. Transmission electron microscopy reveals anti-site disorder and growth defects to be present in the films, but stuffing is not observed. The amount of disorder depends on the growth orientation, with the (110) film showing the least. Magnetization measurements at 1.8 K show the expected magnetic anisotropy and saturation magnetization values associated with a spin ice for all orientations; shape anisotropy is apparent when comparing in and out-of-plane directions. Significantly, only the (110) oriented films display the hallmark spin ice plateau state in magnetization, albeit less well-defined compared to the plateau observed in a single crystal. Neutron scattering maps on the more disordered (111) oriented films show the Q=0 phase previously observed in bulk materials, but the Q=X phase giving the plateau state remains elusive. We conclude that the spin ice physics in thin films is modified by defects and strain, leading to a reduction in the temperature at which correlations drive the system into the spin ice state.

cond-mat.str-el

Probing Anomalous Inelastic Scattering in Spin-ice Ho$_2$Ti$_2$O$_7$ through Resonant Raman Spectroscopy

We report on a study of the inelastic scattering properties of (001) and (111) Ho$_2$Ti$_2$O$_7$ single crystals at room temperature. Structural and compositional analysis along with absorption measurement confirms single crystalline phase of all samples. Room temperature polarized Raman measurements were performed on crystals in non-resonant and two different resonant conditions by using six different laser excitation lines. Lorentzian model fitting analysis is performed on all measured spectra in order to identify the difference in the Raman scattering cross-section in resonant and non-resonant conditions. Variations in the fitting parameters on account of different polarization configurations and crystallographic orientations has helped identifying their symmetry if present. Several possible scattering pathways are discussed in order to qualitatively explain the anomalous scattering results in Ho$_2$Ti$_2$O$_7$

cond-mat.str-el

Far-infrared absorption of undoped and Br-doped carbon nanofiber powder in stacked-cup cone configuration

We carried out room-temperature far-infrared (40--650~cm$^{-1}$) transmission measurements on undoped and bromine-doped powder samples of carbon nanofibers in stacked-cup cone geometry. The transmission spectra of both doped and undoped samples were fit to a Drude-Lorentz model. A single Drude component and a small bandgap (around 8~meV) semiconducting Lorentzian component along with 3 other Lorentz components were essential to get a good fit in the entire measured frequency range. A decreased metallic conductivity along with a red-shift of the lowest semiconducting gap was found after bromine doping. A significant decrease in the scattering rate upon heavy doping has been qualitatively explained as partial ordering of intercalated dopant ions. Absorption spectra were derived from the transmission spectra under the assumption of non-dispersive reflectance. These spectra were compared to Drude-Lorentz model absorption spectra. The free-carrier density of the n-type powder and the electronic mean free path were estimated and compared with previously reported values for single-walled nanotubes and pyrolytic graphite.

cond-mat.mes-hall

Temperature evolution of polaron dynamics and Jahn-Teller distortion modes in strongly correlated La$_{0.67}$Ca$_{0.33}$MnO$_{3}$ manganite film

Reflectivity as a function of temperature for the La$_{0.67}$Ca$_{0.33}$MnO$_{3}$ (LCMO) film has been measured across the metal-insulator phase transition. The optical properties and their temperature dependence were determined in the infrared and visible range by fits to a Drude-Lorentz model, using exact formula for the thin film optics and the measured properties of the substrate. The phonon modes were identified and verified with lattice dynamical calculations for the ideal and distorted perovskite structure of the material. The optical conductivity shows agreement with the double exchange mechanism in conjunction with the Jahn-Teller distortion term in the Hamiltonian. Low temperature metallic phase is dominated by large polaron dynamics, a key component of electron-orbital coupling in a strongly corrrelated system. Free carrier dynamics in the metallic phase is described in terms of coherent heavy polaronic motion in the DC limit with incoherent and asymmetric polaronic background in the mid-IR range. The strength and line width of Jahn-Teller modes has been discussed across the phase transition and their temperature evolution is qualitatively discussed on account of existing electron-phonon coupling. The localized Holstein polaron formation in the high temperature insulative phase is identified as optical conductivity peaks in the visible range above the critical temperature.

cond-mat.str-el

Study of magneto-transport properties and quantum oscillations in PbSe single crystals

PbSe is a low-gap semiconductor with excellent infrared photo-detection properties. Here we report our high magnetic field and low temperature electrical properties measurement performed on a moderately doped PbSe single crystals with p-type bulk carrier density of around $1\times10^{18}$ cm$^{-3}$. Longitudinal resistance (R$_{xx}$) and Hall resistance (R$_{xy}$) were simultaneously measured between 0 T--18 T at several temperatures between 0.8 K--25 K. These transport measurements start showing oscillatory behavior around and above 6 T of magnetic field. The quantum oscillation frequency is ~15 T, giving an estimate for the carrier density of each L pocket in the BZ participating in these oscillations. The effective mass of the free carriers is estimated from the temperature dependence of oscillation amplitudes. Measurements as the magnetic fields is rotated reveal the magneto-transport properties of a 3D-like fermi surface. Free carrier scattering rate from the transport data has been estimated which also gave an estimation of Dingle temperature in PbSe. Room temperature optical measurements has been conducted and other optical properties has been estimated. The Drude-Lorentz model fit has been performed which show a low frequency phonon mode around 45 cm$^{-1}$ and bandgap of around 0.2 eV along with other interband electronic transitions. Some of the optical and transport results has been compared against other members of class IV-VI chalcogenides.

cond-mat.mes-hall

Temperature-driven band inversion in Pb$_{0.77}$Sn$_{0.23}$Se: Optical and Hall-effect studies

Optical and Hall-effect measurements have been performed on single crystals of Pb$_{0.77}$Sn$_{0.23}$Se, a IV-VI mixed chalcogenide. The temperature dependent (10--300 K) reflectance was measured over 40--7000 cm$^{-1}$ (5--870 meV) with an extension to 15,500 cm$^{-1}$ (1.92 eV) at room temperature. The reflectance was fit to the Drude-Lorentz model using a single Drude component and several Lorentz oscillators. The optical properties at the measured temperatures were estimated via Kramers-Kronig analysis as well as by the Drude-Lorentz fit. The carriers were p-type with the carrier density determined by Hall measurements. A signature of valence intraband transition is found in the low-energy optical spectra. It is found that the valence-conduction band transition energy as well as the free carrier effective mass reach minimum values at 100 K, suggesting temperature-driven band inversion in the material. Density function theory calculation for the electronic band structure also make similar predictions.

cond-mat.str-el