arXiv subjects

J. R. Simpson

Publications and source records attributed to J. R. Simpson.

14 recordsLinked to original sources

arXiv2024

Spin-Orbital-Lattice Coupling and the Phonon Zeeman Effect in the Dirac Honeycomb Magnet CoTiO$_3$

The entanglement of electronic spin and orbital degrees of freedom is often the precursor to emergent behaviors in condensed matter systems. With considerable spin-orbit coupling strength, the cobalt atom on a honeycomb lattice offers a platform that can make accessible the study of novel magnetic ground states. Using temperature-dependent Raman spectroscopy and high-magnetic field Raman and infrared (IR) spectroscopy, we studied the lattice and spin-orbital excitations in CoTiO$_3$, an antiferromagnetic material that exhibits topologically protected magnon Dirac crossings in the Brillouin zone. Under the application of an external magnetic field up to 22 T along the crystal's $c$-axis, we observed the splitting of both the spin-orbital excitations and a phonon nearby in energy. Using density functional theory (DFT), we identify a number of new modes that below the antiferromagnetic (AFM) transition become Raman-active due to the zone-folding of the Brillouin zone caused by the doubling of the magnetic unit cell. We use a model that includes both the spin and orbital degrees of freedom of the Co$^{2+}$ ions to explain the spin-orbital excitation energies and their behavior in an applied field. Our experimental observations along with several deviations from the model behavior point to significant coupling between the spin-orbital and the lattice excitations.

cond-mat.str-el↗

arXiv2024

Ring-Exchange Interaction Effects on Magnons in Dirac Magnet CoTiO$_3$

The magnetic interactions that determine magnetic order and magnon energies typically involve only two spins. While rare, multi-spin interactions can also appear in quantum magnets and be the driving force in the ground state selection and in the nature of its excitations. By performing time-domain terahertz and magneto-Raman spectroscopy measurements combined with theoretical modeling, we determine the origin of the magnon excitation gap in Dirac antiferromagnet CoTiO$_3$. By adding a ring-exchange interaction in a hexagonal plaquette of the honeycomb lattice to both an XXZ spin model and to a low energy spin-orbital flavor wave model, a gap is generated in the magnon spectrum at the Brillouin zone center. With this addition, the flavor wave model reproduces a large swath of experimental results including terahertz, Raman, inelastic neutron scattering, and magnetization experiments.

cond-mat.str-el↗

arXiv2020

Magnon-phonon hybridization in quasi-2D antiferromagnet MnPSe$_3$

Magnetic excitations in van der Waals (vdW) materials, especially in the two-dimensional (2D) limit, are an exciting research topic from both the fundamental and applied perspectives. Using temperature-dependent, magneto-Raman spectroscopy, we identify the hybridization of two-magnon excitations with two separate E$_\mathrm{g}$ phonons in MnPSe$_3$, a magnetic vdW material that could potentially host 2D antiferromagnetism. Results from first principles calculations of the phonon and magnon spectra further support our identification. The Raman spectra's rich temperature dependence through the magnetic transition displays an avoided-crossing behavior in the phonons' frequency and a concurrent decrease in their lifetimes. We construct a model based on the interaction between a discrete level and a continuum that reproduces these observations. The strong magnon-phonon hybridization reported here highlights the need to understand its effects on spin transport experiments in magnetic vdW materials.

cond-mat.mtrl-sci↗

arXiv2019

Polarization-resolved Raman spectroscopy of α-RuCl3 and evidence of room temperature two-dimensional magnetic scattering

Polarization-resolved Raman spectroscopy was performed and analyzed from large, high quality, mono-domain single crystal of α-RuCl3, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a 4-fold or 2-fold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as C2h. The low frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is 2-dimensional. We argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.

cond-mat.str-el↗

arXiv2008

Length-dependent Raman spectroscopy of single-walled carbon nanotubes: the effect of dispersant on defects

We compare Raman spectra from aqueous suspensions of length-separated single-walled carbon nanotubes (SWCNTs) dispersed using either polymer adsorption of single-stranded DNA or miscelle encapsulation with sodium deoxycholate surfactant. The Raman spectral features, other than the D-band, increase monotonically with nanotube length in both dispersion schemes. The intensity ratio of the disorder-induced D to G' Raman bands decays as a function of SWCNT length, proportional to 1/L, as expected for endcap defects. While the UV-vis absorption and fluorescence also increase with length for both dispersants, the fluorescence intensity is dramatically lower for DNA-wrapped SWCNTs of equal length. The similarities in the length-dependent D/G' ratios exclude defects as an explanation for the fluorescence decrease in DNA versus deoxycholate dispersions.

cond-mat.mtrl-sci↗

arXiv2003

Optical band edge shift of anatase cobalt-doped titanium dioxide

We report on the optical properties of magnetic cobalt-doped anatase phase titanium dioxide Ti_{1-x}Co_{x}O_{2-d} films for low doping concentrations, 0 <= x <= 0.02, in the spectral range 0.2 to 5 eV. For well oxygenated films (d << 1) the optical conductivity is characterized by an absence of optical absorption below an onset of interband transitions at 3.6 eV and a blue shift of the optical band edge with increasing Co concentration. The absence of below band gap absorption is inconsistent with theoretical models which contain midgap magnetic impurity bands and suggests that strong on-site Coulomb interactions shift the O-band to Co-level optical transitions to energies above the gap.

cond-mat.str-el↗

arXiv2003

Exchange interaction effects on the optical properties of LuMnO3

We have measured the optical conductivity of single crystal LuMnO3 from 10 to 45000 cm-1 at temperatures between 4 and 300 K. A symmetry allowed on-site Mn $d$-$d$ transition near 1.7 eV is observed to blue shift (~0.1 eV) in the antiferromagnetic state due to Mn-Mn superexchange interactions. Similar anomalies are observed in the temperature dependence of the TO phonon frequencies which arise from spin-phonon interaction. We find that the known anomaly in temperature dependence of the quasi-static dielectric constant epsilon_0 below the T_N ~90 K is overwhelmingly dominated by the phonon contributions.

cond-mat.str-el↗

arXiv2003

Temperature dependent optical studies of Ti$_{1-x}$Co$_x$O$_2$

We present the results of Raman and photoluminescence (PL) studies on epitaxial anatase phase Ti$_{1-x}$Co$_x$O$_2$ films for $x$ = 0-0.07, grown by pulsed laser deposition. The low doped system ($x$=0.01 and 0.02) shows a Curie temperature of ~700 K in the as-grown state. The Raman spectra from the doped and undoped films confirm their anatase phase. The photoluminescence spectrum is characterized by a broad emission from self-trapped excitons (STE) at 2.3 eV at temperatures below 120 K. This peak is characteristic of the anatase-phase TiO$_2$ and shows a small blueshift with increasing doping concentration. In addition to the emission from STE, the Co-doped samples show two emission lines at 2.77 eV and 2.94 eV that are absent in the undoped film indicative of a spin-flip energy.

cond-mat.mtrl-sci↗

arXiv2003

High Temperature Ferromagnetism with Giant Magnetic Moment in Transparent Co-doped SnO2-d

Occurrence of room temperature ferromagnetism is demonstrated in pulsed laser deposited thin films of Sn1-xCoxO2-d (x<0.3). Interestingly, films of Sn0.95Co0.05O2-d grown on R-plane sapphire not only exhibit ferromagnetism with a Curie temperature close to 650 K, but also a giant magnetic moment of about 7 Bohr-Magneton/Co, not yet reported in any diluted magnetic semiconductor system. The films are semiconducting and optically highly transparent.

cond-mat↗

arXiv2002

Ferromagnetism in laser deposited anatase Ti$_{1-x}$Co$_{x}$O$_{2-$δ$}$ films

Pulsed laser deposited films of Co doped anatase TiO2 are examined for Co substitutionality, ferromagnetism, transport, magnetotransport and optical properties. Our results show limited solubility (up to ~ 2 %) of Co in the as-grown films and formation of Co clusters thereafter. For Ti0.93Co0.07O2-d sample, which exhibits a Curie temperature (Tc) over 1180 K, we find the presence of 20-50 nm Co clusters as well as a small concentration of Co incorporated into the remaining matrix. After being subjected to the high temperature anneal during the first magnetization measurement, the very same sample shows a Tc ~ 650 K and almost full matrix incorporation of Co. This Tc is close to that of as-grown Ti0.99Co0.01O2-d sample (~ 700 K). The transport, magnetotransport and optical studies also reveal interesting effects of the matrix incorporation of Co. These results are indicative of an intrinsic Ti1-xCoxO2-d diluted magnetic semiconductor with Tc of about 650-700 K.

cond-mat↗

arXiv2001

Temperature Dependence of Low-Lying Electronic Excitations of LaMnO_3

We report on the optical properties of undoped single crystal LaMnO_3, the parent compound of the colossal magneto-resistive manganites. Near-Normal incidence reflectance measurements are reported in the frequency range of 20-50,000 cm-1 and in the temperature range 10-300 K. The optical conductivity, s_1(w), is derived by performing a Kramers-Kronig analysis of the reflectance data. The far-infrared spectrum of s_1(w) displays the infrared active optical phonons. We observe a shift of several of the phonon to high frequencies as the temperature is lowered through the Neel temperature of the sample (T_N = 137 K). The high-frequency s_1(w) is characterized by the onset of absorption near 1.5 eV. This energy has been identified as the threshold for optical transitions across the Jahn-Teller split e_g levels. The spectral weight of this feature increases in the low-temperature state. This implies a transfer of spectral weight from the UV to the visible associated with the paramagnetic to antiferromagnetic state. We discuss the results in terms of the double exchange processes that affect the optical processes in this magnetic material.

cond-mat.str-el↗

arXiv1999

Temperature dependent scattering rate and optical mass of ferromagnetic metallic manganites

We report on the optical properties of the hole-doped manganites La_0.7Ca_0.3MnO_3 and La_0.7Ca_0.3MnO_3. Transmission and reflection of thin films are measured in the infrared at temperatures from 10 - 150 K using Fourier-transform spectroscopy. The scattering rate and optical mass are obtained by fitting the far-infrared transmission to a Drude model. The scattering rate shows a T^2 dependence with temperature. The optical mass enhancement differs only slightly from specific heat results. In addition, we compare the infrared spectral weight to band structure calculations [M. Quijada et al., Phys. Rev. B 58, 16093 (1998)].

cond-mat.str-el↗

arXiv1999

Mid-infrared Hall effect in thin-film metals: Probing the Fermi surface anisotropy in Au and Cu

A sensitive mid-infrared (MIR, 900-1100 cm-1, 112-136 meV) photo-elastic polarization modulation technique is used to measure simultaneously Faraday rotation and circular dichroism in thin metal films. These two quantities determine the complex AC Hall conductivity. This novel technique is applied to study Au and Cu thin films at temperatures down to 20 K and magnetic fields up to 8 T. The Hall frequency is consistent with band theory predictions. We report the first measurement of the MIR Hall scattering rate, which is significantly lower than that derived from Drude analysis of zero magnetic field MIR transmission measurements. This difference is qualitatively explained in terms of the anisotropy of the Fermi surface in Au and Cu.

cond-mat.mtrl-sci↗

arXiv1998

Optical Conductivity of Manganites: Crossover from Jahn-Teller Small Polaron to Coherent Transport in the Ferromagnetic State

We report on the optical properties of the hole-doped manganites Nd_{0.7}Sr _{0.3}MnO_{3}, La_{0.7}Ca_{0.3}MnO_{3}, and La_{0.7}Sr_{0.3}MnO_{3}. The low-energy optical conductivity in the paramagnetic-insulating state of these materials is characterized by a broad maximum near 1 eV. This feature shifts to lower energy and grows in optical oscillator strength as the temperature is lowered into the ferromagnetic state. It remains identifiable well below Tc and transforms eventually into a Drude-like response. This optical behavior and the activated transport in the paramagnetic state of these materials are consistent with a Jahn-Teller small polaron. The optical spectra and oscillator strength changes compare well with models that include both double exchange and the dynamic Jahn-Teller effect in the description of the electronic structure.

cond-mat.str-el↗