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Register a new userComparative Study of Optical and Magneto-Optical Properties of Normal, Disordered and Inverse Spinel Type Oxides
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Co$_3$O$_4$, ZnFe$_2$O$_4$, CoFe$_2$O$_4$, ZnCo$_2$O$_4$, and Fe$_3$O$_4$ thin films were fabricated by pulsed laser deposition at high and low temperatures resulting in crystalline single-phase normal, inverse, as well as disordered spinel oxide thin films with smooth surface morphology. The dielectric function, determined by spectroscopic ellipsometry in a wide spectral range from 0.5 eV to 8.5 eV, is compared with the magneto-optical response of the dielectric tensor, investigated by magneto-optical Kerr effect (MOKE) spectroscopy in the spectral range from 1.7 eV to 5.5 eV with an applied magnetic field of 1.7 T. Crystal field, inter-valence and inter-sublattice charge transfer transitions, and transitions from O$_{2p}$ to metal cation 3d or 4s bands are identified in both the principal diagonal elements and the magneto-optically active off-diagonal elements of the dielectric tensor. Depending on the degree of cation disorder, resulting in local symmetry distortion, the magneto-optical response is found to be strongest for high crystal quality inverse spinels and for disordered normal spinel structure, contrary to the first principle studies of CoFe$_2$O$_4$ and ZnFe$_2$O$_4$. The results presented provide a basis for deeper understanding of light-matter interaction in this material system that is of vital importance for device-related phenomena and engineering.
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We apply the self-interaction corrected local spin density %(SIC-LSD) approximation to study the electronic structure and magnetic properties of the spinel ferrites MnFe$_{2}$O$_{4}$, Fe$_{3}$O$_{4}$, CoFe$_{2}$O$_{4}$, and NiFe$_{2}$O$_{4}$. We concentrate on establishing the nominal valence of the transition metal elements and the ground state structure, based on the study of various valence scenarios for both the inverse and normal spinel structures for all the systems. For both structures we find all the studied compounds to be insulating, but with smaller gaps in the normal spinel scenario. On the contrary, the calculated spin magnetic moments and the exchange splitting of the conduction bands are seen to increase dramatically when moving from the inverse spinel structure to the normal spinel kind. We find substantial orbital moments for NiFe$_{2}$O$_{4}$ and CoFe$_{2}$O$_{4}$.
Magneto-optical spectroscopy based on the transverse magneto-optical Kerr effect (TMOKE) is a sensitive method for investigation of magnetically-ordered media. However, in magnetic materials the optical transitions are usually characterized by spectrally broad resonances with widths considerably exceeding the Zeeman splitting in the magnetic field. Here we investigate experimentally and theoretically the TMOKE in the vicinity of relatively narrow optical resonances provided by confined quantum systems. For experimental demonstration we use the exciton resonance in a (Cd,Mn)Te diluted magnetic semiconductor quantum well, where the strong exchange interaction with magnetic ions enables the giant Zeeman splitting of exciton spin states $Delta$ in magnetic fields of a few Tesla. In the weak coupling regime, when the splitting $Delta$ is smaller than the spectral broadening of the optical transitions $Gamma$, the TMOKE magnitude grows linearly with the increase of the Zeeman splitting and its spectrum has an S-shape, which remains virtually unchanged in this range. In the strong coupling regime ($Delta>Gamma$) the TMOKE magnitude saturates, while its spectrum is strongly modified resulting in the appearance of two separate peaks. The TMOKE is sensitive not only to the sample surface but can be used to probe the confined electronic states in depth if the upper layer is sufficiently transparent. Our results demonstrate that TMOKE of spectrally narrow resonances serves as a versatile tool for probing the charge and spin structure of electronic states in various confined quantum systems and can be used for spin tomography in combination with the conventional polar Kerr effect.
Optical and magneto-optical properties of ZnMnO films grown at low temperature by Atomic Layer Deposition are discussed. A strong polarization of excitonic photoluminescence is reported, surprisingly observed without splitting or spectral shift of excitonic transitions. Present results suggest possibility of Mn recharging in ZnO lattice. Strong absorption, with onset at about 2.1 eV, is related to Mn 2+ to 3+ photo-ionization. We propose that the observed strong circular polarization of excitonic emission is of a similar character as the one observed by us for ZnSe:Cr.
We here report a detailed high-pressure infrared transmission study of BiTeCl and BiTeBr. We follow the evolution of two band transitions: the optical excitation $beta$ between two Rashba-split conduction bands, and the absorption $gamma$ across the band gap. In the low pressure range, $p< 4$~GPa, for both compounds $beta$ is approximately constant with pressure and $gamma$ decreases, in agreement with band structure calculations. In BiTeCl, a clear pressure-induced phase transition at 6~GPa leads to a different ground state. For BiTeBr, the pressure evolution is more subtle, and we discuss the possibility of closing and reopening of the band gap. Our data is consistent with a Weyl phase in BiTeBr at 5$-$6~GPa, followed by the onset of a structural phase transition at 7~GPa.
The discovery of atomically thin two-dimensional (2D) magnetic semiconductors has triggered enormous research interest recently. In this work, we use first-principles many-body perturbation theory to study a prototypical 2D ferromagnetic semiconductor, monolayer chromium tribromide (CrBr$_3$). With broken time-reversal symmetry, spin-orbit coupling, and excitonic effects included through the full-spinor $GW$ and $GW$ plus Bethe-Salpeter equation ($GW$-BSE) methods, we compute the frequency-dependent dielectric function tensor that governs the optical and magneto-optical properties. In addition, we provide a detailed theoretical formalism for simulating magnetic circular dichroism, magneto-optical Kerr effect, and Faraday effect, demonstrating the approach with monolayer CrBr$_3$. Due to reduced dielectric screening in 2D and localized nature of the Cr d orbitals, we find strong self-energy effects on the quasiparticle band structure of monolayer CrBr$_3$ that give a 3.8 eV indirect band gap. Also, excitonic effects dominate the low-energy optical and magneto-optical responses in monolayer CrBr$_3$ where a large exciton binding energy of 2.3 eV is found for the lowest bright exciton state with excitation energy at 1.5 eV. We further find that the magneto-optical signals demonstrate strong dependence on the excitation frequency and substrate refractive index. Our theoretical framework for modelling optical and magneto-optical effects could serve as a powerful theoretical tool for future study of optoelectronic and spintronics devices consisting of van der Waals 2D magnets.
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