Light scattering by magnetic excitons in (FeMn)F2

The transitions between the low lying crystal field split states A_1g and B_1g of the Fe²⁺ ions in pure FeF₂ and in the mixed antiferromagnet Fe_1-xMn_xF₂ have been investigated with Raman light scattering. From the Raman polarization rules the lines have been identified as arising from the magnetic excitons associated with the transitions. The energy and the line-width of the strongest line are studied as a function of the concentration x. From the energy measurement we estimate that the single ion anisotropy parameter D of the Fe²⁺ ions varies from 6.46 cm^-1 in pure FeF₂ to 8.03 cm^-1 in MnF₂: Fe.     

Exciton-magnon interactions in NicMg1−c O single crystals

The effect of chemical composition and temperature on exciton-magnon interactions in Ni_cMg_1?c O single crystals was studied using optical absorption spectra in the region of the magnetic-dipole ³ A _2g (G)→³ T _2g (F) and electric-dipole ³ A _2g (F)→¹ E _g (D) transitions. The two zero-phonon lines at ～7800 and ～7840 cm^?1 on the low-energy side of the magnetic-dipole transition band were assigned to a pure exciton transition and an exciton-one-magnon transition at the center of the Brillouin zone. The intensity of the exciton-one-magnon peak decreases rapidly with increasing magnesium ion concentration and/or temperature, to vanish altogether at T=6 K for c<0.95 and at T=130 K for c≥0.99. Thus, the contribution of long-wavelength magnons in optical absorption spectra of Ni_cMg_1?c O becomes negligible at temperatures substantially lower than the Néel point T _N (the antiferromagnetic ordering temperature). This observation can be explained as being due to a substantial decrease in the characteristic spin-spin interaction length with increasing concentration of the diamagnetic magnesium impurity ions (static disorder) and/or with increasing amplitude of thermal atomic vibrations (dynamic disorder). At the same time, the peak at ～14500 cm^?1, which lies in the electric-dipole transition region and corresponds to excitation of an exciton and two magnons at the Brillouin zone edge, remains visible up to the Néel temperature. This is accounted for by the short-wavelength magnons being sensitive to short-range magnetic order, which persists up to T _N .     

Optical selection rules and magnon assignments for the low temperature magnetic spin structures of CsCoCl3 and CsNiCl3

The optical selection rules for excitons, magnons and exciton-magnon coupled modes are derived for the various magnetic phases of CsCoCl₃ and CsNiCl₃. For CsCoCl₃, these selection rules are used in conjunction with the energy levels calculated in the previous paper (I) to account for the sharp side bands observed in the optical spectrum. For CsNiCl₃, the discussion focuses on the utility of the selections rules to be used as a tool to distinguish phases, particularly in the region of the controversial intermediate phase.     

Two-magnon Raman scattering in two-dimensional antiferromagnets at finite temperatures

The temperature dependence of two-magnon Raman scattering in the quadratic-layer antiferromagnets K₂NiF₄ and K₂MnF₄ is found to agree with the higher-order Green function theory of Balucani and Tognetti. New experimental data on K₂MnF₄ are also presented.     

Biexciton decay and multimagnon sideband in emission spectra of CsMnF3

Emission spectra of intrinsic and impurity-trapped excitons and their side- bands have been measured in CsMnF₃ by a polarized time-resolved spectroscopy. From a biexcitonic decay of an emission an exciton- exciton interaction was found to be very small in contrast with those of MnF₂ and KMnF₃. Multimagnon sidebands have been assigned with the aid of calculation of magnon density of states.     

Influence of magnetic dipolar interaction on one- and two-magnon scattering of light in ferromagnets

It is shown that the presence of magnetic dipolar interaction in a ferromagnetic medium changes the polarization selection rules of light scattered by magnons. In addition it provides a new mechanism for two-magnon scattering.     

Optical properties of antiferromagnetic/ion-crystal superlattices

Transmission, refraction and absorption properties of an antiferromagnetic/ion-crystal superlattice are investigated. The transmission spectra based on FeF₂/TlBr superlattices reveal that there exist two intriguing guided modes in a wide stop band. Additionally, FeF₂/TlBr superlattices possess either the negative refraction or the quasi left-handedness, or even simultaneously hold them at certain frequencies of two guided modes, which require both negative magnetic permeability of antiferromagnetic layers and negative permittivity of ion-crystal layers. Frequency regimes of the guided modes will be dependent on the magnitude of the external magnetic field. Therefore, handedness and refraction properties of the system can be manipulated by modifying the external magnetic field. Absorption spectra exhibit that absorption corresponding to guided modes is noticeable.     

Creation of spin-oriented 2P excitons in CdS by two-photon magneto-absorption

We report experimental results on the creation of 2P excitons in CdS by the two-photon magneto-absorption process involving a simultaneous absorption of visible and infrared photons. For a magnetic field parallel to the c axis and particularly for a visible beam propagating along the c axis, spin-oriented 2P (A) excitons are created from the A (Γ₉) valence band. We explain these results on the basis of the main contribution of the 1SΓ₅ (A) exciton intermediate state.     

Exciton and phonon spectra of acoustooptic Tl3AsS3 crystals

The λ-modulated exciton reflection spectra of Tl₃AsS₃ crystals are investigated at 8 and 77 K, in which the ground (n=1) and excited (n=2, 3) exciton states are revealed. Taking into account the spatial dispersion, the shapes of λ-modulated reflection spectra of the n=1 line are calculated and the basic parameters of excitons and bands are determined (the translational and reduced masses of excitons and the effective masses of electrons and light and heavy holes). The one-phonon reflection spectra are studied in the region from 50 to 500 cm^?1 in polarizations E ∥ c and E ⊥ c. The shapes of one-phonon reflection spectra are calculated and the parameters of vibrational modes E and A ₂ are determined.     

Magnetic excitations in the two dimensional planar antiferromagnets K2FeF4 and Rb2FeF4

The magnetic excitation spectrum of K₂FeF₄ and Rb₂FeF₄, two K₂NiF₄-structure planar antiferromagnets with rather large anisotropy and spins perpendicular to the c-axis, has been measured by Raman and FIR-spectroscopy. One of the two predicted one-magnon transitions and the two-magnon mode have been observed in K₂FeF₄ (Rb₂FeF₄) at 48.5 cm^-1 (37.6 cm^-1) and 182.0 cm^-1 (160.5 cm^-1) respectively. The magnetic field and temperature dependence of the spectra are reported too. The data are discussed on the basis of an easy plane spin model Hamiltonian. In K₂FeF₄: Mn²⁺ a low lying magnetic impurity mode is observed at 40.5 cm^-1.     

Theory of two-magnon dissipation in disordered ferromagnets I. Relation to sample statistics

The theory of two-magnon dissipation in disordered ferromagnetic materials is developed. Fluctuations of one-ion anisotropy energy due to the disorder are assumed to be the source of the linewidth broadening (relaxation of magnons by two-magnon scattering). Ordinary two-magnon theory is reconsidered on the basis of the sample statistics. The main idea of it is to describe the macroscopic properties of materials by means of quantities, whose relative fluctuations over the ensemble of configurations are negligibly small for sufficiently large sample. The energies of magnons — modes with well defined wave vectork — and their lifetimes are shown to be such variables. Further, possible models for a two-component ferromagnet are considered in the approximation of high external field. The energies of magnons in mixed crystal are obtained as linear combinations of those in parent crystals. Finally, the dependence of magnon lifetimes on the ordering is separated from the dependence on the magnitude of anisotropy variations.     

Magnetopolaritons in ZnTe

From an invariant expansion, we construct the exciton Hamiltonian for the Γ₆×Γ₈ excitons in theT _d -type material ZnTe represented by an 8×8 matrix including the influences of a finite wave vector and an external magnetic field. We diagonalize the Hamiltonian matrix to obtain the exciton states. Then the excitons are coupled to the electromagnetic radiation field thus giving the polariton states. The theoretical dispersion curves are fitted to the results of two-photon Raman scattering and reflection experiments in magnetic fields up to 22 T. From this fit we deduce precise values for the eigenergies, exciton masses,g-factors, and diamagnetic shifts.     

Fourth-order spin Hamiltonian terms for Fe2+ in rutile structure antiferromagnet FeF2

The paper deals with the spectroscopic and magnetic properties of Fe²⁺ ions in FeF₂. The microscopic spin Hamiltonian theory for Fe²⁺ in crystalline environments with second-kind orthorhombic symmetry is considered. Explicit formulas for the parameters B₀⁽²⁾(D),B₂⁽²⁾(E), g_x, g_y, g_z and, for the first time in the literature, the fourth-order parameters B₀⁽⁴⁾, B₂⁽⁴⁾ and B₄⁽⁴⁾, are derived. Using semi-empirical data for the ⁵D-term energy levels of Fe²⁺ ion in FeF₂, the pressure dependence of the parameters B_q^(k) in the region from 0 to 133 kbar is discussed. The relative role of the fourth-order parameters with respect to the second-order ones is found to increase strongly with pressure (e.g. in the region studied, D increases only by a factor of 3, whereas B₀⁽⁴⁾ increases by a factor of nearly 20). The magnetocrystalline anisotropy of FeF₂; is considered in the strong anisotropy model taking into account the fourth-order spin Hamiltonian terms. The uniaxial anisotropy constants K₁ and K₂ are derived theoretically and their pressure dependence is discussed quantitatively. The theory and numerical results of this paper are useful with regard to Fe²⁺ in other isomorphic fluorides, namely: MgF₂, ZnF₂, VF₂ and MnF₂. It is found that the fourth-order spin Hamiltonian parameters are accessible to experimental detection from spectroscopic studies on Fe²⁺ in non-magnetic fluorides and magnetic studies on Fe²⁺ : MnF₂ and FeF₂, preferably under high pressure.     

Core level exchange splittings in transition metal compounds

The exchange splittings of the 3s core levels are analyzed for a number of manganese, iron and cobalt compounds. It is found that in MnF₂, MnCl₂, FeF₃, FeF₂, FeCl₂ and CoF₂ the lowest energy state after photoemission has the samed-electron count as the ground state. In CoCl₂ the mixing of thed ⁷L and thed ⁸L^–1 is very strong.     

Spectroscopic properties of Fe ions at tetragonal sites—Crystal field effects and microscopic modeling of spin Hamiltonian parameters for Fe (S=2) ions in K2FeF4 and K2ZnF4

Magnetic and spectroscopic properties of the planar antiferromagnet K₂FeF₄ are determined by the Fe²⁺ ions at tetragonal sites. The two-dimensional easy-plane anisotropy exhibited by K₂FeF₄ is due to the zero field splitting (ZFS) terms arising from the orbital singlet ground state of Fe²⁺ ions with the spin S=2. To provide insight into the single-ion magnetic anisotropy of K₂FeF₄, the crystal field theory and the microscopic spin Hamiltonian (MSH) approach based on the tensor method is adopted. Survey of available experimental data on the crystal field energy levels and free-ion parameters for Fe²⁺ ions in K₂FeF₄ and related compounds is carried out to provide input for microscopic modeling of the ZFS parameters and the Zeeman electronic ones. The ZFS parameters are expressed in the extended Stevens notation and include contributions up to the fourth-order using as perturbation the spin-orbit and electronic spin-spin couplings within the tetragonal crystal field states of the ground ⁵D multiplet. Modeling of the ZFS parameters and the Zeeman electronic ones is carried out. Variation of these parameters is studied taking into account reasonable ranges of the microscopic ones, i.e. the spin-orbit and spin-spin coupling constants, and the energy level splittings, suitable for Fe²⁺ ions in K₂FeF₄ and Fe²⁺:K₂ZnF₄. Conversions between the ZFS parameters in the extended Stevens notation and the conventional ones are considered to enable comparison with the data of others. Comparative analysis of the MSH formulas derived earlier and our more complete ones indicates the importance of terms omitted earlier as well as the fourth-order ZFS parameters and the spin-spin coupling related contributions. The results may be useful also for Fe²⁺ ions at axial symmetry sites in related systems, i.e. Fe:K₂MnF₄, Rb₂Co_1−xFe_xF₄, Fe²⁺:Rb₂CrCl₄, and Fe²⁺:Rb₂ZnCl₄.     

One-magnon luminescence sidebands of the excitonic transition in MnF2

We report the first observation of the π-polarized one-magnon excitonic luminescence sideband in MnF₂. The theory of Loudon is used to fit the experimental spectrum quantitatively. An effective temperature of the crystal is deduced from the simultaneously observed antiStokes sideband emission.     

Room-temperature photoluminescence in MnF2 under high pressure

A novel two-color photoluminescence (PL) is found in MnF₂ at room temperature (RT) under high pressure. In contrast to the low-temperature PL, the observation of room-temperature PL is unusual in transition-metal concentrated materials like MnF₂ since the de-excitation process at RT is fully governed by energy transfer to non-radiative centers. We show that room-temperature MnF₂ emissions originate in the pressure-induced cotunnite phase. Both the nine-fold Mn²⁺ coordination and the Mn–F–Mn exchange pathway inhibit exciton migration among Mn²⁺, favoring two-band PL at RT. The electronic structure and the excited-state dynamics are investigated by time-resolved emission and excitation spectroscopies under pressure. The two PL bands at 2.34 and 1.87 eV above 15 GPa are assigned to Mn²⁺ emissions arising from two distinct Mn²⁺ centers formed in the MnF₂ high-pressure phase. The microscopic origin of the two-color PL is analyzed in terms of exciton dynamics in the MnF₂ cotunnite structure.     

Magneto-optical studies of excitons in AgGaS2

The reflection, absorption and luminescence spectra of the lowest excitons in AgGaS₂ are measured in magnetic fields. The results can be explained by the quasicubic model. The exchange splittings of the Γ₄, Γ₅ and Γ₃ exciton state are evaluated. The Zeeman splittings of the Γ₅ and Γ₅-Γ₃ states yield g-values of + 3.8 and 3.7, respectively. They are determined mainly by the contributions of the hole and conduction electron spins.     

Synthesis, structural and optical properties of a novel bilayered organic-inorganic perovskite C5Pb2I5

Single crystals of [C₅H₁₁NH₃]Pb₂I₅, abbreviated C₅Pb₂I₅, have been prepared. This compound is a new member of the family of the bilayered organic-inorganic lead-iodide based perovskites. Its crystal structure has been determined by X-ray diffraction. The inorganic sub-lattice consists of periodic bilayers of iodoplumbate octahedra. Each PbI₆ octahedra exhibits both edge- and corner-sharing with adjacent octahedra. The vibrational properties of this compound have been studied by Raman scattering spectroscopy. Optical absorption, photoluminescence and diffuse reflectance measurements have been performed. The room-temperature bandgap and free exciton absorption bands are observed at 2.46 and 2.23 eV, respectively. The exciton binding energy is 230 meV which is the largest value ever reported till date for the bilayered PbI based perovskites. Calculations assuming Wannier-type quasi-two-dimensional excitons and taking into account the image potential of the exciton charges showed that nearly 64% of the exciton binding energy is due to the dielectric confinement effect.