Optical Conductivity Spectra Research Articles

DFT analysis of elastic and optoelectronic properties of Cs2NaXCl6 (X=In, La, Sc, Y) double perovskite compounds

This study employs first-principles Density Functional Theory (DFT) to investigate the structural, electronic, and optical properties of double perovskites Cs2NaXCl6 (X = In, La, Sc, and Y) compounds. By applying various functionals (GGA-PBE, GGA-PBEsol, HSE06, and mBJ), we ensure an accurate and thorough description of their electronic structures and other physical properties. Our analysis reveals excellent mechanical, thermodynamic, and dynamical stability of Cs2NaXCl6 compounds. Band gap calculations employing mBJ and HSE06 functionals reveal wide direct band gaps ranging from 4.1 to 6.4 eV, with notable contributions from Cl-p states near the valence band maximum. Furthermore, electron density analysis highlights a mixed covalent-ionic bonding nature, predominantly ionic. Additionally, the optical conductivity and absorption spectra peaks extend beyond the visible region, indicating potential applications in ultraviolet (UV) technologies. Finally, thermal conductivity analyses exhibit a significant reduction with increasing temperature, suggesting promising applications in high-temperature thermal insulation.

Impact of Substitutional Doping of Eu3+ on Optoelectronic Properties of BaMgSiO4 Phosphor Material: A Tunable Blue‐White Color‐Emitting Phosphor

The structure and the optical properties of the tridymite green color phosphor BaMgSiO4 :Eu are systematically examined. Due to the differing ion radii of Eu3+, Mg2+, Si4+, and the three different Ba 2+ sites in the crystal lattice, dopants can only replace the Ba2+ sites because the other sites are insufficiently large to hold the massive Eu3+. BaMgSiO4 is a promising candidate for inorganic photochromatic materials with excellent optical properties. It has attracted much attention in the world due to its applications in high‐density optical memory and light‐emitting diodes. Herein, the generalized gradient approximation and generalized gradient approximation plus Hubbard potential (GGA + U) are used to investigate the electronic structure and the entire optical properties of the parent and Eu‐doped BaMgSiO4, like dielectric function, refractive and extinction coefficients, the optical conductivity, reflectivity, and absorption spectra. It is found that the substitution of Eu ions reduces the energy bandgap of BaMgSiO4 and introduces the sub‐bands in between the valence and conduction bands. Findings show that the bandgap and optical characteristics of the BaMgSiO4 compound are described properly by the GGA + U method.

Electronic, optical, and thermoelectric characteristics of (Ae)xFBiS2 (Ae=Sr, Ba, and x=1.7) layered materials useful in optical modulator devices

The recent discovery of superconductivity behavior in the mother BiS2-layered compounds has captivated the attention of several physicists. The crystal structure of superconductors with alternate layers of BiS2 is homologous to that of cuprates and Fe-based superconductors. The full-potential linearized augmented plane-wave (FP-LAPW) technique was utilized to investigate the electronic structures and density of states in the vicinity of the Fermi energy of SrFBiS2 and BaFBiS2 compounds under the electron carriers doping. The introduction of electron doping (carries doping) reveals that the host compounds SrFBiS2 and BaFBiS2 exhibit features indicative of superconductivity. This carrier doping of SrFBiS2 and BaFBiS2 compounds (electron-doped) has a significant impact on the lowest conduction states near the Fermi level for the emergence of the superconducting aspect. The electron doping modifies and induces changes in the electronic structures with superconducting behavior in (Ae)1.7FBiS2(Ae=Sr,Ba) compounds. A Fermi surface nesting occurred under the modification of electrons (carriers) doping in the host compounds SrFBiS2 and BaFBiS2. Furthermore, the optical characteristics of the carrier-doped SrFBiS2 and BaFBiS2 compounds are simulated. Due to the anisotropic behavior, the optical properties of these materials based on BiS2 demonstrate a pronounced polarization dependency. The starting point at zero photon energy in the infrared region is elucidated by considering the Drude features in the optical conductivity spectra of SrFBiS2 and BaFBiS2 compounds, when the electron carriers doping is applied. It was clearly noticed that the spin-orbit coupling (SOC) influences the electronic band structures, density of states, Femi surface, and optical features because of the heavy Bismuth atom, which may disclose fascinating aspects. Further, we conducted simulations to assess the thermoelectric properties of these mother compounds. The two BiS2-layered compounds could be suitable for practical thermoelectric purposes and are highlighted through assessment of electrical conductivity, thermal conductivity, Seebeck coefficient, and power factor. As a result, we propose that the mechanisms of superconducting behavior in BiS2 family may pave new avenues for investigating the field of unconventional superconductivity. It may also provide new insights into the origin of high-Tc superconductivity nature.

Electron Localization Induced by Disordered Anions in an Organic Conductor.

We report on a new organic conductor κ″-(ET)2Cu[N(CN)2]Br (κ″-Br), which is the first polymorph of an organic superconductor κ-(ET)2Cu[N(CN)2]Br (κ-Br), where ET denotes bis(ethylenedithio)tetrathiafulvalene. κ″-Br has a similar κ-type arrangement of ET molecules to κ-Br, but, in contrast to the orthorhombic κ-Br, which has ordered polyanion chains, presents a monoclinic crystal structure with disordered polymeric anion chains. To elucidate the electronic state of κ″-Br, we performed band calculations as well as transport, magnetic, and optical measurements. The calculated band dispersion, magnitude of electron correlation, and room-temperature optical conductivity spectra of κ″-Br were comparable to those of κ-Br. Despite these similarities, the κ″-Br salt exhibited a semiconducting behavior. The electron spin resonance and Raman spectroscopies indicated that there is neither magnetic nor charge order in κ″-Br, suggesting the occurrence of Anderson localization due to disordered anion layers.

Optical, photo-physical and photo-stability characterizations of malachite green as a laser dye, combined with TD-DFT simulations

The optical properties of Malachite green (Mg) dye were examined experimentally, including absorption, optical energy gab, refractive index, dielectric constant, optical conductivity and emission spectra in various solvents. Additionally, several significant photophysical parameters were evaluated, including the extinction coefficient (ε), the energy yield of fluorescence (Ef), the length of attenuation Λ (λ), oscillator strength (f), quantum yield (Øf), fluorescence lifetime ({uptau }_{{text{f}}}), decay rate radiative constant (kr), and the dipole moment (μ) in addition to absorption and emission cross-sections (σa) and (σe) respectively. Time Dependent Density function theory (TD-DFT) computations were used to generate the theoretical absorption spectra of the (Mg) compound. The energy gap (Eg), electron density, and electrostatic potential were also simulated.

X-ray absorption near-edge, terahertz and Raman spectroscopies evidence growth-orientation dependent cation order, phase transitions and spin–phonon coupling in half-metallic Ca2FeMoO6 thin films

The disorder due to anti-site cation distribution is intrinsic to the double perovskites wherein the crystal orientations of the substrate template are predicted to offer different degrees of cation order in thin film form. To demonstrate this effect, epitaxial thin films of half-metallic double perovskite Ca2FeMoO6 (CFMO) were prepared on (100) and (111) oriented LaAlO3 substrates in vacuum and nitrogen atmospheres. The findings using X-ray absorption near-edge structure, Terahertz (THz) and Raman spectroscopies, in combination with magnetization show that (111) epitaxial template effectively restricts the Fe–Mo anti-site cation disorder. A resultantly enhanced cation order in (111) films induces dramatic transformations in its properties as follows: (i) significantly enhanced ferromagnetic exchange interactions and saturation magnetization, (ii) a significant increase in the Curie temperatures, (iii) a metallic behavior down to much lower temperature (∼75 K) compared to that down to 200 K for (100) film, (iv) an enhanced spin–phonon coupling. The complex THz optical conductivity spectra evaluated in the framework of Drude and Drude–Smith phenomenological models and the temperature-dependent Raman data fitted to the Balkanski model corroborate well to indicate an enhanced cation order in (111) films. While this study establishes a dominant role of crystallographic orientation in the much-desired control of cation order in double perovskites, a demonstration of the same in room temperature half-metallic CFMO system could reinforce its technological utility both as active and passive components in emergent spintronic functionalities.

Unveiling the electronic structure and optical properties of two-dimensional TMDCs: first-principles study

Transition metal dichalcogenide (TMDC) materials are considered extremely efficient materials with significant applications in photovoltaics and optoelectronics. Here, the electronic structure and optoelectronic features of new transition metal-containing dichalcogenides are studied using state-of-the-art density functional theoretical calculations. For the analysis of the electronic band structures, we employed a modified Becke-Johnson potential. According to the band structure analysis, Platinum-based dichalcogenides possess an indirect band profile, having the valence band maximum and the conduction band minimum situated at discrete symmetry regions. At the same time, the zirconium-based materials have a direct type band structure at the same Γ-point. We calculated cohesive energies and formation energies to assess the stability of these materials. The substantial optical parameters such as the two parts of the dielectric constant, absorption coefficients, energy loss functions, reflectivity spectra, refractive index, real optical conductivity spectra, spectra, and the extinction coefficients, are calculated. These findings provide insight into potential applications in optoelectronic devices. The calculated band gaps and refractive index revealed an inverse relationship. This research aims to make a significant contribution to the advancement of various and possibly gainful semiconducting technologies, as well as their practical applications.

The effect of non-metals (O, F) dopant on the electronic structure, Dirac cone, and optical characteristics of graphene sheets applicable for gas sensing

In order to gain a systematic comprehension of the impacts of low-level defects in graphene, ab-initio calculations were performed on monolayer graphene sheets to examine how oxygen and fluorine substitutional impurities affect their energetic stability, electronic and optical characteristics. The optimal configurations, structural stability, electronic band structures, spatial charge density, and optical spectra of graphene single-layer materials doped with oxygen and fluorine atoms are investigated. The fluorine-doped graphene, therefore, showed a lower formation energy than its oxygen-doped counterpart. Additionally, F-doped graphene shows a higher charge density around the fluorine atom than O-doped graphene. Based on band structure analysis, the lower conduction bands of graphene sheets shift below the Fermi state (EF) when two O or F impurities are substituted into it. With two O/F impurity atoms doped into graphene, the conduction states are farther displaced below the EF, resulting in n-type behavior. Consequently, altering graphene structure via an O/F-substituting scheme results from the disruption of the Dirac cone near EF, which has become flat along the high symmetry point (K-point) in the Brillouin zone. Furthermore, the substitution of graphene sheets via O or F impurities exhibit markedly modified optical spectra and refractive indices at low photon energies. As a result, with one or two O/F impurity elements inserted into graphene sheets, the reflectivity and optical conductivity spectra differ at the lowest electromagnetic radiation ranges. Additionally, the electron energy loss functions as well as X-ray absorption spectra of clean and doped graphene monolayers revealed spectral variations at a moderate energy span. These investigations surmise that novel chemical modifications to graphene sheets doped with light non-metallic elements (O/F) may offer the opportunity to tailor their optical characteristics in the infrared spectrum, which may be beneficial in sensor and electrocatalyst uses.

Electronic structure and optical properties of superconducting compounds ScGa3 and LuGa3

The optical properties of bulk AuCu3-type ordered superconducting binary compounds ScGa3 and LuGa3 have been experimentally investigated for the first time in the wide spectral range and explained in terms of the band structure. First-principles calculations of electronic densities of states and optical conductivities are performed within the framework of LSDA+U method using the LMTO-ASA software package. The measured dielectric functions spectra for both materials exhibit a strong absorption region above ∼ 1[Formula: see text]eV, which are in a reasonable agreement with the calculated metal-like energy structures of compounds. Features of quantum light absorption are discussed on the basis of a comparative analysis of experimental and theoretical spectra of interband optical conductivity. Plasma and relaxation frequencies of conduction electrons are determined.

Tightly bound and room-temperature-stable excitons in van der Waals degenerate-semiconductor Bi4O4SeCl2 with high charge-carrier density

Excitons, which represent a type of quasi-particles consisting of electron-hole pairs bound by the mutual Coulomb interaction, are often observed in lowly-doped semiconductors or insulators. However, realizing excitons in semiconductors or insulators with high charge-carrier densities is challenging. Here, we perform infrared spectroscopy, electrical transport, ab initio calculations, and angle-resolved-photoemission spectroscopy study of the van der Waals degenerate-semiconductor Bi4O4SeCl2. A peak-like feature (α peak) is present around ~125 meV in the optical conductivity spectra at low temperature T = 8 K and room temperature. After being excluded from the optical excitations of free carriers, interband transitions, localized states and polarons, the α peak is assigned as an exciton absorption. Assuming the existence of weakly-bound Wannier-type excitons in this material violates the Lyddane-Sachs-Teller relation. Moreover, the exciton binding energy of ~375 meV, which is about an order of magnitude larger than those of conventional semiconductors, and the charge-carrier concentration of ~1.25 × 1019 cm−3, which is higher than the Mott density, further indicate that the excitons in this highly-doped system should be tightly bound. Our results pave the way for developing optoelectronic devices based on tightly bound and room-temperature-stable excitons in highly-doped van der Waals degenerate semiconductors.

Multiorbital Nature of Doped Sr_{2}IrO_{4}.

The low-energy j_{eff}=1/2 band of Sr_{2}IrO_{4} bears stark resemblances with the x^{2}-y^{2} band of La_{2}CuO_{4}, and yet no superconductivity has been found so far by doping Sr_{2}IrO_{4}. Behind such a behavior could be inherent failures of the j_{eff}=1/2 picture, in particular when electrons or holes are introduced in the IrO_{2} planes. In view of this, here we reanalyze the j_{eff}=1/2 scenario. By using the local-density approximation plus dynamical mean-field theory approach, we show that the form of the effective j_{eff}=1/2 state is surprisingly stable upon doping. This supports the j_{eff}=1/2 picture. We show that, nevertheless, Sr_{2}IrO_{4} remains in essence a multiorbital system: The hybridization with the j_{eff}=3/2 orbitals sizably reduces the Mott gap by enhancing orbital degeneracy, and part of the holes go into the j_{eff}=3/2 channels. These effects cannot be reproduced by a simple effective screened Coulomb repulsion. In the optical conductivity spectra, multiorbital processes involving the j_{eff}=3/2 states contribute both to the Drude peak and to relatively low-energy features.

Effect of doping SrTiO3 with Nb studied with wide-range spectroscopic ellipsometry

The low-temperature optical properties of a SrTiO3 crystal doped with 0.7% wt. Nb and a pure SrTiO3 reference crystal were studied using spectroscopic ellipsometry. The optical constants and dielectric functions were obtained in the spectral range of 0.8–8.8 eV at temperatures from 10 to 300 K, and the optical conductivity was obtained in the spectral range of 0.03–1 eV at 300 K. Analysis of the optical conductivity spectra in the infrared spectral range confirmed the presence of free electrons and additional absorption hump between 0.1 and 0.4 eV (806 and 3226 cm−1) in doped SrTiO3 and optical phonons in both doped and undoped SrTiO3. The performed analysis of optical absorption spectra in the range 0.8–8.8 eV revealed frustration of the indirect bandgap and an increase in the direct bandgap energy by ∼0.03 eV in Nb-doped SrTiO3, compared to undoped SrTiO3 over the whole temperature range. The energies of the peaks’ maxima of the dielectric function spectra did not significantly differ for doped and pure SrTiO3. For both Nb-doped and pure SrTiO3, temperature dependence of the direct bandgap energy and that of the index of refraction showed inflection between 100 and 150 K, which may be considered evidence of an antiferrodistortive phase transition from a cubic to a tetragonal structure.

Investigating structural, electronic and optical properties of Sc2CF2@Fe MXene: A first principle study

In this work, the structural, electronic and optical properties of novel 2D Sc2CF2 MXene alloyed with Fe are studied by first-principles calculations. The computational method is based on the density functional theory (DFT) and generalized gradient approximation (GGA) considering non-spin–orbit and spin–orbit coupling (SOC). By analyzing the behavior of spin-polarized band structure and density of states (DOS), metallic behavior for all alloy compositions has been predicted. In addition, for all alloy compositions except for c=0.5, the ferromagnetic property has been discovered. Moreover, the optical properties like real and imaginary parts of dielectric and energy loss functions, optical conductivity, absorption coefficient, and reflectivity spectrum have been studied. The results of the absorption coefficient and reflectivity spectrum as a function of photon energy predict that the compounds can be sound absorbers at both visible-light and ultraviolet wavelength regions.

Electro-optical properties of strained monolayer boron phosphide

In this paper, we use tight-binding approximation and linear response theory to study the electronic and optical properties of strained monolayer boron-phosphide (h-BP). Compared with the previous DFT study and adding on-site energy variation to the Hamiltonian, we propose a theoretical approach to investigate the strain effects on the electronic and optical properties of the h-BP. Applying tensile strain increases the gap while compressive strain reduces it as the maximum and minimum of the gap are 1.45 eV and 1.14 eV respectively and are related to the biaxial strain. Also, we investigate the optical conductivity and electron energy loss spectrum (EELS) of the pristine and strained h-BP. The absorption peak of the Resigma_{xx,yy} appears in energy about 4 eV but applying strain shifts the peak’s energy. Optical properties of pristine h-BP are isotopic and biaxial strain preserves this isotropy, but uniaxial strain exerts anisotropic behavior in the system.

Light-induced coherent interlayer transport in stripe-ordered La1.6−xNd0.4SrxCuO4

We have investigated the photoexcited transient responses of stripe-ordered phase in a cuprate superconductor, ${\rm La}_{1.6-x}{\rm Nd}_{0.4}{\rm Sr}_{x}{\rm CuO}_{4}~(x = 0.12)$ using optical-pump terahertz (THz)-probe spectroscopy. Upon the near-infrared photoexcitation with the electric field polarized along the $c$-axis, a clear plasma edge appears in the THz reflection spectrum along the $c$-axis with its position nearly coinciding with the Josephson plasma resonance of similarly doped ${\rm La}_{2-x}{\rm Sr}_{x}{\rm CuO}_{4}~(x = 0.125)$ in the low-temperature superconducting phase. The appearance of light-induced plasma edge sustains up to the onset temperature of the charge-stripe order, indicating the inherent interplay between the light-induced phase and the charge-stripe order. The optical conductivity spectrum of the light-induced state is mostly reproduced by the Drude model with a scattering rate as small as a few meV, and its imaginary part does not exhibit $1/{\omega}$-divergence behavior in any temporal region after the photoexcitation. We discuss the possible origin of the observed coherent interlayer transport behavior as manifested by the narrow Drude response in the THz reflectivity along the $c$-axis.

Abrupt change reflected by the van Hove singularity in the optical spectra of CaMn2P2

The trigonal CaAl2Si2-type structure CaMn2P2 has been reported undergoing an exotic first order phase transition at the critical temperature T K. In this paper, we present the optical spectra for the ab-plane of CaMn2P2 single crystal from 300 K to 10 K for the first time. In the real part of the optical conductivity spectra σ 1(ω), a direct gap could be determined at all temperatures without any Drude term visible, i.e., the sample goes through the first order phase transition from one insulator state to the other insulator state. At higher energy, an asymmetric sharp interband transition peak appears in all σ 1(ω) spectra, which indicates a divergence of the joint density of states. This sharp peak could be well described by the two dimensional van Hove singularity function. In particular, this peak is very sensitive to the first order phase transition, especially the peak position E whose the most prominent blue shift occurs only when the first order transition happens. Our data and analysis reveal that the first order phase transition leads to a weak partial re-normalization of the band structure. Our study will be useful in further investigations about the mechanism of the first order phase transition in the insulator.

The Electronic Structure and Optical Spectroscopy of ErNi2Mnx Compounds

The electronic structure and optical properties of nonstoichiometric ErNi2Mnx compounds (with х = 0, 0.5, 1) have been studied. Spin-polarization calculations of the total and partial densities of electron states have been performed in terms of DFT + U method with a correction for strong electronic correlations in the 4f shell of Er in the approximation of ErNi2 – xMnx solid-solution. The peculiarities of transformations of the densities of electron states Have been determined depending on the manganese content. The optical properties of these compounds have been studied over a wide wave length range. The calculated interband optical conductivity spectra have been compared with the dependences obtained experimentally. The origin of the quantum absorption of light is discussed. The plasma and relaxation frequencies of current carriers have been determined.

Investigation of semi-metallic properties of GdSb and TbSb compounds

The results of the electronic structure calculations and the optical properties study of antiferromagnetic compounds GdSb and TbSb are presented. In the spectral range 0.078 – 5.6 eV, the energy dependences of the real and imaginary parts of the complex dielectric permittivity are investigated by ellipsometric method. The anomalous behavior of spectral characteristics in the infrared region is associated with the semi-metallic properties of these materials. Based on the performed calculations of the band structure, the energy dependences of the interband optical conductivity spectra are discussed.

Lead-tungsten oxide interfaces designed as gigahertz/terahertz filters

Herein amorphous tungsten oxide thin films of thicknesses of 300 nm are coated onto semitransparent Pb films (100 nm) by the thermal evaporation technique under a vacuum pressure of 10−5 mbar. Optical investigations in these films have shown that Pb nanosheets enhances the light absorbability in the visible and infrared ranges of light without significant change in the energy band gap value. In addition deep analyses of the optical conductivity and terahertz cutoff frequency spectra of the Pb/WO3 optical filters revealed that the cutoff frequency value in the visible range of light is invariant with light signal energy indicating the possibly of filtering none-monochromatic light signals. On the other hand imposing an ac signal between the terminals of Pb/WO3/Au devices has proofed the ability of the device to perform as low pass and as band stop filters workable in the microwave frequency domain. The microwave cutoff frequency for this device reached ∼9 GHz nominating it for use in 5 G mobile technology. The current study showed that coating of tungsten oxide onto semitransparent Pb substrate and coverage small area of the top contact with Au can allow functioning the device as gigahertz/terahertz band filters suitable for communication technology.

Electron-phonon correlations inducing excitonic excitations in semimetal and semiconducting materials

The influence of phonons on the low-energy excitonic excitations at zero temperature in the extended Falicov-Kimball model has been investigated. In the framework of the unrestricted Hartree-Fock approximation, a set of self-consistent equations for the excitonic condensate order parameter and a lattice distortion is derived when both electron-phonon coupling and electron-hole Coulomb interaction are treated on an equal footing. The low-energy excitation properties of the excitonic condensate are addressed in signatures of the optical conductivity and the dynamical excitonic susceptibility function. The real part of the optical conductivity is evaluated by the Kubo linear response theory and the imaginary part of the dynamical excitonic susceptibility is found by adapting the random phase approximation. In the semimetal state, one always finds a sharp peak in the optical conductivity spectrum indicating the stability of the excitonic condensation in the BCS type if the correlation between electrons and phonons becomes significant. In contrast, the peak is smeared out on the semiconducting side indicating the stability of the BEC-type excitonic condensate. In this semiconducting side, the sharp peak signature appears and the system turns to the BCS-type excitonic condensation state by increasing the electron-phonon correlations. In either the semimetal or the semiconducting normal state, increasing the electron-phonon correlations always reinforces a low-energy sharp peak in the dynamical excitonic susceptibility spectrum, indicating the existence of the tightly bound excitonic excitations before the condensation state. Specifically, on the semiconducting side, the ``halo'' phase with the preformed excitons exiting outside of the BEC-excitonic condensation state has been specified. The halo phase becomes more recognizable by raising the electron-phonon correlations.