Pseudodielectric Function Research Articles

Optical Properties and Growth Characteristics of 8-Quinolinolato Lithium (Liq) Nano-Layers Deposited by Gas Transport Deposition.

Organometallic complexes containing reactive alkali metals, such as lithium (Li), represent a promising material approach for electron injection layers and electron transport layers (EILs and ETLs) to enhance the performance of Organic Light-Emitting Diodes (OLEDs). 8-Quinolinolato Lithium (Liq) has shown remarkable potential as an EIL and ETL when conveyed in very thin films. Nevertheless, the deposition of nano-layers requires precise control over both thickness and morphology. In this work, we investigate the optical properties and morphological characteristics of Liq thin films deposited via Organic Vapor Phase Deposition (OVPD). Specifically, we present our methodology for analyzing the measured pseudodielectric function <ε(ω)> using Spectroscopic Ellipsometry (SE), alongside the nano-topography of evaporated Liq nano-layers using Atomic Force Microscopy (AFM). This information can contribute to the understanding of the functionality of this material, since ultra-thin Liq interlayers can significantly increase the operational stability of OLED architectures.

Dielectric function and interband critical points of compressively strained ferroelectric K0.85Na0.15NbO3 thin film with monoclinic and orthorhombic symmetry

The dielectric function and interband critical points of compressively strained ferroelectric K0.85Na0.15NbO3 thin film grown by metal-organic vapor phase epitaxy (MOVPE) are studied in broad spectral and temperature ranges by spectroscopic ellipsometry (SE). The temperature dependence of the measured pseudodielectric functions is strongly affected by a structural phase transition from the monoclinic Mc-phase to the orthorhombic c-phase at about 428 K. Using a parametric optical constant model, the corresponding dielectric functions as well as the interband optical transitions of the film are determined in the spectral range of 0.73–6.00 eV. Standard critical point (SCP) analysis of the 2nd derivatives of the dielectric functions identified three and four critical points for monoclinic and orthorhombic symmetries, respectively. A systematic redshift of the threshold energies with increasing temperatures was observed.

Electron-enhanced atomic layer deposition of Ru thin films using Ru(DMBD)(CO)3 and effect of forming gas anneal

Ruthenium (Ru) thin films were deposited utilizing electron-enhanced atomic layer deposition (EE-ALD). Sequential exposures of Ru(DMBD)(CO)3 (DMBD = 2,3-dimethylbutadiene) and low-energy electrons at ∼125 eV were used to grow the Ru films at temperatures ≤160 °C. The electrons were obtained from a hollow cathode plasma electron source that provided an electron current of ∼200 mA over a surface area of ∼4 cm2. Low-energy electrons can desorb surface ligands derived from Ru(DMBD)(CO)3, such as CO, through electron-stimulated desorption. The desorbed surface ligands leave chemically reactive sites for subsequent Ru(DMBD)(CO)3 precursor absorption. Ru EE-ALD film growth was monitored utilizing in situ spectroscopic ellipsometry (SE). The electron exposures resulted in rapid Ru film nucleation and growth. Under saturation conditions at 160 °C, the growth rate for Ru EE-ALD was 0.2 Å/cycle. The electron efficiency factor for Ru EE-ALD was ∼21 500 electrons/deposited Ru atom. There was no film growth without electron exposures. Ru growth was observed on various substrates including silicon with native oxide and titanium. Ru growth was also obtained on insulating substrates such as 400 nm thick thermal SiO2 substrates. XPS analysis measured &amp;lt;1 at. % oxygen in the deposited Ru films. XRD, x-ray reflectivity, and SE were used to characterize the Ru films before and after forming gas anneal (FGA). FGA successfully removed carbon impurities from the as-deposited Ru films. The resistivity of the Ru EE-ALD films after FGA was determined to be as low as 17 μΩ cm for a film thickness of 6.7 nm. SE measurements of the imaginary part of the pseudodielectric function, 〈ɛ2〉, were utilized to characterize the as-deposited Ru films and the high purity Ru films after FGA. The low resistivity of the Ru films after FGA was consistent with a prominent Drude absorption in the ⟨ε2⟩ spectrum at ≤1 eV. Various reactive background gases such as H2, NH3, and H2O were utilized during EE-ALD to attempt to remove the carbon from the as-deposited Ru EE-ALD films.

Influence of microstructure on dielectric function and plasmonic properties of silver nanoparticles grown by solid state dewetting: a spectroscopic ellipsometry study

This work reports the microstructure influence on dielectric function and plasmonic properties of silver nanoparticles (Ag NPs). Ag NPs with varying microstructures were grown on corning glass substrate by solid-state dewetting (SSD) of sputtered silver thin films deposited by varying RF power. Dielectric function and plasmonic properties of Ag NPs were investigated from spectroscopic ellipsometry (SE) data using a quite unique model in terms of the combination of different oscillators. Drude–Lorentz model along with two Gauss oscillators was used to account for intraband, interband transitions and different modes of localized surface plasmon resonance (LSPR) of Ag NPs. It was observed that peak of imaginary part of pseudo dielectric function, which is due to LSPR of Ag NPs, shifted towards the lower energy at higher RF power due to increase in thickness of precursor films which subsequently resulted in to increase in particle size. A shift in the LSPR peak in absorbance spectra in UV–Vis-NIR spectroscopy was also observed. No LSPR peak is observed in SE or UV–Vis absorbance spectra for thick films deposited at high RF power due to the presence of continuous silver film even after annealing. This change in microstructure from nanoparticle formation to continuous films is also reflected in the values of void fraction and surface roughness calculated from SE using Bruggeman Effective Medium Approximation (BEMA). Field Emission Electron Microscopy (FESEM), Atomic Force Microscopy (AFM), and X-ray diffraction (XRD) were used to probe the microstructure of Ag NPs. Root mean square (RMS) roughness evaluated from AFM matched well with surface roughness measured from SE.

Pseudo-dielectric functions, band-to-band transitions, and dielectric-related factors in a single-crystal LiTi2O4 thin film

This article is devoted to studying the optical properties of a novel single-crystal LiTi2O4 thin film. A high-quality (011)-oriented LiTi2O4 single-crystal thin film was prepared on a MgAl2O4 (011) substrate by pulsed laser deposition. The weak in-plane optical anisotropy is discovered by Mueller-matrix spectroscopic ellipsometry, which can be attributed to the cooperative Jahn-Teller distortion in the Ti–O octahedrons. The pseudo-dielectric functions were determined in the photon energy of 1.24–5.06 eV using the ellipsometric spectra. The optical conductivity, plasma frequency, effective mass, scattering time and other dielectric-related factors are also discussed. The critical points obtained in the pseudo-dielectric functions are originated from the charge-transfer transitions of the Ti related pairs. The results demonstrate that the enhanced effective mass is responsible for the high optical transparency of LiTi2O4 rather than the large high frequency dielectric constant ε∞.

Temperature dependence of the infrared dielectric function and the direct bandgap of InSb from 80 to 725 K

The temperature dependence of the complex pseudodielectric function of bulk InSb (100) near the direct band gap was measured with Fourier-transform infrared ellipsometry between 30 and 500 meV at temperatures from 80 to 725 K in ultrahigh vacuum. Using the Jellison–Sales method for transparent glasses, the thickness of the native oxide was found to be 25±5 Å, assuming a high-frequency dielectric constant of about 3.8 for the native oxide. After this surface correction, the dielectric function was fitted with a Herzinger–Johs parametric semiconductor model to determine the bandgap and with a Drude term to determine the electron concentration and the mobility. We find that the bandgap decreases from 230 meV at 80 K to 185 meV at 300 K, as expected from thermal expansion and a Bose–Einstein model for electron-phonon scattering renormalization of the bandgap. Between 450 and 550 K, the bandgap remains constant near 150 meV and then increases again at even higher temperatures, presumably due to a Burstein–Moss shift resulting from thermally excited electron-hole pairs. The broadening of the direct bandgap increases steadily with temperature. The electron concentration (calculated from the Drude tail at low energies assuming parabolic bands with a constant electron mass of 0.014m0) increases from 2×1016cm−3 at 300 K to 3×1017cm−3 at 700 K, in reasonable agreement with temperature-dependent Hall measurements. The electron mobility was found to decrease from 105cm2/Vs at 450 K to 2×104cm2/Vs at 700 K, also in good agreement with Hall effect results. We describe a theoretical model that might be used to explain these experimental results.

Spectroscopic ellipsometry and raman spectroscopy of Bi1-xSbxTeI solid solutions with x≤0.1

Spectroscopic ellipsometry supported by reflectivity measurements and Raman spectroscopy are applied at room temperature to n-type Rashba semiconductors BiTeI and Bi1-xSbxTeI with nominal compositions x = 0.05 and 0.1. Complementary four probe Hall measurements are made using standard ac technique and the concentration of free carriers is determined. The Raman spectra, including TO-LO resonances are found to occupy a frequency range below 250 cm−1 in the studied materials. The pseudodielectric function, retrieved at different angles of incidence is analyzed focusing on the free carrier absorption (intraband transitions) and the optical transitions between the Rashba-split branches of the conduction band (intersubband vertical transitions). The former transitions with screened plasma frequency anchored to the zero-crossing point of the real part of the pseudodielectric function are described within a simple Drude model and the important parameters such as electron effective mass, electron mobility and high frequency dielectric constant are obtained. Anchored to the Rashba energy, the intersubband transitions obtained for each material by refining the pseudodielectric function from Drude contribution, appear in the imaginary part as a broad peak in the photon energy range between 0.15 and 0.4 eV. A noticeable red shift of this peak for Bi0.9Sb0.1TeI as compared to BiTeI is proposed to be a manifestation of the reduction of the spin splitting after part of Bi atoms is replaced by lighter Sb atoms.

Spectro-ellipsometric probing of wetting, nucleation, and dot/island formation during photo-excited chemical vapor deposition of Ge on SiO2 substrate

The morphological evolution of Ge layers growing on the SiO2/Si(100) substrate by photo-excited chemical vapor deposition was traced through an analysis of pseudodielectric functions measured by real-time spectroscopic ellipsometry. Simulation and fitting were carried out on multiple samples with various Ge film thicknesses as well as on sequential optical spectra from a sample with an incremental buildup of Ge atoms on one substrate. Single- and two-layer models involving crystalline Ge (c-Ge), amorphous Ge (a-Ge), and void components were employed under the Bruggeman effective medium approximation to represent wetting of the SiO2 surface, nucleation of Ge seeds for the subsequent dot/island formation, and steady-state dot/island growth. A combination of c-Ge and a-Ge represents intermediate crystallinity, and void represents vacant space between dots/islands. A single-layer model with a mixture of c-Ge, a-Ge, and void components was used for crude estimation of the composition from which the time evolution of the volume fraction of the components was derived. However, fitting in the early growth stage resulted in an unrealistic structure, indicating that the dielectric function of the thin hydrogenated Ge network layer was very different from those of c-Ge and a-Ge. The optical spectra of dots/islands at the intermediate growth stage could be reproduced by a two-layer model consisting of a (a-Ge + void) layer overlaid on a (c-Ge + void) base layer. The real-time Ψ–Δ trajectories of ellipsometric angles monitored at a photon energy of 3.4 eV consisted of three branches. They could be reproduced by assuming the growth of an outer layer with an appropriate composition. After wetting on SiO2 (branch 1), the Ge seed layer nucleates while the volume fraction of Ge rapidly decreases from 70% to 25% with proceeding growth (branch 2). Then, the volume fraction of Ge continuously increases up to 65%, eventually reaching steady-state dots/island growth (branch 3)

Optical and electronic properties of defect chalcopyrite ZnGa2Se4: Experimental and theoretical investigations

The optical properties of ZnGa2Se4 single crystals obtained by gas transport reaction have been systematically explored using ellipsometry measurements and first-principles calculations. Analysis of X-rays diffraction pattern showed that the compound has a single-phase and tetragonal structure (space group (I4‾2 m)). The determined and calculated lattice parameters are in good agreement with each other. Spectral dependence of optical parameters; real εr and imaginary εi parts of the pseudodielectric function, absorption and reflectivity coefficients were obtained from the analysis of ellipsometry measurements. Absorption coefficient–photon energy dependency revealed the existence of direct band gap transitions with an energy of 2.81eV. This result is very close to the band gap obtained from our theoretical calculation. To explore the origins of the interband optical transitions theoretical group analysis was carried out.

DFT Calculations Using Quantum ESPRESSO for Optical and Electronic Properties of Si Crystal

The DFT calculations were performed to study the structural, electronic and optical properties of Si. The open source computer code, Quantum ESPRESSO used is for first-principles electronic structure modeling based on density functional theory. The optimized crystal lattice constant, band gap, density of states (DOS) and band structure were calculated. The calculated value of lattice constant was in good agreement with reported value. The band gap was calculated using three different pseudo potentials. The HSE hybrid functional provided best agreement of band gap calculations with literature values. The pseudo-dielectric functions was also calculated to estimate the optical properties including refractive indices, extinction coefficients, reflectivities and absorption coefficients in the spectral energy ranges from 0 eV to 10 eV.

Pseudo-dielectric function spectra of the near surface layer of GaAs implanted with various fluence of Xe+ ions

Monocrystalline (100) semi-insulating gallium arsenide (GaAs) samples were irradiated with a 250-keV Xe+ ion beam at room temperature. To investigate the effect of ion irradiation on GaAs samples, the ion fluence was varied from 1 × 1012 to 3 × 1016 ions/cm2. The spectroscopic ellipsometry (SE) method and the Rutherford backscattering spectrometry (RBS) with nuclear reaction (NR) method were used to determine the properties of the virgin and implanted samples. The SE approach reveals that the pseudo-dielectric function of implanted GaAs samples varies with ion fluence. The RBS approach, which exposes the depth-profile of As, Ga, and Xe in the implanted samples, allows us to correlate changes in the pseudo-dielectric function with structural modifications caused by the ion irradiation. The NR approach points out the existence of an oxygen-enriched layer on the surface of implanted GaAs samples. Lastly, the optical study involving the Cauchy and Urbach dispersion model measures the refractive index n and extinction coefficient k of the native oxide layer on the surface of GaAs samples.

Spectroscopic ellipsometry study of dielectric functions of Ag films and chemically deposited layers of Ag nanoparticles on silicon

The optical properties of thin films and layers of Ag nanoparticles on a c-Si substrate are modeled by calculating the complex pseudo-dielectric function <ε>. The evolution of the imaginary part <ε2> with an increase in the thickness of continuous layers from the dielectric function ε of the substrate to ε of bulk silver is studied, which demonstrates the appearance of optical characteristics of Ag and the suppression of c-Si features in the form of critical points. The data measured on the spectroscopic ellipsometer for Ag films produced by magnetron sputtering for several nominal thicknesses from 10 to 300 nm, and layers of Ag nanoparticles chemically deposited on a c-Si substrate, were interpreted using a pseudo-dielect ric function and by calculating the complex dielectric functions ε using the Drude-Lorentz model. Morphological parameters obtained by atomic force microscopy and scanning electron microscopy were also used in the calculations. Since the Ag layers and films were deposited on the c-Si substrate without any additional layers (except for the native layer), the determined pseudo-dielectric functions for thicknesses in the range of 7−50 nm turned out to be close to the calculations of the dielectric functions using the Drude-Lorentz model. It was found that in the calculated and experimental spectra in the imaginary part of ε2 and <ε2> a peak appears at E ∼ 3.9 eV, which is interpreted as a plasmon resonance in the longitudinal mode at oblique incidence of light. In the ε2 spectrum of a layer of disordered Ag nanoparticles produced by chemical deposition, there is a broader localized surface plasmon resonance peak at E ∼ 2.5 eV, in contrast to thin films. Whereas, in a layer of larger nanoparticles, the peak is absent, and its ε dependence is close to ε for bulk Ag.

Bi Layer Properties in the Bi–FeNi GMR-Type Structures Probed by Spectroscopic Ellipsometry

Bismuth (Bi) having a large atomic number is characterized by a strong spin–orbit coupling (SOC) and is a parent compound of many 3D topological insulators (TIs). The ultrathin Bi films are supposed to be 2D TIs possessing a nontrivial topology, which opens the possibility of developing new efficient technologies in the field of spintronics. Here we aimed at studying the dielectric function properties of ultrathin Bi/FeNi periodic structures using spectroscopic ellipsometry. The [Bi(d)–FeNi(1.8 nm)]N GMR-type structures were grown by rf sputtering deposition on Sitall-glass (TiO2) substrates. The ellipsometric angles Ψ(ω) and Δ(ω) were measured for the grown series (d = 0.6, 1.4, 2.0, and 2.5 nm, N = 16) of the multilayered film samples at room temperature for four angles of incidence of 60∘, 65∘, 70∘, and 75∘ in a wide photon energy range of 0.5–6.5 eV. The measured ellipsometric angles, Ψ(ω) and Δ(ω), were simulated in the framework of the corresponding multilayer model. The complex (pseudo)dielectric function spectra of the Bi layer were extracted. The GMR effects relevant for the studied Bi–FeNi MLF systems were estimated from the optical conductivity zero-limit (optical GMR effect). The obtained results demonstrated that the Bi layer possessed the surface metallic conductivity induced by the SOC effects, which was strongly enhanced on vanishing the semimetallic-like phase contribution on decreasing the layer thickness, indicating its nontrivial 2D topology properties.

Coherent Acoustic Phonon Oscillations and Transient Critical Point Parameters of Ge from Femtosecond Pump–Probe Ellipsometry

Herein, the complex pseudodielectric function of Ge and Si from femtosecond pump–probe spectroscopic ellipsometry with 267, 400, and 800 nm pump–pulse wavelengths is analyzed by fitting analytical lineshapes to the second derivatives of the pseudodielectric function with respect to energy. This yields the critical point parameters (threshold energy, lifetime broadening, amplitude, and excitonic phase angle) of and in Ge and in Si as functions of delay time. Coherent longitudinal acoustic phonon oscillations with a period of about 11 ps are observed in the transient critical point parameters of Ge. From the amplitude of these oscillations, the laser‐induced strain is found to be on the order of 0.03% for Ge measured with the 800 nm pump pulse, which is in reasonable agreement with the strain calculated from theory.

The spectroscopic ellipsometry measurement of non-polar freestanding GaN: comparison between isotropic and anisotropic models

For anisotropic materials, the pseudo-dielectric function (DF) from isotropic model is often applied in spectroscopic ellipsometry data analysis instead of the DF from anisotropic model because of its simplicity. Whether this approximation is applicable depends on the discrepancy between the pseudo-DF and the DF, which we find to be related to the illumination configuration greatly. For the ellipsometry spectra obtained from a non-polar freestanding GaN in two configurations with the c-axis perpendicular and parallel to the incident plane respectively, both anisotropic model and isotropic model are used to compare the difference between the fitted absorption coefficient and pseudo-absorption coefficient. As a consequence, the discrepancy between the two coefficients is less than 10 even at the absorption edge when electric field is perpendicular to the c-axis, while the discrepancy exceeds 40 at the absorption edge when electric field is parallel to the c-axis. These results indicate that the approximation of using isotropic model instead of anisotropic model is reasonable in the former configuration, while it is not applicable in the latter configuration and will render an overestimation of bandgap. The above two different discrepancies could be explained by the first-order term approximation of pseudodielectric function. We further demonstrate the necessity for anisotropic model by comparing the deviations of the crystal-field splitting obtained from anisotropic and isotropic model with the theoretical value respectively.

Strain and annealing temperature effects on the optical properties of GaNAs layers grown by molecular beam epitaxy

The ex-situ characterization of GaNAs/GaAs system grown by Molecular Beam Epitaxy with two different GaNAs layer thicknesses and similar nitrogen concentration (%N) is presented to explore the residual strain effect in the optimization of the inclusion of nitrogen on the GaAs host matrix by a rapid thermal annealing (RTA). Raman spectroscopy was used to study the effects of post-growth RTA on the alloy´s crystallinity and on %N by analyzing mode´s intensities and frequencies where both an increase of the local vibration mode and lattice disorder with the temperature were noticed. Band structure of the epilayers in the range of 1 to 1.5 eV and their modification with RTA were analyzed by photoreflectance. The E- transition redshifts, indicating increase of nitrogen in the alloy together with a modification of the spectral signature of GaAs by residual strain. Critical points above 1.5 eV were studied by ellipsometry where clear changes in the line shape of the second derivative of the pseudo-dielectric function imaginary part are produced with RTA, making more evident the presence of E+. The E1, E1+Δ1 and E΄0 transitions were also explored, E1 blue-shifts when the annealing has been successfully applied. With this study we show that in the optimization of GaNAs layers properties through RTA processes not only %N should be considered, but also additional parameters as thickness and strain.

Investigation of dielectric functions of a layer of Ag nanoparticles on silicon using spectro-ellipsometry and spectrophotometry

An investigation of the optical characteristics of a layer of Ag nanoparticles deposited from an AgNO3 solution on the surface of single-crystal Si is presented. The measurements were carried out using spectroscopic ellipsometry and spectrophotometry at the same tilt angle and sample probe location in a wide spectral range from 200 to 1700 nm. From the obtained experimental data, the parameters of the Drude-Lorentz model and the complex dielectric function were determined, which was compared with the pseudo-dielectric function. Both dependences revealed resonances of a bulk plasmon near the energy E = 3.8 eV, while a localized plasmon was detected in the pseudo-dielectric function at E = 1.65 eV, and in the dielectric function at E = 1.84 eV. Keywords: dielectric function, Drude-Lorentz model, silver nanoparticles, plasmon, pseudo-dielectric function, spectrophotometry, ellipsometry

Исследование диэлектрических функций слоя наночастиц Ag на кремнии с помощью спектроэллипсометрии и спектрофотометрии

An investigation of the optical characteristics of a layer of Ag nanoparticles deposited from an AgNO3 solution on the surface of single-crystal Si is presented. The measurements were carried out using spectroscopic ellipsometry and spectrophotometry at the same tilt angle and sample probe location in a wide spectral range from 200 to 1700 nm. From the obtained experimental data, the parameters of the Drude-Lorentz model and the complex dielectric function were determined, which was compared with the pseudo-dielectric function. Both dependences revealed resonances of a bulk plasmon near the energy E = 3.8 eV, while a localized plasmon was detected in the pseudo-dielectric function at E = 1.65 eV, and in the dielectric function at E = 1.84 eV.

Modeling of plasmon resonance of silver nanoparticles on a silicon surface

Silver nanoparticles have unique optical properties due to resonance effects that arise due to the presence of conduction electrons in them. When these electrons interacte with photons, they can create localization of electric fields at the interfaces with the environment. Silver nanoparticles deposited on a transparent substrate are often used for research, while Ag nanostructures on Si are studied in this work. They have great potential for practical applications. The interaction of light with nanostructures can be described using various models (pseudo-dielectric functions, effective medium, thin-layer structures, etc.) and optical methods for the experimental determination of their parameters (refractometry, spectrophotometry). Bulk plasmon resonance is considered in this work, which is excited when plasmons are excited at their resonant frequency by an external electromagnetic wave. Calculations were performed for different diameters of silver nanoparticles on a silicon substrate with different structure periods. The calculated spectra are in good agreement with the experimental data of the obtained samples. As a result of the plasmon resonance modeling, the position of the plasmon resonance depends on the density of the arrangement of silver nanoparticles, with an increase in the displacement resonance towards the long-wavelength region.

Bismuth layer properties in the ultrathin Bi–FeNi multilayer films probed by spectroscopic ellipsometry

Using wideband (0.5–6.5 eV) spectroscopic ellipsometry, we study ultrathin [Bi(0.6–2.5 nm)–FeNi(0.8,1.2 nm)]N multilayer films grown by rf sputtering deposition, where the FeNi layer has a nanoisland structure and its morphology and magnetic properties change with decreasing the nominal layer thickness. From multilayer model simulations of the ellipsometric angles, Ψ(ω) and Δ(ω), complex (pseudo)dielectric function spectra of the Bi layer were extracted. The obtained results demonstrate that the Bi layer can possess the surface metallic conductivity, which is strongly affected by the morphology and magnetic properties of the nanoisland FeNi layer in GMR-type Bi–FeNi multilayer structures.