Optical functions of InGaP/GaAs epitaxial layers from 0.01 to 5.5 eV

In_0.49Ga_0.51P films, both undoped and doped n- and p-type (up to 10¹⁸ cm^-3), were grown lattice matched on GaAs substrates, with different miscut angles, by Metal-Organic Vapour Phase Epitaxy (MOVPE) at different temperatures. The shift of the fundamental gap E₀, caused by “ordering effect” was measured as a function of temperature by photoluminescence. The complex refractive index = n + ik and the dielectric function = ɛ ₁ + iɛ ₂ at room temperature were determined from 0.01 to 5.5 eV by using complementary data from fast-Fourier-transform far-infrared (FFT-FIR), dispersive, and ellipsometric spectroscopies. The effect of the native oxide was accounted for and the self-consistency of the optical functions was checked in the framework of the Kramers-Kronig causality relations. In the restrahlen region the dielectric function was well fitted by classical Lorentz oscillators; in the transparent region below E₀, the refractive index was modelled by a Sellmeier dispersion relation; in the interband region the dielectric function was well reproduced by analytical lineshapes associated to seven critical points. Thus parametrized analytical expressions were obtained for the optical functions all over the spectral range, without discontinuities, to be used in the modelling and characterization of multi-layer structures, also on opaque substrates. Received 13 December 2001 Published online 25 June 2002     

Third harmonic generation of laser radiation in Fe- and Zn-doped polyvinylpyrrolidone

The results of third-order nonlinear susceptibilities studies of Fe- and Zn-doped polyvinylpyrrolidone (PVP) aqueous solution in processes of third harmonic generation of Nd:YAG laser radiation are presented. Nonlinear susceptibilities of PVP:Fe and PVP:Zn were calculated to be 5×10^-13 esu and 3×10^-13 esu respectively. Third harmonic conversion efficiencies in these metallocomplexes were measured to be 8×10^-7 and 5×10^-7 respectively. The Z-scan method was applied to determine Kerr effect influence on frequency conversion process. The value of nonlinear refractive index of PVP:Fe at the wavelength of λ = 1064 nm was measured to be n ₂ = - 6.7×10^-13 esu. Received 30 November 2001 / Received in final form 27 March 2002 Published online 28 June 2002     

Polarized infrared reflectivity study of an oriented ceramic of Bi 2 Sr 2 Ca 2 Cu 3 O 10 + δ (Bi-2223)

The reflectivity spectra of an oriented ceramic of Bi-2223 has been investigated by polarized infrared reflectivity spectroscopy in the energy range 0.005-2.2 eV. It is shown that the data for the polarization parallel to the c axis cannot be fitted with a one-component Drude or extended-Drude model. The conductivity spectrum is then obtained from the best fit of a “double-damping Drude” model to reflectivity spectra, itself derived from the factorized form of the dielectric function, and by a Kramers-Kronig inversion as well. The data and their analysis give a new insight of the 2D character of the system. Received 26 April 2001 and Received in final form 28 August 2001     

Optical properties and temperature dependence of critical transitions in ZnSe

The dielectric function of ZnSe has been deduced from ellipsometric measurements between 20 K and 380 K. is analysed around each critical point with the standard critical point model. The variations of the different parameters characterising each transition with temperature are presented and analysed. The temperature coefficients of the energies of the critical transitions are given. is essentially governed by the Coulomb interaction near the fundamental gap. Thanks to the high binding energy of the exciton and the low spectral width of the ellipsometer, the fundamental state of the exciton is found completely separated from the first excited states and the continuum at low temperature. In return the strong transition E₁ near the L points of the Brillouin zone can be described equally well with a 2D or an excitonic transition. Received 5 February 1999 and Received in final form 15 June 1999     

An improved reflectometric method to measure the azimuthal anchoring energy of nematic liquid crystals

Some years ago we developed an automatized reflectometric method to measure the surface azimuthal anchoring energy of nematic liquid crystals on an optically isotropic substrate. This method provides a high accuracy and sensitivity but requires the use of wedge glass plates and a sufficiently high anisotropy of the intensity reflectivity coefficients. This latter condition restricts greatly the number of possible substrates that can be investigated with this technique. Here we develop a new reflectometric method which offers comparable or better accuracy and sensitivity but does not require wedge plates and high anisotropy of the reflectivity coefficients. The method is fully automated and provides a direct measurement of the azimuthal director angle. The experimental procedure exploits the dependence of the reflectivity tensor on the surface director orientation. The measurement of the azimuthal angle does not require any knowledge of the optical parameters of the nematic material and of the optically isotropic substrate, and provides an absolute accuracy better than 0.2^° in the whole range 0-360^° and a sensitivity better than 0.1^°. This reflectometric method can be also used with weakly anisotropic substrates as well as thin rubbed polymeric layers. In this latter case, the effective uncertainty in the measurement of the director azimuthal angle depends on the substrate anisotropy. A simple and direct experimental procedure to estimate this uncertainty is proposed. Received 8 January 2002 and Received in final form 27 February 2003 / Published online: 15 April 2003 RID="a" ID="a"e-mail: faetti@df.unipi.it     

Photoreflectance investigation of hydrogenated (InGa)(AsN)/GaAs heterostructures

The optical response of as grown and hydrogenated In_0.32Ga_0.68As_1-yN_y/GaAs single quantum wells (y = 0, 0.027) has been investigated from T = 80 K to room temperature by photoreflectance. Three excitonic spectral features detected in the N free sample shift to lower energy in the N containing sample and back to higher energy upon H irradiation of the N containing sample. In the hydrogenated sample, a progressive change with increasing temperature of the nature of the lowest energy transition from an excitonic to a band-to-band character has been explained in terms of an increasing release of carriers from traps formed by H and N clusters. A reduction in the oscillator strength of the lowest energy transition and an increase in the binding energy of the heavy-hole exciton have been explained in terms of an increase in the electron effective mass upon N introduction into the In_xGa_1-xAs lattice. Received 23 June 2002 Published online 19 November 2002     

Structural, electronic and optical properties of SrCl2 under hydrostatic stress

The results of first-principles theoretical study of the structural, electronic and optical properties of SrCl₂ in its cubic structure, have been performed using the full-potential linear augmented plane-wave method plus local orbitals (FP-APW+lo) as implemented in the WIEN2k code. In this approach both the local density approximation (LDA) and the generalized gradient approximation (GGA) are used for the exchange-correlation (XC) potential. Also we have used the Engel-Vosko GGA formalism, which optimizes the corresponding potential for band structure calculations. We performed these calculations with and without spin-orbit interactions. Including spin-orbit coupling cause to lifts the triple degeneracy at Γ point and a double degeneracy at X point. Results are given for structural properties. The pressure dependence of elastic constants and band gaps are investigated. The dielectric function, reflectivity spectra and refractive index are calculated up to 30 eV. Also we calculated the pressure and volume dependence of the static optical dielectric constant.     

Pump and probe nonlinear processes: new modified sum rules from a simple oscillator model

The nonlinear oscillator model is useful to basically understand the most important properties of nonlinear optical processes. It has been shown to give the correct asymptotic behaviour and to provide the general features of harmonic generation to all orders, in particular dispersion relations and sum rules. We investigate the properties of pump and probe processes using this model, and study those cases where general theorems based on the holomorphic character of the Kubo response functions cannot be applied. We show that it is possible to derive new sum rules and new Kramers-Kr?nig relations for the two lowest moments of the real and of the imaginary part of the third order susceptibility and that new specific contributions become relevant as the intensity of the probe increases. Since the analytic properties of the susceptibility functions depend only upon the time causality of the system we are confident that these results are not model dependent and therefore have a general validity, provided one substitutes for the equilibrium values of the potential derivatives the density matrix expectation values of the corresponding operators. Received 25 January 1999 and Received in final form 26 April 1999     

Properties of two-photon fluorescence and superradiance of a new organic dye C46H51N2B

Linear and nonlinear optical properties of a new organic dye, trans-4-[p-(N-n-butyl-N-n-butylamino)-styryl]-N-methyl-pyridinium tetraphenylborate solution in dimethyl formamide (DMF) have been studied systematically. When excited with mode-locked picosecond 1 064 nm laser beam, intense upconversion fluorescence and superradiance can be obtained. The temporal behaviors of one-photon absorption and two-photon absorption (TPA) fluorescence and superradiance have been studied. The highest upconversion efficiency was found to be 4.1% at a pump energy of 4 mJ. By using an optical parameter amplifier (OPA) as the pump laser, the nonlinear transmittance and upconversion efficiencies of the dye solution at different wavelengths were measured. The strongest linear absorption was found at a wavelength of 930 nm whereas the highest upconversion efficiency was at 1 030 nm. The 100 nm red-shift for the highest upconversion efficiency wavelength compared with the strongest nonlinear absorption are caused by excited state absorption. Received 17 October 2001 and Received in final form 21 December 2001     

Optical properties of silver clusters formed by ion irradiation

Precipitation of silver clusters in silica is achieved by different methods: ion implantation, ion beam mixing of superimposed layers and ion irradiation of films deposited by means of co-sputtering or sol-gel technique. Main features of the nanoparticles depending on the preparation method are investigated by TEM. The optical extinction resonance of these clusters is analysed in terms of sizes and interaction between the clusters on the basis of calculations. We found that resonances in sputtered and gel films with low metal concentrations are well described by plasmon polaritons in isolated clusters and calculations based on Mie theory allow the study of their growth under irradiation. This theory is not appropriate to describe the optical response of silver clusters in silica implanted with Ag concentrations higher than 5 at.% or in ion beam mixed films, because of the interaction between clusters. Using an effective medium model, it is demonstrated that the random dispersion of clusters in implantation films causes fluctuations and, on average, an increase of the clusters polarization. On the contrary, the particular arrangement of the clusters with a bimodal size distribution in ion beam mixed films induces a screening effect between the clusters of largest size. Received 10 January 2002 / Received in final form 26 April 2002 Published online 19 July 2002     

First principles study of electronic structure and optical properties of CaTiO3

The electronic-energy band structure, site and angular momentum decomposed density of states (DOS) and charge-density contours of perovskite CaTiO ₃ are calculated by the first principles tight-binding linear muffin-tin orbitals method with atomic sphere approximation using density functional theory in its local density approximation. The calculated band structure shows an indirect (R-Γ) band gap of 1.5 eV. The total DOS as well as the partial density of states (PDOS) are compared with the experimental photoemission spectra. The calculated DOS are in reasonable agreement with the experimental energy spectra and the features in the spectra are interpreted by a comparison of the spectra with the PDOS. The origin of the various experimentally observed bands have been explained. From the DOS analysis, as well as charge-density studies, we conclude that the bonding between Ca and TiO ₃ is mainly ionic and that the TiO ₃ entities bond covalently. Using the projected DOS and band structure we have analyzed the interband contribution to the optical properties of CaTiO ₃ . The real and imaginary parts of the dielectric function and hence the optical constants such as refractive index and extinction coefficient are calculated. The calculated spectra are compared with the experimental results for CaTiO ₃ and are found to be in good agreement with the experimental results. The effective number of electrons per unit cell participating in the interband transitions are calculated. The role of band structure calculation as regards the optical properties of CaTiO ₃ is discussed. Received 1 February 2000 and Received in final form 21 July 2000     

Surface and interface effects in the optical properties of silver nanoparticles

We present novel experimental results about influences of surrounding foreign materials on optical properties of small silver clusters. First we show spectra of free cluster beams produced with different seeding gases Ar, Kr, Xe. Second, we estimate, from measured spectra, the cluster deformations and contact areas after deposition on different substrates (Cr₂O₃ and MgF₂) at room temperature and on SiO₂ at 110 K and between 160 K and 300 K. Third, we present and compare the static and dynamic charge transfer after embedding the clusters in various fluorides and compare with previous results on oxides. Received 2 September 1998 and Received in final form 3 January 1999     

Importance of lattice contraction in surface plasmon resonance shift for free and embedded silver particles

The size evolution of the surface plasmon resonance was investigated for free and embedded silver particles between about 2 to 10 nm in size. The crystal lattice of such particles as analyzed by high resolution electron microscopy show linear contraction with reciprocal particle size. Based on this, a model was presented by combining the lattice contraction of particles and the free path effect of electrons to predict the size evolution of the resonance. The results reveal a contribution of the lattice contraction to the resonance shift according to a roughly linear relation that changes slightly with particle radius (> 1.0 nm) and surrounding media. This surface plasmon resonance shift proceeds linearly with reciprocal size for Ag particles in vacuum and argon, but for Ag particles embedded in glass it appears to be independent of the radius down to nearly 1 nm. All predictions are quantitatively compared to previously reported experimental data and a good agreement is obtained. An unusual red-shift observed for Ag particles in glass may be attributed to a thermal expansion mismatch induced lattice dilatation. Received 26 July 2000 and Received in final form 14 September 2000     

Optical properties of ZnO related to the dc sputtering power

Zinc oxide thin films were sputter deposited on (100) silicon substrates at 250 ^○C substrates temperature via reactive unbalanced dc magnetron process using pure zinc target and argon/oxygen gases. The influence of the applied dc sputtering power (between 100 to 250 Watts, step 50 Watts) on the optical properties of the grown films was systematically investigated by variable angle of incidence spectroscopic ellipsometry (VASE) technique. The refractive indices were found to follow the second-order Sellmeier dispersion relation. However, Cauchy-like dispersion model was formulated to account for the absorption tail and excitonic structure near the direct band gap. The optical properties such as refractive indices, extinction coefficients, optical band gaps, Urbach's energies, excitonic binding structure and absorption coefficients of the grown films were reported as a function of dc power in the photon energy range between 1.2 eV and 4.2 eV. The films were found to be polycrystalline with (002) preferred orientation.     

Detecting a true quantum pump effect

Reflectance measurements from p-type GaSb:Zn epitaxial films with different hole concentrations (10¹⁷–10¹⁸ cm^-3) have been investigated over the frequency region of 100–1000 cm^-1. A minimum broadening feature corresponding to the hole plasmon was observed in the reflectance spectra. The experimental infrared spectra were well fitted using a Lorentz-Drude dispersion model. The real part ε₁ of the dielectric function decreases with increasing hole concentration. However, the imaginary part ε₂ increases with hole concentration in the far-infrared region. This indicates that the acoustic- and optic-phonons mainly participate in the free carrier absorption processes. The hole mobility obtained from Hall-effect measurements is slightly larger than that derived from optical measurements and the average ratio of mobilities is estimated to be 1.33. Owing to overdamping effects, the upper branch of longitudinal-optical phonon plasmon (LPP) coupled modes was observed. The upper LPP⁺ frequency increases with hole concentration and it shows a transition from phonon-like to plasmon-like behavior. A theoretical analysis with solutions in the complex frequency plane describes these experimental results.     

Photophysics of C<Subscript>60</Subscript> and C<Subscript><Emphasis Type="Bold">60</Emphasis></Subscript><Superscript><Emphasis Type="Bold">-</Emphasis></Superscript> in faujasite zeolites

While the intercalation of C₆₀ and the formation of C ₆₀ ^- in the supercages of NaX and NaY are confirmed by using ¹²⁹Xe NMR and ESR, the photophysical properties of C₆₀ and C ₆₀ ^- are characterized by monitoring transient reflectance spectra and kinetics, fluorescence kinetics, and diffuse reflectance spectra. C ₆₀ ^- is considerably more abundant in NaY than in NaX. This difference is explained in terms of polarity difference between two zeolites. Both C₆₀ and C ₆₀ ^- have remarkably elongated excited-state lifetimes due to their collision-free environment in zeolitic nanocavities although C ₆₀ ^- has much shorter lifetimes than C₆₀. C ₆₀ ^- , in particular, shows intense absorption and emission due to its reduced symmetry in zeolites. Received 13 July 2001 and Received in final form 8 October 2001     

Extinction theorem and propagation of electromagnetic waves between two anisotropic materials

We systematically investigate the reflection and refraction of an electromagnetic wave between two semi-infinite anisotropic magnetoelectric materials. Using the integral formulation of Hertz vectors and the principle of superposition, we generalize the extinction theorem and derive the propagation characteristics of wave. Applying the results obtained, we find a general origin of Brewster effect. We also show that, through choosing appropriate material parameters, oblique or omnidirectional total transmission can occur to TE and TM waves. Compared to the traditional method, the method used here discloses the underlying mechanism of wave propagation between two arbitrary anisotropic materials and can be applied to other problems of propagation.     

Fully relativistic calculations of the L2,3-edge XANES spectra for vanadium oxides

Fully relativistic multielectron method based on the numerical solution of the Dirac equation was used to calculate the L_2,3-edge X-ray absorption near edge structure (XANES) spectra of VO₂, V₂O₃, and V₂O₅ crystals. The key-points of the method are: i) usage of the molecular orbitals (MO); ii) absence of any fitting parameters; iii) wide area of application: to any ion in any symmetry; iv) possibility of numerical analysis of the MO composition. The calculated spectra are in a satisfactory agreement with experimental data available in the literature, including the absolute values of the transitions energy, the shape of the absorption bands, and polarization dependence. The assignment of the absorption bands in terms of the electronic configurations was done. The structure of the absorption bands is attributed to the splitting of the vanadium p- and d-orbitals; the magnitude of this splitting is estimated from the spectra. Covalency effects were considered for all hosts; it was shown that the contribution of the oxygen wave functions increases with increasing the vanadium oxidation state. Dependence of the relative positions of the vanadium 3d and oxygen 2p levels and energies of the “ligand–metal” charge transfer transitions on the vanadium oxidation state was analysed.     

Magneto-optical Kerr effect in bilayer structures

This paper describes the magneto-optical effects and the reflectivity behaviors of bilayers based on magnetic and isotropic ()/anisotropic () layers under the condition of total internal reflection. In the framework of Green's dyadic technique, we show accurately the optical properties of anisotropic layers deposited on a substrate. We present numerical simulations which account for the variation of angle of incidence at the HeNe laser wavelength. The Kerr rotation is found to increase significantly around the optical modes in total reflection. We also discuss the importance of anisotropic effects due to the crystallization of the dielectric material () which occur in the reflectivity and Kerr rotation spectra. Received 26 January 2000     

Angular tuning of defect modes spectrum in the one-dimensional photonic crystal with liquid-crystal layer

A one-dimensional ZrO₂/SiO₂ photonic crystal with a 4-n -pentyl-4' -cyanobiphenyl (5CB) nematic defect layer was used to investigate the transmission spectra of light polarized parallel and perpendicular to the liquid-crystal director at different angles of incidence. The spectra of the photonic crystal were shown to split into four polarized components T_ij at oblique incidence. When the incident angle increased, the bandgap edges and the defect modes shifted towards short wavelengths, while the amplitudes of the defect modes increased for the transverse magnetic polarization and decreased for the transverse electric polarization. The observed discrepancy between the defect mode amplitudes in the center and near the edges of the photonic bandgap was found to be related to the radiation losses inside the defect layer of a non-ideal photonic crystal. The simulated transmission spectra obtained using recurrence relations and taking into account the decay of defect modes are in good agreement with the experimental data.