Optical and waveguiding properties of Nd:KGW films grown by pulsed laser deposition

 Nd: KGd(WO₄)₂ thin films were deposited by KrF laser ablation on MgO, YAP, YAG and Si substrates at temperatures up to 800 °C. Film crystallinity, morphology, stoichiometry (WDX, RBS and PIXE), excitation spectra, fluorescence, refractive index and waveguiding properties were studied in connection with deposition conditions. The best films were crystalline and exhibited losses of approximately 5 dB cm^-1 at a wavelength of 633 nm. Received: 8 January 2001 / Accepted: 7 November 2001 / Published online: 11 February 2002     

Anomalous dispersion in nanocomposite films at the surface plasmon resonance

Nanocomposite thin films formed by Cu nanocrystals (NCs) embedded in an amorphous aluminium oxide (Al₂O₃) host have been prepared by alternate pulsed laser deposition. Spectroscopic ellipsometry is used to determine the effective refractive index (n=n+ik). The extinction coefficient is non-negligible and shows a broad absorption band related to the surface plasmon resonance. In the neighbourhood of this wavelength, the real part of the refractive index undergoes an anomalous dispersion, leading to a significant increase of the n value of the composite compared to that of the host. When the Cu content is low enough, about 2 at. %, the use of an effective medium approach combined with a regression method allows us to determine the metal content and film thickness from the ellipsometric measurements. For larger concentrations this approach is no longer valid. Received: 31 July 2001 / Revised version: 21 September 2001 / Published online: 15 October 2001     

Optical properties of SrTiO<Subscript>3</Subscript> thin films by pulsed laser deposition

SrTiO₃ thin films were prepared on a fused-quartz substrate by pulsed laser deposition (PLD). Dense and homogeneous films with a thickness of 260 nm were prepared. Optical constants (refractive index n and extinction coefficient k) were determined from the transmittance spectra using the envelope method. The optical band gap energy of the films was found to be 3.58 eV, higher than the 3.22 eV for bulk SrTiO₃, attributable to the film stress exerted by the substrate. The dispersion relation of the refractive index vs. wavelength follows the single electronic oscillator model. The refractive index and the packing density for the PLD-prepared SrTiO₃ thin films are higher than those for the SrTiO₃ films prepared by physical vapor deposition, sol–gel and RF sputtering. Received: 18 March 2002 / Accepted: 7 October 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: mszhang@nju.edu.cn     

Structure, refractive-index dispersion and the optical absorption edge of chemically deposited ZnxCd(1-x)S thin films

Zinc cadmium sulfide, Zn_xCd_(1-x)S, thin films have been deposited by a simple and inexpensive chemical bath deposition method from an aqueous medium using thiourea as a sulfide-ion source. The structure of the deposited films has been characterized by X-ray diffraction and transmission electron microscopy. It was observed from X-ray diffraction that the as-deposited films were amorphous in nature. However Zn_xCd_(1-x)S films annealed at 423 K for 1.5 h show a crystalline structure with a small scattering volume. The obtained results were confirmed throughout the transmission electron microscopy and the corresponding electron-diffraction patterns. The optical constants of Zn_xCd_(1-x)S films annealed at 423 K for 1.5 h in the compositional range 0≤x≤1 were estimated using transmission and reflection spectra in the wavelength range 300–2500 nm. The band gap varies non-linearly with the value of x. The dependence of the refractive index on the wavelength obeys the single-oscillation model, from which the dispersion parameters and the high-frequency dielectric constant were determined. A graphical representation of the surface and volume energy-loss functions was also given. Received: 23 February 2001 / Accepted: 26 February 2001 / Published online: 27 June 2001     

Optical constants of 3,4,9,10-perylenetetracarboxylic dianhydride films on silicon and gallium arsenide studied by spectroscopic ellipsometry

The optical constants of 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) films grown by organic molecular beam deposition on Si and GaAs substrates were determined in the spectral range from 300 nm to 1700 nm. All PTCDA layers deposited at room temperature with a low deposition rate of about 0.2 nm/min are uniaxial and strongly optically anisotropic. For the layers on Si a refractive index of 2.21 is derived in the substrate plane at 830 nm. The out-of-plane refractive index has a much lower value of 1.58. A similar anisotropy is observed for PTCDA layers on GaAs. The altogether lower refractive indices of 2.03 and 1.54, however, indicate a lower density of the films, which can be explained by the film structure. Received: 6 November 2000 / Accepted: 10 August 2001 / Published online: 17 October 2001     

Holographic recording mechanisms of gratings in indium oxide films using 325 nm helium–cadmium laser irradiation

UV (325 nm) holographic recording of gratings in indium oxide films fabricated by reactive pulsed laser deposition has been investigated as a function of growth temperature, oxygen pressure and angle of incidence of the plasma plume on the substrate. The influence of the ambient environment (air or vacuum) and the film temperature during recording has also been studied. Large steady state refractive index changes up to 6×10^-3 were observed in layers grown at an oblique angle of 75°. About 77% of the magnitude of these changes residues after thermal annealing and is attributed to UV-induced permanent structural rearrangements. In contrast, refractive index changes in films grown at normal incidence were smaller in magnitude and completely reversible. Received: 30 July 2001 / Accepted: 20 November 2001 / Published online: 23 January 2002     

Growth and characterization of silicon nitride films on various underlying materials

Characteristics of silicon nitride (SiN_x:H) films, grown by plasma enhanced chemical vapor deposition (PECVD) on various metals such as Ta, IrMn, NiFe, Cu, and CoFe at various temperatures down to 100 °C, were studied using measurements of BHF etch rate, surface roughness and Auger electron spectroscopy (AES). The results were compared with those obtained for SiN_x:H films on Si. The deposition rate of SiN_x:H films increased slightly as deposition temperature decreased, and showed a weak dependence on the underlying materials. The surface of the nitride films deposited on all underlying materials at lower temperatures (below 150 °C) became rougher. In particular, a bubble-like surface was observed on the nitride film deposited on NiFe at 100 °C. At higher deposition temperatures (above 200 °C), SiN_x:H films on all the above metals had small RMS values, except for films on Cu which cracked at 250 °C. BHF (10:1) etch rate increased dramatically for nitride films deposited below 150 °C. For different underlying films, the BHF etch rate was quite different, but exhibited the same trend with decrease in deposition temperature. AES measurements showed that Si and N concentrations in the SiN_x:H films were only slightly different for the various deposition temperatures and underlying materials. AES depth profile of nitride films indicated that both surface O content and the depth of oxygen penetrating into SiN_x:H increased for low temperature-deposited films. However, there was no observed oxygen signal from within the films, even for films deposited at 100 °C, and both Si and N concentrations were uniform throughout the film. Received: 26 October 2001 / Accepted: 2 March 2001 / Published online: 20 June 2001     

Correlation between photoluminescence, optical and structural properties of amorphous nitrogen-rich carbon nitride films

Amorphous nitrogen-rich carbon nitride (CN_x) films have been prepared by inductively coupled plasma chemical vapour deposition (ICP-CVD) utilizing transport reactions from a solid carbon source. The nitrogen atomic fraction N/(C+N) is about 1 or even higher as detected by various surface and bulk sensitive methods. An investigation of the chemical bonding structure showed that the films are composed of >C=N units with a small fraction of C≡N groups. Based on these findings, several structural units derived from cis- and trans-conjugated carbon–nitrogen chains are proposed. The optical properties of the CN_x films were studied by transmission spectroscopy and spectral ellipsometry; the optical Tauc gap was determined to 2.1±0.05 eV. The photoluminescence characteristics were measured at three different excitation wavelengths (476, 488 and 515 nm) and revealed two individual contributions. These data are interpreted in terms of the different structural units comprising the nitrogen-rich CN_x films. Received: 14 July 2000 / Accepted:17 July 2000 / Published online: 22 November 2000     

Structural and electrical characteristics of zirconium oxide layers derived by photo-assisted sol–gel processing

This paper reports the photo-assisted formation of ZrO₂ layers derived by sol–gel processing at low temperatures using intense radiation from ultraviolet (UV) excimer lamps. Excellent layer properties can be readily obtained for these sol–gel layers after 5-min exposure to the UV irradiation at around 300 °C. Analyses of the as-deposited sol–gel layers by UV/VIS spectrophotometry show that the organic species contained in the layers have been removed to a large extent after 5-min irradiation. This is further confirmed by X-ray photoelectron spectroscopy analyses of the same irradiated layers, which indicate the formation of ZrO₂ with little carbon contamination contributed by the organic species and less oxidation of Si at the interface. Electrical measurements of these layers are also reported. Received: 31 July 2001 / Accepted: 6 September 2001 / Published online: 17 October 2001     

A study on the aluminum fire-through to a-SiNx:H thin film for crystalline solar cells

The relationship between aluminum fire-through and the properties of a-SiN_x:H thin films was investigated to aid their use as dielectric layers in rear side and front passivation layers in crystalline solar cells. Aluminum fire-through was shown to depend on the refractive index and the deposition rate of the films.Refractive index, density and deposition rate increased with increasing SiH₄/NH₃ ratio, while the etching rate decreased. Aluminum fire-through occurred in a sample of refractive index 2.0 during fast deposition but not when the deposition rate was slow. Aluminum fire-through occurred during extended firing, despite it not occurring during normal firing by RTP. The results of this work demonstrate that refractive index was the major determinant of aluminum fire-through, and that the aluminum and the a-SiN_x:H thin film reacted immediately at the beginning of firing at a rate determined by the deposition rate.     

An effective compliant substrate for low-dislocation relaxed Si1-xGex growth

An effective compliant substrate for Si_1-xGe_x growth is presented. A silicon-on-insulator substrate was implanted with B and O forming 20 wt % borosilicate glass within the SiO₂. The addition of the borosilicate glass to the buried oxide acted to reduce the viscosity at the growth temperature of Si_1-xGe_x, promoting the in situ elastic deformation of the thin Si (∼20 nm) layer on the insulator. The sharing of the misfit between the Si and the Si_1-xGe_x layers was observed and quantified by double-axis X-ray diffraction. In addition, the material quality was assessed using cross-sectional transmission electron microscopy, photoluminescence and etch pit density measurements. No misfit dislocations were observed in the partially relaxed 150-nm Si_0.75Ge_0.25 sample as-grown on a 20% borosilicate glass substrate. The threading dislocation density was estimated at 2×10⁴ cm^-2 for 500-nm Si_0.75Ge_0.25 grown on the 20% borosilicate glass substrate. This method may be used to prepare compliant substrates for the growth of low-dislocation relaxed SiGe layers. Received: 4 January 2001 / Accepted: 30 May 2001 / Published online: 17 October 2001     

Structural and electrical properties of polycrystalline PbZr0.5Ti0.5O3 films deposited on La0.5Sr0.5CoO3 coated silicon by sol-gel process

La_0.5Sr_0.5CoO₃ (LSCO) films have been grown on Si (100) by a metalorganic chemical liquid deposition (MOCLD) technique using lanthanum acetate, strontium acetate and cobalt acetate as the starting materials. Subsequent PbZr_0.5Ti_0.5O₃ (PZT) films were deposited onto LSCO films by a modified sol-gel method. Field-emission scanning electron microscopy and X-ray diffraction analysis show that PZT and LSCO films are polycrystalline and entirely perovskite phase. At an applied electric field of 250 kV/cm, the Pt/PZT/LSCO capacitor shows no polarization fatigue after 3×10⁹ switching cycles and an internal electric field; the remnant polarization P_r and the coercive field E_c are about 22 μC/cm² and 73 kV/cm, respectively. The dielectric constant of PZT films is 650 at a frequency of 1 kHz. Received: 20 February 2001 / Accepted: 6 June 2001 / Published online: 30 August 2001     

Effect of incorporating nonlanthanoidal indium on optical properties of ferroelectric Bi4Ti3O12 thin films

Bi₄Ti₃O₁₂ (BTO) and Bi_3.25In_0.75Ti₃O₁₂ (BTO:In) thin films were prepared on fused quartz and LaNiO₃/Si (LNO) substrates by chemical solution deposition (CSD). Their microstructures, ferroelectric and optical properties were investigated by X-ray diffraction, scanning electron microscope, ferroelectric tester and UV-visible-NIR spectrophotometer, respectively. The optical band-gaps of the films were found to be 3.64 and 3.45 eV for the BTO and BTO:In films, respectively. Optical constants (refractive indexes and extinction coefficients) were determined from the optical transmittance spectra using the envelope method. Following the single electronic oscillator model, the single oscillator energy E₀, the dispersion energy E_d, the average interband oscillator wavelength λ₀, the average oscillator strength S₀, the refractive index dispersion parameter (E₀/S₀), the chemical bonding quantity β, and the long wavelength refractive index n_∞ were obtained and analyzed. Both the refractive index and extinction coefficient of the BTO:In films are smaller than those of the BTO films. Furthermore, the refractive index dispersion parameter (E₀/S₀) increases and the chemical bonding quantity β decreases in the BTO and BTO:In films compared with those of bulk.     

Variable UV laser exposure processing of photosensitive glass-ceramics: maskless micro- to meso-scale structure fabrication

A novel variable UV laser processing technique was developed that enables the concurrent fabrication of structures in photosensitive glass-ceramic (PSGC) materials that range from the micro-scale to the meso-scale domains. This technique combines the advantages of direct-write volumetric laser patterning and batch chemical processing. The merged non-thermal laser fabrication approach relies on the ability to precisely and selectively alter the chemical etch rate of the PSGC by varying the laser exposure during pattern formation. The present study determined that the chemical etch rate of a commercial photosensitive glass-ceramic (Foturan^TM, Schott Corp., Germany) in dilute hydrofluoric (HF) acid is strongly dependent on the incident laser irradiance during patterning at λ=266 nm and λ=355 nm. For low laser irradiances, the etch rate ratio (R_exposed/R_unexposed) increased nearly linearly with laser irradiance. The slopes of the linear ranges of the etch rate ratios were measured to be 435.9±46.7 μm²/mW and 46.2±2.3 μm²/mW for λ=266 nm and λ=355 nm, respectively. For high laser irradiances, the measured etch rate ratio saturated at ∼30:1 with a maximum absolute etch rate of 18.62±0.30 μm/min. The maximum absolute chemical etch rate was independent of the exposure wavelength. Consequently, variation of the laser exposure during direct-write patterning permits the formation of variegated and proximal high and low aspect ratio structures on a common substrate. The results show that adjacent microstructures with aspect ratios ranging from <1:1 to ∼30:1 can be fabricated in a single, simultaneous batch chemical etch step without the need for a complex masking sequence or post-process ablation step. This new technique facilitates rapid prototype processing with pattern and component uniformity, and achieves material processing over large areas without incurring high cost. PACS 42.62.-b; 42.79.-e; 81.05.Kf; 81.20.-n     

Al2O3 thin films by plasma-enhanced chemical vapour deposition using trimethyl-amine alane (TMAA) as the Al precursor

2 O₃ thin films by plasma-enhanced chemical vapour deposition (PECVD) using trimethyl-amine alane (TMAA) as the Al precursor. The thin films were deposited on both Si and quartz silica (SiO₂) substrates. Deposition rates were typically 60 Å min^-1 keeping the TMAA temperature constant at 45 °C. The deposited Al₂O₃ thin films were stoichiometric alumina with low carbon contamination (0.7–1.3 At%). The refractive index ranged from 1.54 to 1.62 depending on the deposition conditions. The deposition rate was studied as a function of both the RF power and the substrate temperature. The structure and the surface of the deposited Al₂O₃ thin films were studied using X-ray diffraction, atomic force microscopy (AFM) and scanning electron microscopy (SEM). Received: 20 May 1997/Accepted: 12 June 1997     

Nitrogen incorporation in amorphous SiCN layers prepared from electron cyclotron resonance plasmas

Electron cyclotron resonance plasma chemical vapor deposition with nitrogen, methane, and argon-diluted silane as precursors has been used to prepare SiCN thin films. Optical emission from CN species in the plasma has been observed. Infrared measurements show that most of the nitrogen is incorporated to the thin solid films in the form of Si-N, C=N and C≡N bonds suggesting a basic structure of incomplete SiN tetrahedra with C=N and C≡N bridging bonds. The deposited films are nearly transparent in the visible range with a weak absorption threshold between 2.2 and 3.5 eV. Received: 3 April 1998 / Accepted: 5 January 1999 / Published online: 31 March 1999     

Metastable phases in HxLi1-xTaO3 waveguide layers and pure LiTaO3

The formation of high-temperature phases in low-doped H:LiTaO₃ waveguide layers in Z-cut LiTaO₃ has been observed both by refractive-index and IR-spectra measurements. This permits us to correlate the index jumps to the changes of the OH bonds in the crystal lattice. Reversible phase transitions were detected in the temperature interval T=50–200 °C over a wide range of hydrogen content including as-grown LiTaO₃. The high-temperature phases are metastable close to room temperature. This was demonstrated by tracing the time evolution of the refractive-index change. It was shown that the high-temperature phases are responsible for the long-term refractive-index instabilities in both H:LiTaO₃ waveguides and virgin LiTaO₃. Received: 7 May 2001 / Revised version: 10 August 2001 / Published online: 30 October 2001     

Group-IV nanocluster formation by ion-beam synthesis

A short review of our investigations devoted to the use of ion-beam-synthesized nanoclusters for silicon-based light emission and nonvolatile memory effects is presented. Blue-violet light emission is demonstrated based on Ge-implanted silicon dioxide layers thermally grown on silicon substrates. This version of silicon-based light emission relies on Ge-related defects in the amorphous ≡Si–O–Si≡ network. The photoluminescence and electroluminescence are excited by a singlet S₀–S₁ transition of a neutral oxygen vacancy and by electron injection from the silicon substrate into the silicon dioxide layer, respectively. Whereas the photoluminescence excitation is a well-known mechanism, for the case of electroluminescence an interpretation was performed for the first time in the course of our studies. It was found that the most probable way to excite luminescence centers is the impact excitation by hot electrons. Whereas the injection is explained by trap-assisted tunneling of electrons from the substrate into the oxide, the electrons will be transported via traps or in the SiO₂ conduction band. The application of the silicon-based light-emitting devices for an integrated optocoupler arrangement is described. Another application of nanoclusters is based on the investigation of thin Si-implanted silicon dioxide layers for nonvolatile memory devices. First promising results demonstrate that the observed programming window can reach several volts and the devices exhibit excellent retention behavior. A 256 K-nv-SRAM is demonstrated showing a programming window of >1 V for write pulses of 12 V/8 ms. Received: 21 August 2002 / Accepted: 21 August 2002 / Published online: 12 February 2003 RID="*" ID="*"Corresponding author. Fax: +49-351/260-3411, E-mail: w.skorupa@fz-rossendorf.de     

Nonlinear refraction and absorption in hetero- thiometallic planar clusters

The nonlinear absorption and refraction of the clusters [MoS₄Cu₄Br₂(py)₆] and [Et₄N]₂[MoS₄Cu₄(SCN)₄(2-pic)₄] have been investigated using the z-scan technique with a ns laser at 532 nm wavelength. They have the same planar ‘open’ structures and the same skeleton metal atoms; the only difference is that the former has halogen ligands while the latter possesses pseudo-halogen groups – SCN – as ligands. Alteration of nonlinear refractive index and enhancement of nonlinear absorption were found in these two clusters. A steady state model of excited state nonlinear refraction was proposed to explain this phenomenon. Received: 12 June 2001 / Revised version: 4 September 2001 / Published online: 29 November 2001     

Characterization of LaF3 coatings prepared at different temperatures and rates

LaF₃ thin films were prepared by thermal boat evaporation at different substrate temperatures and various deposition rates. X-ray diffraction (XRD), Lambda 900 spectrophotometer and X-ray photoelectron spectroscopy (XPS) were employed to study crystal structure, transmittance and chemical composition of the coatings, respectively. Laser-induce damage threshold (LIDT) was determined by a tripled Nd:YAG laser system with a pulse width of 8 ns. It is found that the crystal structure became more perfect and the refractive index increased gradually with the temperature rising. The LIDT was comparatively high at high temperature. In the other hand, the crystallization status also became better and the refractive index increased when the deposition rate enhanced at a low level. If the rate was super rapid, the crystallization worsened instead and the refractive index would lessen greatly. On the whole, the LIDT decreased with increasing rate.