Electroluminescence of silicon nanocrystals in MOS structures

We have studied the structural, electrical and optical properties of MOS devices, where the dielectric layer consists of a substoichiometric SiO_x (x<2) thin film deposited by plasma-enhanced chemical vapor deposition. After deposition the samples were annealed at high temperature (>1000 °C) to induce the separation of the Si and the SiO₂ phases with the formation of Si nanocrystals embedded in the insulating matrix. We observed at room temperature a quite intense electroluminescence (EL) signal with a peak at ∼850 nm. The EL peak position is very similar to that observed in photoluminescence in the very same device, demonstrating that the observed EL is due to electron–hole recombination in the Si nanocrystals and not to defects. The effects of the Si concentration in the SiO_x layer and of the annealing temperature on the electrical and optical properties of these devices are also reported and discussed. In particular, it is shown that by increasing the Si content in the SiO_x layer the operating voltage of the device decreases and the total efficiency of emission increases. These data are reported and their implications discussed. Received: 31 August 2001 / Accepted: 3 September 2001 / Published online: 17 October 2001     

Al2O3/SiO2 films prepared by electron-beam evaporation as UV antireflection coatings on 4H-SiC

Al₂O₃/SiO₂ films have been deposited as UV antireflection coatings on 4H-SiC by electron-beam evaporation and characterized by reflection spectrum, scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The reflectance of the Al₂O₃/SiO₂ films is 0.33% and 10 times lower than that of a thermally grown SiO₂ single layer at 276 nm. The films are amorphous in microstructure and characterize good adhesion to 4H-SiC substrate. XPS results indicate an abrupt interface between evaporated SiO₂ and 4H-SiC substrate free of Si-suboxides. These results make the possibility for 4H-SiC based high performance UV optoelectronic devices with Al₂O₃/SiO₂ films as antireflection coatings.     

Electroluminescence from Multilayered Diamond/CeF3/SiO2 Films

We report a thin film electroluminescent device with a three-layer structure （diamond/CeF3/SiO2 films）, which has a luminance of 1.5 cd/m^2 at dc voltage 215 V. The electroluminescence spectrum at room temperature shows that the main peaks locate at 527 and 593nm, which are attributed to isolated emission centers of Ce^3＋ ions.     

Electroluminescence from a ZnO homojunction device grown by pulsed laser deposition

A ZnO homojunction light emitting device was grown on n+ GaAs substrate by pulsed laser deposition. As-doped ZnO film by diffusion of As from the substrate was used for the p-type side and Al-doped ZnO film for the n-type side of the device. A distinct electroluminescence emission consisting of a dominant emission peak at ∼2.5 eV and a weak shoulder centered at ∼3.0 eV was observed at room temperature. The I-V characteristic of the ZnO homojunction showed a good rectifying behavior with a turn-on voltage of ∼4.5 V and a reverse breakdown voltage of ∼9 V.     

Pulsed Nd:YAG laser depositions of ITO and DLC films for OLED applications

Indium-tin oxide (ITO) films deposited on heated and non-heated glass substrates by a pulsed Nd:YAG laser at 355 nm and ∼2.5 J/cm² were used in the fabrication of simple organic light-emitting diodes (OLEDs), ITO/(PVK + Alq₃ + TPD)/Al. The ITO was deposited on heated glass substrates which possessed resistivity as low as ∼3 × 10⁻⁴ Ω cm, optical transmission as high as ∼92% and carrier concentration of about ∼5 × 10²⁰ cm⁻³, were comparable to the commercial ITO. Substrate heating transformed the ITO microstructure from amorphous to polycrystalline, as revealed by the XRD spectrum. While the polycrystalline ITO produced higher OLED brightness, it was still lower than that on the commercial ITO due to surface roughness. A DLC layer of ∼1.5 nm deposited on this ITO at laser fluence of >12.5 J/cm² improved its device brightness by suppressing the surface roughness effect.     

Voltage-controlled electroluminescence from SiO2 films containing Ge nanocrystals and its mechanism

Luminescent SiO₂ films containing Ge nanocrystals are fabricated by using Ge ion implantation, and metal–oxide–semiconductor structures employing these films as the active layers show yellow electroluminescence (EL) under both forward and reverse biases. The EL spectra are strongly dependent on the applied voltage, but slightly on the mean size of Ge nanocrystals. When the forward bias increases towards 30 V, the EL spectral peak shifts from 590 nm to 485 nm. It is assumed that the EL originates from the recombination of injected electrons and holes in Ge nanocrystals near the Si/SiO₂ interface, or through luminescent centers in the SiO₂ matrix near the SiO₂/metal interface. The mismatch of the injection amounts between holes and electrons results in the low EL efficiency. Received: 28 February 2000 / Accepted: 28 March 2000 / Published online: 5 July 2000     

Photovoltaic and Electroluminescence Bifunctional Devices with Starburst Amine and Rare-Earth-Complexes

We fabricate the organic photovoltaic （PV） devices, in which 4,4＇,4＂-tris-（2-methylphenylphenylamino）triphenylamine （m-MTDATA） and rare earth （RE） （dibenzoylmethanato）a（bathohenanthroline） （RE（DBM）abath） （RE = Nd or Pr） are used as electron donor and acceptor, and investigate their PV properties. The PV diode fabricated in the optimum processing conditions shows the open-circuit voltage of 1.91 V, short-circuit current of 0.1 mA/cm^2, fill factor of 0.38, and the overall power conversion efficiency of 1.9% when it is irradiated under UV light （4 m W/cm^2）. The photocurrent density exhibits an increase of 20% at least when a very thin LiF layer is inserted between the RE-complexes and the A1 cathode. A strong electroluminescence from the interface is also observed and the maximum luminance of a yellow emission resulted from the exciplex is 580 cd/m^2 at 17 V bias.     

Photovoltaic and Electroluminescence Characters in Hybrid ZnO and Conjugated Polymer Bulk Heterojunction Devices

We report electroluminescence in hybrid ZnO and conjugated polymer poly[2-methoxy-5-（3′, 7′-dimethyloctyloxy）- 1,4-phenylenevinylene] （MDMO-PPV） bulk heterojunction photovoltaic cells. Photoluminescence quenching experimental results indicate that the ultrafast photoinduced electron transfer occurs from MDMO-PPV to ZnO under illumination. The ultrafast photoinduced electron transfer effect is induced because ZnO has an electron affinity a bout 1.2 e V greater than that of MDMO-PP V. Electron ＇back transfer＇ can occur if the interfacial barrier between ZnO and MDMO-PPV can be overcome by applying a substantial electric field. Therefore, electrolumi- nescence action due to the fact that the back transfer effect can be observed in the ZnO：MDMO-PPV devices since a forward bias is applied. The photovoltaic and electroluminescence actions in the same ZnO：MDMO-PPV device can be induced by different injection ways： photoinjection and electrical injection. The devices are expected to provide an opportunity for dual functionality devices with photovoltaic effect and electroluminescence character.     

Nitrogen binding behavior in ZnO films with time-resolved cathodoluminescence

ZnO film with (1 0 0) orientation was produced on silicon substrate and doped with nitrogen using plasma immersion ion implantation. The effects due to N doping were investigated using cathodoluminescence (CL). In the heavily nitrogen-doped ZnO film, the intensity of ultraviolet (UV) band decreases and that of the visible band increases as a function of the electron bombardment cycle i.e. time. Based on the X-ray photoelectron spectroscopy (XPS) analysis, the unstable ZnN bond is responsible for the CL behavior and the experimental results agree well with the first-principle calculation. Our work is helpful to our understanding of the role of p-type dopants in ZnO.     

Room temperature photoluminescence from amorphous silicon nanoparticles in SiOx thin films

Amorphous SiO_x thin films with four different oxygen contents (x=1.15, 1.4, 1.5, and 1.7) have been prepared by thermal evaporation of SiO in vacuum and then annealed at 770 or 970 K in argon for various times ?40 min. The influence of annealing conditions and the initial film composition on photoluminescence (PL) from the annealed films has been explored. Intense room temperature PL has been observed from films with x?1.5, visible with a naked eye. It has been shown that PL spectra of most samples consists of two main bands: (i) a ‘green’ band centered at about 2.3 eV, whose position does not change with annealing conditions and (ii) an ‘orange-red’ band whose maximum moves from 2.1 to 1.7 eV with increasing annealing time and temperature and decreasing initial oxygen content. These observations have been explained assuming recombination via defect states in the SiO_x matrix for the first band and emission from amorphous Si nanoparticles for the second one.     

Thermal quenching of electroluminescence assisted by an electric field in thin films of tris-(8-hydroxyquinolinato) aluminum (III)

Temperature dependence of the electroluminescence (EL)-current efficiency of tris-(8-hydroxyquinolinato) aluminum (III) (Alq₃)-based organic light-emitting diodes (OLEDs) operated at a constant current density was investigated. The effects of temperature and electric field on photoluminescence (PL) efficiency of Alq₃ thin layers were also investigated. On the basis of these results, it was found that the EL efficiency decreases more markedly with increasing temperature than does PL efficiency. The temperature dependence of the EL efficiency can be interpreted in terms of the thermal dissociation of excitons that is assisted by the electric field.     

Structural and optical evaluation of WOxNy films deposited by reactive magnetron sputtering

Thin films of tungsten oxynitrides were deposited on substrates preheated at 300 °C from metallic tungsten target using reactive pulsed d.c. magnetron sputtering. The deposition was carried out at different nitrogen to total reactive gas partial pressures ratios. The energy dispersive analysis of X-ray showed that significant incorporation of nitrogen occurred only when the nitrogen partial pressure exceeded 74% of the total reactive gas pressure. X-ray diffraction analysis revealed that the formation of a specific crystalline phase is affected by the composition and the possibility of competitive growth of different phases. The increase of nitrogen content into the films increases the optical absorption and decreases the optical band gap. The refractive index was determined from the transmittance spectra using Swanepoel's method. It was found that the refractive index increases with increasing nitrogen content over the entire spectral range. The values of the tungsten effective coordination number, N_c, was estimated from the analysis of the dispersion of the refractive index, and an increase in N_c with increasing nitrogen content was observed.     

Room temperature photoluminescence mechanism of SiOx film after annealing at different temperatures

SiO_x films were deposited on Si(1 0 0) substrates by evaporation of SiO powder. The samples were annealed from room-temperature (RT) to 1100 °C. After the samples were cooled down to RT, photoluminescence (PL) spectra from these samples were measured. It was found that when the annealing temperature Ta is not higher than 1000 °C, there is a PL centered at 620 nm, and with Ta increasing the intensity increases at first and then decreases when Ta is higher than 500 °C. When Ta is no less than 1000 °C another PL peak located at 720 nm appears. Combined with Raman and XRD spectra, we confirm that the latter PL is from Si nanocrystals that start to form when Ta is higher than 1000 °C. PL spectra for Ta<900 °C were discussed in detail and was attributed to defects in the matrix rather than from Si clusters.     

Structural, electrical and optical properties of ZnS films deposited by close-spaced evaporation

ZnS films have been deposited on glass substrates by close-spaced evaporation (CSE) technique. The films were grown at different temperatures in the range, 200-350 °C. The layers have been characterized with X-ray diffractometer (XRD), atomic force microscope (AFM), energy dispersive analysis of X-rays (EDAX) and optical spectrophotometer to evaluate the quality of the layers for photovoltaic applications. The studies showed that the optimum substrate temperature for the growth of ZnS layers was 300 °C. The films grown at these temperatures exhibited cubic structure with nearly stoichiometric composition. The AFM data revealed that the films had nano-sized grains with a grain size of ∼40 nm. The optical studies exhibited direct allowed transition with an energy band gap of 3.61 eV. The other structural and optical parameters such as lattice stress, dislocation density, refractive index and extinction coefficient were also evaluated. The temperature-dependent conductivity measured in the range, 303-523 K showed a change in the conduction mechanism at 120 °C. The activation energy values evaluated using the temperature dependence of electrical conductivity are 7 and 29 meV at low and high temperature regions, respectively.     

Realization of Ultraviolet Electroluminescence from ZnO Homojunction Fabricated on Silicon Substrate with p-Type ZnO:N Layer Formed by Radical N2O Doping

ZnO homojunction light-emitting diodes are fabricated on Si（100） substrates by plasma assisted metal organic chemical vapour deposition. A p-type layer of nitrogen-doped ZnO film is formed using radical N2O as the acceptor precursor. The n-type ZnO layer is composed of un-doped ZnO film. The device exhibits desirable rectifying behaviour with a turn-on voltage of 3.3 V and a reverse breakdown voltage higher than 6 V. Distinct electrolumineseence emissions centred at 395nm and 490nm are detected from this device at forward current higher than 20mA at room temperature.     

Study on the orientation of silver films by ion-beam assisted deposition

Low energy ion beam assisted deposition (IBAD) was employed to prepare Ag films on Mo/Si (100) substrate. It was found that Ag films deposited by sputtering method without ion beam bombardment were preferred (111) orientation. When the depositing film was simultaneously bombardment by Ar⁺ beam perpendicular to the film surface at ion/atom arrival ratio of 0.18, the prepared films exhibited weak (111) and (200) mixed orientations. When the direction of Ar⁺ beam was off-normal direction of the film surface, Ag films showed highly preferred (111) orientation. Monte Carlo method was used to calculate the sputtering yields of Ar⁺ ions at various incident and azimuth angles. The effects of channeling and surface free energy on the crystallographic orientation of Ag films were discussed.     

Room temperature electroluminescence from ZnO/Si heterojunction devices grown by metal-organic chemical vapor deposition

Heterojunction light-emitting diodes with ZnO/Si structure were fabricated on both high-resistivity (p) and low-resistivity (p⁺) Si substrates by metal-organic chemical vapor deposition technology. Fairly good rectifications were observed from the current-voltage curves of both heterojunctions. Ultraviolet (UV) and blue-white electroluminescence (EL) from ZnO layer were observed only from ZnO/p⁺-Si heterojunction under forward bias at room temperature (RT), while strong infrared (IR) EL emissions from Si substrates were detected from both ZnO/p-Si and ZnO/p⁺-Si heterojunctions. The UV and IR EL mechanisms have been explained by energy band structures. The realization of RT EL in UV-visible and IR region on Si substrate has great applicable potential for Si-based optoelectronic integrated circuits.     

Preparation and characterization of indium tin oxide films formed by oxygen ion beam assisted deposition

Indium tin oxide (ITO) films were produced by low-energy oxygen ion beam assisted electron-beam evaporation. The dependence of surface morphology, electrical and optical properties on evaporation rate, oxygen ion beam energy and density, as well as substrate temperatures was characterized by atomic force microscopy, X-ray photoelectron spectroscopy, Hall-effect and optical transmittance measurements. The results show that high-quality ITO films (resistivity of 7.0×10⁻⁴ Ω cm, optical transmittance above 85% at wavelength 550 nm, surface roughness of 0.6 nm in root mean square) can be obtained at room temperature.     

Electroluminescence of a Multi-Layered Organic Light-Emitting Diode Utilizing Trans-4-[p-[N-methyl-N-(hydroxymethyl)amino]styryl]-N-Methylphridinium Tetraphenylborate as the Active Layer

Employing an organic dye salt of trans-4-[p-[N-methyl-N-(hydroxymethyl)amino]styryl]-N-methylphridinium tetra\-phenylborate (ASPT) as the active layer, 8-hydrocyquinoline aluminium (Alq₃) as the electron transporting layer and N,N’-diphenyl-N,N’-bis(3-methylphenyl)-[1,1’-biphenyl]-4,4’-diamine (TPD) as the hole transporting layer, respectively, we fabricate a multi-layered organic light-emitting diode and observe the colour tunable electroluminescence (EL). The dependence of the EL spectra on the applied voltage is investigated in detail, and the recombination mechanism is discussed by considering the variation of the hole-electron recombination region.     

Fabrication of DLC films by pulsed ion beam ablation in a dense plasma focus device

The pulsed intense ion beam, emitted from a dense plasma focus (DPF) discharges performed with hydrogen gas, has been used to ablate the graphite target depositing diamond-like carbon (DLC) films on Si substrates. The substrates were mounted on a holder, which allowed for deposition at positions between normal and 20° off-normal to the target. The samples were removed for analysis after 10 and 20 shots. Nano-particles were observed in the films by a field-emission scanning electron microscope. Raman spectra indicate that sample deposited at 20° off-normal with 20 shots possesses the highest sp³ content among the samples. The film deposited at this position was also found has the highest hardness.