Laser modification of silver nanoclusters in SiO2 thin films

Thin films of silica containing silver nanoclusters have been deposited by magnetron co-sputtering followed by thermal annealing. Laser modification of the mean cluster size was performed using the fourth harmonic of a Nd:YAG laser with energies of between 35 and 125 mJ/cm². The mean size of the clusters was estimated from the shape of the plasmon resonance band in the optical absorption spectra with the help of a computer simulation based on the Mie theory in static approximation. It was found that laser treatment with fluences above a certain threshold leads to a reduction of the mean size of the clusters and this reduction is greater for greater fluences. After a long treatment with the same fluence the effect saturates. The final mean size of the clusters after saturation depends only on the laser fluence and not on the initial mean cluster size. When lower laser fluences were used it was possible after laser annealing to return the mean cluster size to its initial value by thermal annealing. In this way by using a combination of laser treatment and thermal annealing a predetermined mean cluster size could be achieved. The mechanism of laser-induced cluster-size modification is discussed. PACS 81.07.-b; 42.62.-b; 36.40.Qv     

Size dependence of non-linear optical properties of SiO2 thin films containing InP nanocrystals

SiO₂ composite thin films containing InP nanocrystals were fabricated by radio-frequency magnetron co-sputtering technique. The microstructure of the composite thin films was characterized by X-ray diffraction and Raman spectrum. The optical absorption band edges exhibit marked blueshift with respect to bulk InP due to strong quantum confinement effect. Non-linear optical absorption and non-linear optical refraction were studied by a Z-scan technique using a single Gaussian beam of a He-Ne laser (632.8 nm). We observed the saturation absorption and two-photon absorption in the composite films. An enhanced third-order non-linear optical absorption coefficient and non-linear optical refractive index were achieved in the composite films. The nonlinear optical properties of the films display the dependence on InP nanocrystals size. Received: 27 June 2000 / Accepted: 27 June 2000 / Published online: 13 September 2000     

Synthesis of crystalline Ge nanoclusters in PE-CVD-deposited SiO2 films

The synthesis of evenly distributed Ge nanoclusters in plasma-enhanced chemical-vapour-deposited (PE-CVD) SiO₂ thin films containing 8 at. % Ge is reported. This is of importance for the application of nanoclusters in semiconductor technology. The average diameter of the Ge nanoclusters can be controlled in the range of 3–6 nm by variation of the annealing parameters. Using a combination of transmission electron microscopy and Raman-scattering spectroscopy, the nanoclusters were shown to be crystalline. However, photoluminescence measurements showed no light emission that could be definitively correlated to the presence of the nanoclusters. PACS 61.82.Rx; 78.67.Bf; 81.07.Bc     

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     

Photoluminescence studies from silicon nanocrystals embedded in spin on glass thin films

Photoluminescence (PL) from silicon nanocrystals (Si-nc) prepared from pulverised porous silicon and embedded in undoped (SOG) or phosphorus-doped spin-on-glass (SOD) solutions was studied. Effects of rapid thermal annealing on the PL was also investigated. A strong room temperature PL signal was observed at 710 nm due to the recombination of electron-hole pairs in Si-nc and the PL maximum shifts to the blue region as the phosphorus concentration in the spin on glass increases. However, the rapid thermal annealing process (30 s, 900°C) quenches the PL response. These results suggest that for Si-nc/SOG (SOD) the surface termination is efficient but high phosphorus doping of Si-nc is detrimental to the PL.     

Photo-induced charge transport in SiO2films containing Si nanocrystals

Photo-induced charge transport is reported in metal–insulator–semiconductor structures containing Si nanocrystals produced by ion implantion and annealing. Successive shifts in current–voltage (I–V) and capacitance–voltage (C–V) curves are shown to be induced by ultra-violet (UV) light exposure under no bias. These shifts are shown to be enhanced by the application of a negative bias voltage during illumination. The application of a positive bias voltage during illumination is shown to reverse the direction of the shifts in both the I–V and C–V curves. This behaviour can be explained by charging of the nanocrystals induced by photoionization of electrons and charge movements in the insulator layer.     

Growth of Nb thin films on SiO2

Nb thin films have been prepared by electron beam evaporation under ultrahigh vacuum conditions on fused silica substrates at various temperatures, and their structural and morphological evolutions have been investigated using X-ray diffraction and atomic force microscopy. The crystallographic texture of the Nb films is found to depend on the growth temperature. At room temperature, the [1 1 0] texture is dominant. However, at 200°C, the [3 1 0] oriented growth is favored, co-existing with [1 1 0] and [2 0 0] oriented grains. At 400–600°C, a completely [1 1 0] textured film is formed. At even higher temperature (800°C), a complex texture of [1 1 0] (dominant), [2 0 0] and [3 1 0] is observed again. It is also found that the single [1 1 0] textured Nb films have smooth surfaces, and the complex textured Nb films have rough surfaces.     

The mechanism of energy transfer from Si nanocrystals to Er ions in SiO2

The mechanism of energy transfer from silicon nanocrystals (Si-nc’s) to erbium (Er) ions is studied by analyzing time transient of Er photoluminescence at 1.54 μm. It is shown that two different energy transfer mechanisms, i.e., fast and slow, exist in SiO₂ films containing Si-nc’s and Er ions, and that the ratio of slow to fast processes depends on size of Si-nc’s and Er concentration. A quantitative analysis reveals that Er ions located within about 1.5 nm from the surface of Si-nc’s are excited by the fast process, and those located within about 2.5 nm by the slow process if no Er ions exist within 1.5 nm from the surface. Er ions staying outside these regions cannot be sensitized by Si-nc’s.     

Temperature effect on elastic modulus of thin films and nanocrystals

The stability of nanoscale devices is directly related to elasticity and the effect of temperature on the elasticity of thin films and nanocrystals. The elastic instability induced by rising temperature will cause the failure of integrated circuits and other microelectronic devices in service. The temperature effect on the elastic modulus of thin films and nanocrystals is unclear although the temperature dependence of the modulus of bulk materials has been studied for over half a century. In this paper, a theoretical model of the temperature-dependent elastic modulus of thin films and nanocrystals is developed based on the physical definition of the modulus by considering the size effect of the related cohesive energy and the thermal expansion coefficient. Moreover, the temperature effect on the modulus of Cu thin films is simulated by the molecular dynamics method. The results indicate that the elastic modulus decreases with increasing temperature and the rate of the modulus decrease increases with reducing thickness of thin films. The theoretical predictions based on the model are consistent with the results of computational simulations, semi-continuum calculations and the experimental measurements for Cu, Si thin films and Pd nanocrystals.     

The growth of Y2SiO5:Ce thin films with pulsed laser deposition

Y₂SiO₅:Ce phosphor thin films were grown onto Si(100) substrates with pulsed laser deposition (PLD) using a 248-nm KrF excimer laser. Process parameters were varied during the growth process and the effect on the surface morphology and cathodoluminescence (CL) was analysed. The process parameters that were changed included the following: gas pressure (vacuum (5×10⁻⁶ Torr), 1×1⁻² Torr and 1 Torr O₂), different gas species (O₂, Ar and N₂ at a pressure of 455 mTorr), laser fluence (1.6±0.1 J cm⁻² and 3.0±0.3 J cm⁻²) and substrate temperature (400 and 600°C). The surface morphology was investigated with atomic force microscopy (AFM). The morphology of the thin films ablated in vacuum and 10 mTorr ambient O₂ showed more or less the same trend. An increase in the pressure to 1 Torr O₂, however, showed a definite increase in deposited particle sizes. Ablation in N₂ gas resulted in small particles of 20 nm in diameter and ablation in O₂ gas produced bigger particles of 20, 30 and 40 nm as well as an agglomeration of these particles into bigger size clusters of 80 to 100 nm. Ablation in Ar gas led to particle sizes of 30 nm and the particles were much more spherically defined and evenly distributed on the surface. The higher fluence deposition led to bigger particle and grain sizes as well as thicker layers with respect to the lower fluence. The particle sizes of the higher fluence vary mainly between 130 and 140 nm and the lower fluence sizes vary between 50 and 60 nm. The higher fluence particles consist of smaller particles ranging from 5 to 30 nm as measured with AFM. The surface structure of the thin film ablated at 400°C substrate temperature is less compact (lesser agglomeration of particles than at 600°C). The increase in substrate temperature definitely resulted in a rougher surface layer. CL was measured to investigate the effect of the surface morphology on the luminescent intensities. The increased O₂ ambient (1 Torr) resulted in a higher CL intensity compared to the thin films ablated in vacuum. The thin film ablated in Ar gas showed a much higher CL intensity than the other thin films. Ablation at a high fluence resulted in a higher CL intensity. The higher substrate temperature resulted in better CL intensities. The more spherically shaped particles and rougher surface led to increase CL intensities.     

Conduction switching in aluminum nitride thin films containing Al nanocrystals

Conduction switching, i.e., a sharp change in the conduction from a lower-conductance state to a higher-conductance state or vice versa in aluminum nitride thin films embedded with Al nanocrystals (nc–Al) has been observed in the ramped-voltage and ramped-current current–voltage (I–V) measurements and the time-domain current measurement as well. Each state is well defined and its I–V characteristic follows a power law. It is observed that the conductance decreases (or increases) with charging (or discharging) in the nc–Al. It is shown that the conduction switching is due to the charging and discharging in the nc–Al at certain strategic sites. With the connecting (or breaking) of some conductive tunneling paths formed by the uncharged nc–Al due to the discharging (or charging) in the nc–Al at the strategic sites, a conduction switching occurs.     

Electrode effects in electrical measurements in SiO thin films

We report results obtained from thermally stimulated current and capacitance measurements of metal-SiO-metal structures having different metals for the electrodes. Dependence of relaxed charge on the polarized electrode suggests the existence of space charge near the metal-insulator interface. The measurements of capacitance under superimposed DC voltages support this interpretation and show that space charge is not negligible at high fields. The density of lacalised states evaluated from the data is of the order of 10¹⁷ cm^?3     

微晶硅薄膜带隙态及微结构的研究

研究了氢化微晶硅薄膜费米能级以上的带隙态密度分布与薄膜微结构关系.采用拉曼谱和红外谱表征不同H稀释比制备的微晶硅薄膜的微结构.薄膜带隙态密度分布由调制光电流的相移分析技术测得.采用三相模型（非晶相、晶相和界面相）分析了薄膜带隙态密度与薄膜微结构的关系.结果表明,材料的带隙态密度随着界面相的增加而增加,当界面体积分数达到最大时,薄膜的带隙态密度也最大,即材料的带隙态密度与界面体积分数正相关. 关键词： 带隙态 界面相 微晶硅 调制光电流     

Raman analysis of amorphous silicon ruthenium thin films embedded with nanocrystals

We report the Raman analysis of both as‐deposited and annealed amorphous silicon ruthenium thin films embedded with nanocrystals. In the Raman spectra of as‐deposited films, variations of TO peak indicate a short‐range disorder of a‐Si network with an increase of Ru concentration. The substitutional Ru atoms lower the concentration of Si―Si bonds and suppress the intensity of TO peak, but have less effect on TA, LA and LO peaks. In the Raman spectra of annealed films, characteristic parameters confirm the upgrade of a‐Si network at a low annealing temperature and the emergence of both ruthenium silicide and silicon nanocrystals at 700 °C. Although ruthenium silicide nanocrystals present no Raman peaks in the Raman spectra of as‐deposited samples, the non‐linear variations of intensity ratios I_{LA + LO}/I_TO and I_TA/I_TO still suggest their existence, and these nanocrystals are subsequently verified by high‐resolution transmission electron microscopy. Copyright © 2015 John Wiley & Sons, Ltd.     

Hydrogen-release mechanisms in the breakdown of thin SiO2 films

The mechanism of hydrogen release from the anode Si/SiO(2) interface that triggers defect generation and finally the dielectric breakdown of the oxide in metal-oxide-semiconductor structures is investigated. Extensive experimental charge-to-breakdown statistics are used to derive the defect generation efficiency as a function of gate voltage and oxide thickness in wide ranges. The presented results provide strong support to single-electron assisted Si-H bond breakage and discard multiple electron induced incoherent vibrational heating mechanisms.     

Laser sintering of silver nanoparticle thin films: microstructure and optical properties

We present a method for the sintering of silver (Ag) nanoparticle thin films by millisecond pulsed laser irradiation. The microstructure of sintered thin films and sintering behaviors of nanoparticles were systematically investigated in this paper. Absorption spectra of sintered thin films showed blue-shifted surface plasmon resonances (SPR) from 500 nm to 480 nm and red-shifted from 480 nm to 550 nm when laser power was varied from 100 W to 140 W and from 140 W to 200 W, respectively. This indicates a new technique to control light absorption through joining nanoparticles with laser sintering. According to theoretical calculations based on a heat diffusion model, the melting temperature of these Ag nanoparticles was estimated to be 440 °C during laser irradiation.     

Subthreshold photoemission from copper nanoclusters on the SiO2 surface

Subthreshold photoemission from copper nanoclusters formed on the SiO₂ surface has been observed under irradiation of the surface by photons in the 3.1–6.5-eV energy range. The average size of copper nanoclusters on the silicon oxide surface is 250–500 nm. Besides the conventional photoemission from the filled Shockley surface state (SS), strong photoemission has been recorded at incident photon energies of 0.5 eV below the work function of the copper surface. This emission is assumed to be generated in direct electron transitions from the SS state to the unfilled electron surface states formed by the Coulomb image potential, followed by escape from these states into vacuum.