Showing papers in "Applied Physics A in 1995"

Sub-picosecond UV laser ablation of metals

Abstract: Laser ablation of Nickel, Copper, Molybdenum, Indium, Tungsten and Gold by short ultraviolet laser pulses (0.5 ps, 248 nm) in vacuum is reported for the first time. For Nickel and Indium, ablation is also studied in air to demonstrate the influence of the ambient atmosphere. Metal ablation in air is significantly less efficient than in vacuum due to redeposition of ablated material. The ablation rates in vacuum are discussed using a thermal model, which also allows to estimate ablation rates for other metals from basic optical and thermal properties. A comparison of the morphology of ablation sites after nanosecond and sub-picosecond ablation shows unequivocally the advantages of short-pulse laser ablation for high-precision patterning of thermally good conducting materials in micron-scale dimensions.

Generalized Planck's radiation law for luminescence via indirect transitions

Abstract: Based on microscopic transition probabilities and on the principle of detailed balance, absorption and emission rates are calculated for indirect transitions. It is found that the emission rate at a photon energy ħω can be expressed by the absorption coefficient for the same photon energy in the same way as for direct transitions. This relation is quite generally valid including cases where the electrons in the exited state (conduction band) and the electrons in the ground state (valence band) are distributed according to two different quasi-Fermi distributions. A generalized Planck's law is formulated for luminescence which contains a nonzero chemical potential of the emitted photons as the only difference to the description of thermal radiation.

Hall mobility of undoped n-type conducting strontium titanate single crystals between 19 K and 1373 K

Abstract: The Hall mobility of undoped n-type conducting SrTiO3 single crystals was investigated in a temperature range between 19 and 1373 K. Field calculations were used to estimate the influence of sample shape and electrode geometry on the measured values. Between 19 and 353 K samples, which were quenched under reducing conditions, show an impurity scattering behavior at low temperature and high carrier concentrations and a phonon scattering mechanism at room temperature. In this temperature region, no carrier-density-dependent mobility was found. In conjunction with measurements of the mass difference before and after reoxidation, the oxygen deficiency and the oxygen vacancy concentration could be determined. The oxygen vacancies proved to be singly ionized. Above 873 K, Hall mobility and carrier concentration had been determined as a function of both oxygen partial pressure and temperature for the first time. In this temperature range the mobility does not depend on carrier concentration, but shows aT−1.5 dependence.

Nanosecond and femtosecond excimer-laser ablation of oxide ceramics

Abstract: The uv laser-ablation behavior of various oxide ceramics (Al2O3, MgO, ZrO2) has been studied using different wavelengths (248 nm, 308 nm) and pulse durations (30 ns, 500 fs). Time-resolved absorption measurements of the sample and the ablation plume during ablation were performed. Using sub-ps pulses the ablation threshold fluence is generally lower than for ns pulses; the ablation rate is higher in the whole investigated fluence range up to 20 J/cm2. The study of the morphology of the ablation structures and the results of the absorption experiments lead to the conclusion that different ablation mechanisms are involved. Using ns pulses “plasma mediated ablation” is dominating, whereas in the fs case the process is controlled by multi-photon absorption enabling microstructuring of the material.

Transient thermal gratings at surfaces for thermal characterization of bulk materials and thin films

Abstract: Transient Thermal Gratings (TTGs) at surfaces of absorbing materials have been utilized for investigating heat diffusion in bulk materials and thin films. In this report, we describe the theoretical background of the technique and present experimental data. TTGs were excited in the surface plane by interference of two pulsed laser beams and monitored by a cw probe beam, either via temperature dependence of the reflectivity or by deflection from the displacement pattern. A theoretical model describing the thermal and thermoelastic surface response was developed, both for a homogeneous material and a multilayer structure. The potential of the technique will be demonstrated by experimental results on (i) thermal diffusivities of bulk materials, (ii) anisotropic lateral heat transport, and (iii) thermal diffusivities of metal and diamond films. Furthermore, we will show that TTGs allow thermal depth profiling of inhomogeneous materials whenever there is a vertical gradient in thermal conductivity.

Mechanisms of melt droplets and solid-particle ejection from a target surface by pulsed laser action

Abstract: We suggest an explanation of the effect of melt droplets and solid particle ejection from a target surface under the impact of laser radiation with intensity 108–1010 W/cm2. We consider the capillary wave instabilities on the evaporating surface of melt, which lead to growth of large-scale surface structures and ejection of macroparticles. The instability increments and characteristic droplet sizes are determined. Conditions are found for droplet-free evaporation in terms of the dynamic pressure of evaporated matter.

Controlled lateral manipulation of single molecules with the scanning tunneling microscope

Abstract: We report on the first successful lateral manipulation of molecules and controlled formation of nanostructures with the Scanning Tunneling Microscope (STM) at temperatures above 4 K as used by Eigler and collaborators. Among the first structures, we built the letters F and U forming the logo of our university at 30 K with CO molecules on a Cu(211) substrate. Our method to manipulate the molecules is analogous to that employed successfully up to now only by Eigler and co-workers. First experiences concerning the manipulation of the CO molecules on the highly anisotropic substrate are presented and the crucial role of the tip composition in imaging the CO molecules is demonstrated.

Hydrogen on Si: Ubiquitous surface termination after wet-chemical processing

Abstract: The manufacture of microelectronic devices based on silicon technology is largely dominated by wet chemical processes By ultraclean sample preparation in air and a fast transfer into UltraHigh Vacuum (UHV) we open up a way for the atomic-scale structural and chemical characterization of silicon surfaces immediately after wet-chemical processing Using Scanning Tunneling Microscopy (STM), ThermoDesorption (TDS) and InfraRed Spectroscopy (IRS), we find that a surface termination predominantly by hydrogen results from all the different wet-chemical treatments investigated (etching with hydrofluoric acid, rinsing with hot water, chemomechanical polishing)-despite the different chemical ambients and process parameters involved Microscopically, a crystallographically preferential attack of the silicon is observed in all these processes which results, to a different extent, in anisotropic defect structures on the surfaces This is explained by an interplay of aqueous reaction kinetics and sterical hindrance on the silicon surface It is pointed out how a UHV surface analysis of the micromorphology of wet-chemically treated silicon surfaces, so far carried out mostly on Si(111) due to its easier preparation and experimental accessability, may help to provide the in-depth understanding of the atomic-scale mechanisms during wet-chemical processing demanded by the progressing miniaturization of microelectronic devices The atomically smoother and chemically more homogeneous Si(111) obtained after preferential etching with NH4F suggests that in future applications Si(111) may gain importance over Si(100), which still dominates in today's semiconductor technology, since future devices increasingly rely on tailor-made and “ideal” properties on an atomic scale Due to their structural and chemical simplicity and well-controlable characteristics, H-teminated surfaces after wet-chemical preparation also form ideal substrates for conventional UHV surface studies such as absorption and MBE-growth experiments

Influence of the laser-spot diameter on photo-ablation rates

Abstract: The dependence of the ablation rate of various materials on the laser spot diameter on the sample surface has been investigated. The experiments have been performed with excimer lasers at the wavelengths 193, 248 and 308 nm. Polymers, aluminum oxide ceramics, and glasses have been ablated under vacuum and ambient atmosphere conditions. In general, all materials show a more or less pronounced increase of the ablation rate with decreasing spot diameter in the range of 10–200 μm if pulses with nanosecond pulse durations are applied. For ultrashort pulses (500 fs) at 248 nm this diameter dependence is not observed. The expansion of the ablation plume over areas of different size seems to be the main reason for this effect.

One-dimensional metal structures at decorated steps

Abstract: It is shown how wire structures a few nanometers wide can be fabricated by decorating step edges at vicinal surfaces. Their growth modes and electronic states are studied using Scanning Tunneling Microscopy (STM) and inverse photoemission. The observed growth modes are two-dimensional analogs of Stranski-Krastanov growth and layer-by-layer growth in three dimensions, e.g., for Cu on stepped Mo(1 1 0) and W(1 1 0), respectively. Contrast between different metals is achieved in STM pictures by resonant tunneling via surface states and image states, with the latter providing a map of the work function. The limit of single atomic rows decorating step edges is studied by inverse photoemission, and an energy shift of 0.4 eV is found for electronic states of step atoms. We expect stripe structures to become useful for the study of two- vs one-dimensional magnetism, for magnetoresistive films, and in the design of anisotropic materials.

New concepts for controlled homoepitaxy

Abstract: On the basis of a kinetic growth model we discuss new methods to grow atomically flat homoepitaxial layers in a controlled way. The underlying principle of these methods is to change the growth parameters during growth of an atomic layer in such a way that nucleation on top of a growing layer is suppressed, and thus, layer-by-layer growth is achieved. Experimentally, this can be realized by changing the substrate temperature or deposition rate during monolayer growth in a well-defined way. The same can be achieved at constant temperature and deposition rate by simultaneous ion bombardment during the early stages of growth of a monolayer, or by adding suitable surfactants to the system. Model experiments on Ag(111) and on Cu(111) using thermal energy atom scattering and scanning tunneling microscopy demonstrate the success of these methods.

Anisotropy of sliding friction on the triglycine sulfate (010) surface

Abstract: The frictional properties of freshly cleaved (010) surfaces of the ferroelectric TriGlycine Sulfate (TGS) were investigated by combined scanning and friction force microscopy under ambient conditions. A frictional contrast could be observed between domains with different electrical polarity, as well as between terraces inside individual domains which are separated by steps of half of the unit-cell height or an odd multiple of this value. The latter contrast mechanism originates from the arrangement of the molecules at the surface which is chemically homogeneous, but structurally rotated by 180° between different terraces. The resulting asymmetric surface potential gives rise to a frictional anisotropy in different directions that can be detected by the force microscope, as well as to a change of the frictional force between forward and backward scan direction.

Maximum-entropy data analysis

Abstract: The reconstruction of physical quantities from (computer-) experimental data is very often hampered by the presence of noise, insufficient information and above all by the ill-posed nature of the underlying inversion problem. It will be demonstrated that the maximum entropy concepts is particularly suited for this type of data-analysis problems. It is based on Bayesian statistics and provides a consistent probabilistic theory to obtain unbiased results, independent of any model assumptions. This is particularly desirable if there is no additional information to justify these hypotheses. If, on the other hand, additional prior knowledge is available, it can be effectively incorporated into the computation, leading to more stringent confidence intervals.

Mechanical and elastic properties of amorphous hydrogenated silicon films studied by broadband surface acoustic wave spectroscopy

Abstract: Mechanical and elastic properties of a-Si∶H films were measured by broadband Surface Acoustic Wave Spectroscopy (SAWS). In the frequency range achieved, the SAW dispersion curves extend to 300 MHz, which allowed the density, Young's modulus, and Poisson's ratio to be evaluated for films grown by laser CVD or plasma CVD with different hydrogen concentrations. The films deposited by either method have the best mechanical and elastic properties. at a hydrogen concentration of about 10 at. %. For this material, a density of (2300±20) kg/m3 and Young's modulus of (134±5) GPa was determined. The network structures of amorphous silicon are discussed by applying the constraint-counting model to estimate the mean coordination number.

Note on the interpretation of injection-level-dependent surface recombination velocities

Abstract: The surface recombination velocityS=U/n is defined as the ratio between the surface recombination current densityU and the excess minority carrier concentrationn at the semiconductor surface. Measurements of injection-dependent surface recombination velocities apply modulation techniques, and thus, in reality, a differential surface recombination velocitySdiff=dU/dn is determined. The significance to distinguishS andSdiff when evaluating measurements is shown.

Hydrogen implantation and diffusion in silicon and silicon dioxide

Abstract: Depth profiles of hydrogen implanted into crystalline silicon in random direction at different fluences have been measured by the15N technique and by SIMS. Whereas hydrogen implanted at a fluence of 1015 ions/cm2 shows some limited mobility, no such mobility is observed for higher implantation fluences. In these cases, ballistic computer codes describe the depth distributions well, within the ranges of both experimental and theoretical accuracy. Annealing up to 510 K does not change the hydrogen distributions.

The surface structure of icosahedral Al68Pd23Mn9 measured by STM and LEED

Abstract: For the first time the surface structure of an icosahedral quasicrystal has been successfully investigated in Ultra-High Vacuum (UHV) by Scanning Tunneling Microscopy (STM) and Low-Energy Electron Diffraction (LEED). After cleaning an i-Al68Pd23Mn9 sample in UHV by cycles of ion-sputtering and annealing at temperatures close to the melting point atomically flat terraces are observed by STM. Successive step heights show quasiperiodic order according to the Fibonacci chain. The normals of these terraces are parallel to a five-fold axis as revealed by highly resolved STM images. On the terraces five-fold stars and pentagonal holes are observed. Their orientation is the same on all terraces investigated. Additionally to this long-range orientational order, a high degree of quasiperiodic order is found for the pentagonal holes. This indicates that the quasiperiodic order of this highly ordered and thermodynamically stable quasicrystal extends even up to the surface. Both the step heights and the distances between the pentagonal holes well agree with the values derived from a structural model of this material. Five-fold symmetric LEED patterns can be analysed by means of the Fourier transform of a Fibonacci pentagrid as suggested by the STM data. The analysis yields the same line separations within the pentagrid as deduced from the STM experiments.

LiNbO3 with the damage-resistant impurity indium

Abstract: We report on a detailed investigation (EPR, SHG, optical absorption, luminescence and Raman scattering) on the new damage-resistant impurity indium in LiNbO3, where the increased photoconductivity strongly reduces the photorefractive effect. EPR and optical absorption measurements point to a complete disappearance of the Nb antisite in LiNbO3: In for all In concentrations. We believe that the very effective driving out of Nb antisites by In is due to the trivalent charge state of In and the possibility of charge self-compensation. Similarities in the properties of Mg-, Zn- or Indoped samples are discussed. Simultaneous doping with In and Zn leads to an addition of both contributions, in particular for optical frequency doubling and luminescence. Raman studies prove that In does not improve the stoichiometry of the crystals. Indium doping provides the possibility to control simultaneously phase-matching conditions and to reduce drastically photorefraction. Therefore, In co-doped LiNbO3 compositions are promising materials for applications after solving contemporary growth problems.

Theory for the laser-induced femtosecond phase transition of silicon and GaAS

Abstract: We analyze he femtosecond instability of the chamond lattice of silicon and GaAs, which is induced by a dense electron-hole plasma after excitation by a very imense laser pulse. We obtain that the electron-hole plasma causes an instability of both transverse acoustic and longitudinal optical phonons. So, within less than 200fs, the atoms are displaced more than 1 A from their equilibrium position. The gap between the conduction and the valence band then vanishes and the symmetries of the diamond structure are destroyed, which has important effects on the optical reflectivity and second-harmonic generation. After that, the crystal melts very rapidly because of the high kinetic energy of the atoms. Note that mis is in good agreement with recent experiments done on Shand GaAs using a pump laser to excite a dense electron hole plasma and a probe laser to observe the resulting changes in the atomic and electronic structure.

Two-dimensional micelle formation of polystyrene-poly(vinylpyridine) diblock copolymers on mica surfaces

Abstract: We have used atomic force microscopy to study the adsorption of PolyStyrene-Poly(VinylPyridine) (PS-PVP) block copolymers from a selective solvent onto atomically smooth mica surfaces. At certain copolymer concentrations, we observe a highly regular array of spherical surface micelles covering macroscopic areas of the substrate surface. Evidence is given for a thin homogeneous layer underneath the micelles which is probably due to adsorption of free copolymer chains and brush formation prior to the formation of the micellar structures. We discuss the quality of the self-assembled structures regarding different types of defects and try to identify means for improving the long range periodicity of the structures.

Femtosecond time-resolved reflection second-harmonic generation on polycrystalline copper

Abstract: Optical Second-Harmonic Generation (SHG) in reflection from a polycrystalline copper surface in air was studied using femtosecond time-resolved pump and probe measurements at λ=625 nm. The observed time dependence of second-harmonic yield from the probe beam demonstrates, that SHG is a very sensitive technique for measuring transient electron temperatures of metals even when these are covered by an oxide layer. For polycrystalline copper, an electron-phonon energy transfer time of 2 ps was observed, corresponding to a coupling constant of 3.75×1017 W/m3 K at average lattice temperatures of about 500 K. The analysis of experimental data indicates that the time dependence of SHG is governed by the linear dielectric function e which, in turn, is affected by the electron temperature. There is no evidence for a temperature dependence of the nonlinear susceptibility χ(2).

New azo-dye-doped polymer systems as dynamic holographic recording media

Abstract: Polymer materials show their impact on optical storage technology for developing high information density and fast access-type memories with a high read-out efficiency. New azo-dye-doped polymer materials have been developed and used for recording dynamic holograms. Dynamic holograms with reasonably high diffraction efficiency have been recorded at 468 nm, and the efficiency of the Write, Read and Erase (WRE) cycle in these azo-dye-doped polymer materials was determined. Significant observations in these materials are: (i) there is no need to change the polarization of the writing beam to erase the recorded holograms, (ii) the whole WRE cycle is very fast (3–6 s) and (iii) recording of more than 250 WRE cycles without any fatigue of the recording materials is possible.

Optical second-harmonic generation by supported metal clusters: Size and shape effects

Abstract: Optical Second Harmonic Generation (SHG) by metal clusters has been investigated. For this purpose clusters were generated by the deposition and nucleation of metal atoms on a LiF(100) single crystal surface under ultrahigh vacuum conditions. The size and shape of the metal particles was characterized by optical transmission spectroscopy. The SHG intensity was detected in situ as a function of cluster size during the nucleation. Fundamental wavelengths of λ=1064 and 532 nm were used and the SHG signal was measured for different polarization combinations of the incident and registered light. SH radiation is detectable for particles as small as approximately 1 nm. The signal grows monotonically as a function of particle size, passes a maximum and finally drops off. This behavior is discussed in terms of resonant enhancement of the signal by surface plasmon excitation and changes ofχ (2) as a function of particle size and shape. In further experiments the chemisorption of oxygen on the surface of the metal particles was studied. The SH signal decreases as a function of oxygen coverage and amounts to only about 15% of the initial value upon chemisorption of one monolayer. This indicates that the SH signal originates almost exclusively from the surface of the clean clusters and that higher order bulk contributions are negligible.

Photoinduced refractive-index changes in fulgide-doped PMMA films

Abstract: As an example for a photochromic system we study an active fulgide in a polymer matrix. For theoretical description a two-state model is suggested. Absorption spectroscopy,m-line spectroscopy and UV real-time holography are tools to characterize the optical properties of the guest/host system. The photoinduced refractive-index change is about 7.5×10−4 per % dye concentration. The diffraction efficiency of the holographic grating induced by UV-illumination reaches a high value for photochromic materials of about 7%. The obtained gratings are nonlinear in the case of higher exposure energies.

Dynamics of excimer laser ablation of thin tungsten films monitored by ultrafast photography

Abstract: The time course of laser light induced transport of tungsten films from a glass support is followed by ultrafast photography using delayed dye laser pulses. The photographs provide unambiguous evidence that the material transport in the 40–200 mJ/cm2 intensity domain takes place via removal of solid pieces from the film material. These results are consistent with heat flow calculations which predict the overall melting of the metal layer above 380 mJ/cm2. The series of photographs presented give detailed insight into the melting process and have revealed an unexpected in-flight phase separation of solid fracture pieces and molten droplets throughout the 200–900 mJ/cm2 domain. The faster propagating molten droplets form a condensed halo in front of the solid pieces, thereby providing an efficient shield between the processing laser light and the solid phase.

Permittivity and AC conductivity in yttria-stabilized zirconia

Abstract: Alternating current (ac) conductivity and permittivity measurements were carried out on yttriastabilized cubic zirconia, with yttria varying from 9.6 to 25.5 mol%. In this composition range, the dielectric constant measured at 103 Hz decreased from 29.8 to 23.2 as the yttria concentration increased. A plot of the ac conductivity versus frequency exhibited a plateau conductivity (σdc) and a frequency (ω) dependent term σ'(ω). An analysis of σ'(ω) with a suitable theoretical approach based on a pairs-approximation model, resulted in a calculated binding energy for the yttrium-associated oxygen vacancy of 0.29±0.05 eV, which compares favorably with values obtained by different means in previous studies. The experimental determination of the frequency dependence of the conductivity and its analysis provides an effective basis for understanding the ionic conductivity mechanism.

Positron mobility in polyethylene in the 60–400 K temperature range

Abstract: We have determined the positron mobility (μ+) in polyethylene samples (67.2% crystalline, glass transition temperatureTg=151 K) in the 64–400 K temperature range by Doppler shift measurements. A method based on the simulataneous observation of two γ lines from133Ba and137Cs radioactive sources together with the positron annihilation γ line, was employed to measure the Doppler shift of the 511 keV γ line as a function of the electric field applied to the samples. With this method we were able to measure at the same time the drift velocity of positrons and theS parameter. This parameter is very important in the interpretation of the mobility trend in samples where the positron states change with temperature. The positron mobility was corrected for positronium formation. μ+ at 64 K is 31.7±0.8 cm2 V−1 s−1 then decreases up to 123 K, increases at 148 K and decreases again up to 170 K (μ+=26.9±0.8 cm2 V−s−). This sharp change in mobility is centred around the glass transition temperature of our samples. Then the mobility remains almost constant up to 230 K. From 250 K to 377 K, μ+ increases and reaches the value of 38.4±1.0 cm2 V−1s−1. The corrected experimental data were well fitted by a simple model taking into account scattering and a thermally activated process (hopping mechanism).

Investigation of localized surface plasmons with the photon scanning tunneling microscope

Abstract: A Photon Scanning Tunneling Microscope (PSTM) with probe-sample distance control by electron tunneling is used to probe the localized surface-plasmon fields of individual nanometric silver particles. As samples, conventional island films produced by thermal evaporation and regular particle arrays produced by an electron-beam-lithography-based technique, respectively, are used. In either case the strength and spatial localization of the surface-plasmon fields strongly depend on the excitation wavelength. The results are interpreted as different resonance frequencies of individual particles or of different sample areas. On regular arrays consisting of particles with a smallest diameter of 40 nm, the PSTM maps represent the plasmon field strength spatially resolved for individual particles.

Laser-induced etching of silicon

Abstract: Conventional fabrication method of porous silicon is anodisation of single crystal silicon in hydrofluoric acid. In this report, we show that it is possible to fabricate porous silicon by laser-induced etching. An earlier report by us has demonstrated the dependence of porous silicon photoluminescence characteristic on the etching laser wavelength [1]. Here we used 780 nm line from a diode laser as the etching source, and the optimum etching conditions were obtained. A simple model was proposed to explain the etching process. Scanning Electron Microscope (SEM) images of the samples support the proposed process.

Laser-reactive ablation deposition of silicon-nitride films

Abstract: Silicon-nitride films were deposited on silicon waters by XeCl (308 nm) excimer-laser ablation of silicon in low-pressure (0.05–5 mbar) ammonia atmospheres. Series of 10 000 pulses at the repetition rate of 8 Hz were directed to the target surface. The fluence was set at about 5 J/cm2. Pulse duration was about 30 ns. The deposited films were characterized by different techniques (X-ray diffraction, X-ray photoelectron spectroscopy, Auger electron spectroscopy, Rutherford backscattering spectrometry, scanning electron microscopy, profilometry). Silicon-nitride films with thickness close to 1 μm were obtained under specific experimental conditions.