ALBERT

Notes: Single and multiple Ga0.4In0.6P/(Al0.4Ga0.6)0.5In0.5P quantum wells have been grown using atmospheric pressure organometallic vapor phase epitaxy. The Ga0.4In0.6P well layers are coherently strained to match the lattice parameter of the GaAs substrate. Transmission electron microscopic results showed that the quantum-well layers are very uniform in thickness and the interface is abrupt and free of misfit dislocations. The photoluminescence peak energy increases as the well width decreases, due to carrier confinement in the quantum well. Growth interruptions do not change the photoluminescence peak energy of the quantum well. However, the photoluminescence intensity is drastically reduced for longer growth interruption times. Higher-order x-ray diffraction satellite peaks and a narrow photoluminescence halfwidth are observed in a 20-layer multiple-quantum-well sample, indicative of high structural uniformity and precise control of the composition and thickness during the growth process. Considering the effect of strain on the heterojunction band offsets, the photoluminescence peak energy of the strained quantum well can be described by a simple theory as a function of the well width.

Notes: CuPt type ordering, which consists of a monolayer compositional modulation along one of the 4 〈111〉 directions in the lattice, was studied using transmission electron microscopy for GaAs1−xPx with values of x extending from 0.25 to 0.85. The samples were grown by organometallic vapor phase epitaxy on nominal (001) GaAs substrates that were misoriented by varying amounts in three directions. No CuPt type ordering was observed for GaAs1−xPx with x ≤0.35, while ordering was found to occur for 0.4≤x≤0.85. The direction of substrate misorientation has a major effect on the determination of which of the four possible CuPt variants are formed for 0.4≤x≤0.85. Two variants, with ordering on the (1¯11) and (11¯1) planes, appear for epilayers grown on substrates oriented exactly on the (001) plane and for substrates misoriented by 6° towards the [110] direction. Only one variant, with ordering on the (1¯11) plane, appears for epilayers grown on substrates misoriented by 6° towards [1¯10]. These ordering-induced spots observed in transmission electron diffraction (TED) patterns for GaAsP occur only for the [110] cross section. From TED studies of GaInP grown on similar substrates, we conclude that the CuPt variants in GaAsP are exactly the same as for GaInP. Further evidence supporting this conclusion was obtained by growing first a layer of GaInP followed by a layer of GaAsP. High-resolution dark field electron micrographs show domains of the same variants in both layers. A mechanism describing the formation of the specific ordered variant for both GaAsP and GaInP is proposed. From studies of ordering in a strain-layer superlattice, the strain due to lattice mismatch was found to play no significant role in the propagation of ordered domains. Microtwins, also generated due to lattice mismatch, can act as domain boundaries and prevent the propagation of the ordered domains.

Notes: Tantalum-related thin films containing different amounts of nitrogen are sputter deposited at different argon-to-nitrogen flow rate ratios on (100) silicon substrates. Using x-ray diffractometry, transmission electron microscopy, composition and resistivity analyses, and bending-beam stress measurement technique, this work examines the impact of varying the nitrogen flow rate, particularly on the crystal structure, composition, resistivity, and residual intrinsic stress of the deposited Ta2N thin films. With an adequate amount of controlled, reactive nitrogen in the sputtering gas, thin films of the tantalum nitride of nominal formula Ta2N are predominantly amorphous and can exist over a range of nitrogen concentrations slightly deviated from stoichiometry. The single-layered quasi-amorphous Ta2N (a-Ta2N) thin films yield intrinsic compressive stresses in the range 3–5 GPa. In addition, the use of the 40-nm-thick a-Ta2N thin films with different nitrogen atomic concentrations (33% and 36%) and layering designs as diffusion barriers between silicon and copper are also evaluated. When subjected to high-temperature annealing, the single-layered a-Ta2N barrier layers degrade primarily by an amorphous-to-crystalline transition of the barrier layers. Crystallization of the single-layered stoichiometric a-Ta2N (Ta67N33) diffusion barriers occurs at temperatures as low as 450 °C. Doing so allows copper to preferentially penetrate through the grain boundaries or thermal-induced microcracks of the crystallized barriers and react with silicon, sequentially forming {111}-facetted pyramidal Cu3Si precipitates and TaSi2 Overdoping nitrogen into the amorphous matrix can dramatically increase the crystallization temperature to 600 °C. This temperature increase slows down the inward diffusion of copper and delays the formation of both silicides. The nitrogen overdoped Ta2N (Ta64N36) diffusion barriers can thus be significantly enhanced so as to yield a failure temperature 100 °C greater than that of the Ta67N33 diffusion barriers. Moreover, multilayered films, formed by alternately stacking the Ta67N33 and Ta64N36 layers with an optimized bilayer thickness (λ) of 10 nm, can dramatically reduce the intrinsic compressive stress to only 0.7 GPa and undergo high-temperature annealing without crystallization. Therefore, the Ta67N33/Ta64N36 multilayered films exhibit a much better barrier performance than the highly crystallization-resistant Ta64N36 single-layered films. © 2000 American Institute of Physics.

Notes: AlGaInP epitaxial layers grown at 690 °C by atmospheric pressure organometallic vapor phase epitaxy are investigated by transmission electron microscopy. For the first time, compositionally modulated and ordered structures are simultaneously observed in AlGaInP alloys. The ordering is of the CuPt type with ordering along the {111} directions. The ordered regions appear as plate-like microdomains, while the composition modulation takes the form of a fine columnar constrast oriented along the growth direction. In addition, from the results of (001) plan-view diffraction contrast examination, the principal strain direction associated with the modulation structures is found to be perpendicular to the growth direction and lies in the surface plane. Thus, it is concluded that the spinodal decomposition is initiated and developed on the surface during the growth of the AlGaInP epitaxial layers and, finally, forms the columnar structure.

Notes: Effects of (001) GaAs substrate misorientation on the formation of the group V sublattice {111} (CuPt) ordered structure are studied for the first time for GaAs0.5P0.5. It is found that the direction of substrate misorientation has a strong effect on the determination of which variants are formed. Two of the four possible ordered variants appear for epilayers grown on exact (001) substrates. The same two variants also appear for the epilayers grown on the (001) substrates misoriented by 6° towards [110]. Only one variant appears on epilayers grown on (001) substrates misoriented by 6° towards the [1¯10] direction. Most significantly, all the ordered-induced diffraction spots in GaAsP are found to occur on the [110] cross section. Thus, the variants found in GaAsP are exactly the same as for GaInP, an alloy with CuPt ordering on the group III sublattice. This result is contradictory to expectations based on the bond-length model proposed previously for GaInP alloys. In addition, for all the 6° misorientated GaAs substrates, independent of the direction of misorientation, large ordered domains with dimensions on the order of micrometers are found in the GaAsP alloys. This has not been reported for other ternary or quaternary alloy systems.

Notes: Ga0.5In0.5P is observed to form the CuPt ordered structure during organometallic vapor phase epitaxy (OMVPE). Of the four possible {111} planes on which CuPt ordering could occur, only two are observed for growth on (001)-oriented substrates, giving the (1¯11) and (11¯1) variants. The mechanism by which ordering occurs is not completely understood. Recent total energy calculations indicate that the phenomenon can be explained on the basis of thermodynamic considerations. Indirect evidence indicates that kinetic factors, including processes occurring at steps propagating across the surface in the two-dimensional growth mode, affect ordering. In this letter, Ga0.5In0.5P layers have been grown on (001)GaAs substrates by OMVPE. In order to examine the effects of surface kinetic factors, the substrates were first patterned with [110] oriented grooves 5 μm wide and from 0.2 to 1 μm deep. This yields adjacent areas of epitaxial material within the grooves produced by growth via the motion of steps in opposite directions. Transmission electron diffraction reveals that the two directions of step motion produce two different variants. For exactly (001) oriented substrates, one half of the groove is filled with a single domain of the (1¯11) variant while the other half is also a single domain, but of the (11¯1) variant. For substrates misoriented by 6° to give [110] steps, the domains are asymmetric. The domains are very large, several square microns in cross section extending along the entire length of the groove. The strong intensities of the order-induced spots indicate a high degree of order in the material grown in the grooves. These results demonstrate directly, for the first time, that kinetic factors related to the motion of steps on the surface determine the ordered structure formed. They also demonstrate the possibility of producing very large domains of ordered material.

Notes: GaAs1−xPx with 0.4≤x≤0.85 forms the CuPt ordered structure during organometallic vapor phase epitaxy (OMVPE). Only the (1¯11) and (11¯1) variants are observed for growth on (001)-oriented substrates. The mechanism by which ordering occurs is only now being discovered. Total energy calculations, including the effects of surface reconstruction, indicate that the phenomenon can be explained purely on the basis of energy considerations. Indirect evidence indicates that kinetic factors, including processes occurring at steps propagating across the surface in the two-dimensional growth mode, control ordering. In this work, GaAs1−xPx layers have been grown by OMVPE on (001)-oriented GaAs0.6P0.4"substrates.'' In order to examine the effects of surface kinetic factors, the substrates were first patterned with [110]-oriented grooves 5 μm wide and a fraction of a micron deep. The groove is used to provide a source of steps moving in opposite directions from the two edges. Transmission electron diffraction reveals the formation of large domains of the two variants that meet in the center of the groove. A surprising feature is the presence of a region in the groove with absolutely no ordering. Tracing the surface shape during growth using a superlattice structure indicates that the disordered region is due to growth on {511} facets. The domains formed after the groove is filled are very large, several square microns in cross-sectional area and extending along the entire length of the groove. These results demonstrate that natural ordering in GaAsP, an alloy with mixing on the group V sublattice, can be controlled by regulating the propagation of steps during growth, exactly as for GaInP where mixing is on the group III sublattice.

Notes: InAsP epilayers grown by organometallic vapor phase epitaxy have been investigated using transmission electron microscopy. Electron diffraction studies using 〈110〉 cross sections indicate the formation of CuPt-like ordering on the group V sublattice. Only two of the four possible ordered variants are observed for epilayers grown on the exactly (001) oriented InP substrates. All the order-induced diffraction spots for InAsP are found to occur on the [110] cross section. Thus, the variants found in InAsP are 1/2(1¯11) and 1/2(11¯1), exactly the same as those found in GaInP, an alloy with CuPt ordering on the group III sublattice. This result is in agreement with recent studies on GaAsP and is contradictory to expectations based on the bond-length model proposed previously for GaInP alloys. The direction of substrate misorientation has a strong effect on the formation of ordered structures for normally (001) oriented InP substrates.

Notes: We have discovered that a thin film of SiO2 can be directly reduced to Si under electron beam irradiation. The application of this effect to the fabrication of nanometer-sized Si dots and wires is demonstrated. In particular, if SiO2 is irradiated with a high intensity 100 keV electron beam of nanometer scale, then a column of Si is formed which can be as small as 2 nm in diameter. If the beam is moved in a straight line, then a very thin wire of Si is formed. These columns and wires are formed directly under electron irradiation with a dose of ≥3×109 C m−2 and no resists or chemical development are required.

Notes: Transmission electron microscopy is used to investigate electron-induced crystallization of thermally evaporated amorphous AlF3(a-AlF3). It is shown that this material undergoes a very complicated crystallization process with three crystalline substances (Al, AlF3, and Al2O3) formed as the dose increases. The sequence of the crystallization is highly sensitive to the presence of water, which inhibits radiolytic dissociation of a-AlF3 into Al and fluorine, reduces the dose required for the crystallization of a-AlF3, and causes the transformation of AlF3 into Al2O3. © 1996 American Institute of Physics.