Jerrold A. Floro

The Dynamic Competition Between Stress Generation and Relaxation Mechanisms During Coalescence of Volmer-Weber Thin Films

Real-time measurements of stress evolution during the deposition of Volmer–Weber thin films reveal a complex interplay between mechanisms for stress generation and stress relaxation. We observed a generic stress evolution from compressive to tensile, then back to compressive stress as the film thickened, in amorphous and polycrystalline Ge and Si, as well as in polycrystalline Ag, Al, and Ti. Direct measurements of stress relaxation during growth interrupts demonstrate that the generic behavior occurs even in the absence of stress relaxation. When relaxation did occur, the mechanism depended sensitively on whether the film was continuous or discontinuous, on the process conditions, and on the film/substrate interfacial strength. For Ag films, interfacial shear dominated the early relaxation behavior, whereas this mechanism was negligible in Al films due to the much stronger bonding at the Al/SiO2 interface. For amorphous Ge, selective relaxation of tensile stress was observed only at elevated temperatures...

Extensions of the Stoney Formula for Substrate Curvature to Configurations with Thin Substrates or Large Deformations

Two main assumptions which underlie the Stoney formula relating substrate curvature to mis-match strain in a bonded thin film are that the film is very thin compared to the substrate, and the deformations are infinitesimally small. Expressions for the curvature-strain relastionship are derived for cases in which thses assumptions are relaxed, thereby providing a biasis for interpretation of experimental observations for a broader class of film-substrate configurations.

Stress evolution during metalorganic chemical vapor deposition of GaN

The evolution of stress in gallium nitride films on sapphire has been measured in real time during metalorganic chemical vapor deposition. In spite of the 16% compressive lattice mismatch of GaN to sapphire, we find that GaN consistently grows in tension at 1050 °C. Furthermore, in situ stress monitoring indicates that there is no measurable relaxation of the tensile growth stress during annealing or thermal cycling.The evolution of stress in gallium nitride films on sapphire has been measured in real time during metalorganic chemical vapor deposition. In spite of the 16% compressive lattice mismatch of GaN to sapphire, we find that GaN consistently grows in tension at 1050 °C. Furthermore, in situ stress monitoring indicates that there is no measurable relaxation of the tensile growth stress during annealing or thermal cycling.

Tensile stress evolution during deposition of Volmer–Weber thin films

A simple model is presented that predicts the kinetics of tensile stress evolution during the deposition of thin films that grow by the Volmer–Weber mechanism. The generation of a tensile stress was attributed to the impingement and coalescence of growing islands, while concurrent stress relaxation was assumed to occur via a microstructure-dependent diffusive mechanism. To model the process of island coalescence, finite element methods were employed and yielded average tensile stresses more consistent with experimental observations than those predicted using previously reported analytical models. A computer simulation was developed that models the process of film growth as the continuous nucleation of isolated islands, which grow at a constant rate to impinge and coalesce to form a continuous polycrystalline film. By incorporating the finite element results for stress generation and a microstructure-dependent stress relaxationmodel, the simulation qualitatively reproduced the complex temperature-dependent trends observed from in situ measurements of stress evolution during the deposition of Ag thin films. The agreement includes simulation of the decreasingstress relaxation rate observed during deposition at increasing temperatures.

Brittle-ductile relaxation kinetics of strained AlGaN/GaN heterostructures

The authors have directly measured the stress evolution during metal organic chemical vapor deposition of AlGaN/GaN heterostructures on sapphire. In situ stress measurements were correlated with ex situ microstructural analysis to directly determine a critical thickness for cracking and the subsequent relaxation kinetics of tensile-strained Al{sub x}Ga{sub 1{minus}x}N on GaN. Cracks appear to initiate the formation of misfit dislocations at the AlGaN/GaN interface, which account for the majority of the strain relaxation.

Epitaxial grain growth in thin metal films

Epitaxial alignment has been obtained by means of grain growth in polycrystalline films deposited on single‐crystal substrates. A theory for epitaxial grain growth is outlined and results given for experiments on Au, Al, Cu, and Ag films on vacuum‐cleaved NaCl, KBr, KCl, or mica. Epitaxial grain growth provides a fundamentally different alternative to conventional epitaxy, and can lead to very thin films with improved continuity and crystalline perfection, as well as non‐lattice‐matched orientations.

Misfit dislocation formation in the AlGaN∕GaN heterointerface

Heteroepitaxial growth of AlxGa1−xN alloy films on GaN results in large tensile strain due to the lattice mismatch. During growth, this strain is partially relieved both by crack formation and by the coupled introduction of dense misfit dislocation arrays. Extensive transmission electron microscopy measurements show that the misfit dislocations enter the film by pyramidal glide of half loops on the 1∕3⟨1123⟩∕{1122} slip system, which is a well-known secondary slip system in hcp metals. Unlike the hcp case, however, where shuffle-type dislocations must be invoked for this slip plane, we show that glide-type dislocations are also possible. Comparisons of measured and theoretical critical thicknesses show that fully strained films can be grown into the metastable regime, which we attribute to limitations on defect nucleation. At advanced stages of relaxation, interfacial multiplication of dislocations dominates the strain relaxation process. This work demonstrates that misfit dislocations are important mec...

In situ measurements of the critical thickness for strain relaxation in AlGaN∕GaN heterostructures

Using in situ wafer-curvature measurements of thin-film stress, we determine the critical thickness for strain relaxation in AlxGa1−xN∕GaN heterostructures with 0.14⩽x⩽1. The surface morphology of selected films is examined by atomic force microscopy. Comparison of these measurements with critical-thickness models for brittle fracture and dislocation glide suggests that the onset of strain relaxation occurs by surface fracture for all compositions. Misfit-dislocations follow initial fracture, with slip-system selection occurring under the influence of composition-dependent changes in surface morphology.

Nonlinear amplitude evolution during spontaneous patterning of ion-bombarded Si(001)

The time evolution of the amplitude of periodic nanoscale ripple patterns formed on Ar+ sputtered Si(OOl ) surfaces was examined using a recently developed in situ spectroscopic technique. At sufficiently long times, we find that the amplitude does not continue to grow exponentially as predicted by the standard Bradley-Harper sputter rippling model. In accounting for this discrepancy, we rule out effects related to the concentration of mobile species, high surface curvature, surface energy anisotropy, and ion-surface interactions. We observe that for all wavelengths the amplitude ceases to grow when the width of the topmost terrace of the ripples is reduced to approximately 25 nm. This observation suggests that a short circuit relaxation mechanism limits amplitude . growth. A strategy for influencing the ultimate ripple amplitude is discussed.

Strain relaxation in AlGaN multilayer structures by inclined dislocations

To examine further the strain relaxation produced by inclined threading dislocations in AlGaN, a heterostructure with three AlGaN layers having successively increasing Ga contents and compressive strains was grown on an AlN template layer by metalorganic vapor-phase epitaxy. The strain state of the layers was determined by x-ray diffraction (XRD) and the dislocation microstructure was characterized with transmission electron microscopy (TEM). As the GaN mole fraction of the heterostructure increased from 0.15 to 0.48, the increased epitaxial strain produced inclined dislocations with successively greater bend angles. Using the observed bend angles, which ranged from 6.7° to 17.8°, the measured strain relaxation within each layer was modeled and found to be accounted for by threading-dislocation densities of 6–7×109/cm2, in reasonable agreement with densities determined by TEM and XRD. In addition to the influence of lattice-mismatch strain on the average bend angle, we found evidence that local strain inh...