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Defect structures created during abnormal grain growth in pulsed-laser deposited nickel

Acta Materialia

Hattar, K.; Follstaedt, David M.; Knapp, J.A.; Robertson, I.M.

The thermal stability of nanograined pulsed-laser deposited nickel was studied by annealing free-standing thin films in situ in a transmission electron microscope. The observed grain growth was sporadic and catastrophic, as expected for abnormal grain growth. The large grains contained a variety of defects that included twins, dislocation lines, small dislocation loops and stacking-fault tetrahedra. This microstructure was developed at annealing temperatures as low as 498 K and was stable at the annealing temperature. The proposed source of the defects and especially the stacking-fault tetrahedra is the grain boundaries, which have excess free volume. This defect source provides insight to the structure of the deposited grain boundaries, which has important consequences for the macroscopic mechanical properties of nanograined pulsed-laser deposited nickel. © 2007 Acta Materialia Inc.

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Strain fields around high-energy ion tracks in α-quartz

Journal of Applied Physics

Follstaedt, David M.; Norman, A.K.; Doyle, B.L.; McDaniel, F.D.

Transmission electron microscopy has been used to image the tracks of high-energy 197Au +26 (374 MeV) and 127I +18 (241 MeV) ions incident in a nonchanneling direction through a prethinned specimen of hexagonal α-quartz (SiO 2). These ions have high electronic stopping powers in quartz, 24 and 19 keV/nm, respectively, which are sufficient to produce a disordered latent track. When the tracks are imaged with diffraction contrast using several different reciprocal lattice vectors, they exhibit a radial strain extending outward from their disordered centerline approximately 16 nm into the crystalline surroundings. The images are consistent with a radial strain field with cylindrical symmetry around the amorphous track, like that found in models developed to account for the lateral expansion of amorphous SiO 2 films produced by irradiation with high-energy ions. These findings provide an experimental basis for increased confidence in such modeling. © 2006 American Institute of Physics.

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Materials physics and device development for improved efficiency of GaN HEMT high power amplifiers

Koleske, Daniel; Shul, Randy J.; Follstaedt, David M.; Provencio, P.N.; Allerman, A.A.; Lee, Stephen R.; Wright, Alan F.; Missert, Nancy; Baca, Albert G.; Briggs, Ronald D.; Marsh, Phil F.; Tigges, Chris P.

GaN-based microwave power amplifiers have been identified as critical components in Sandia's next generation micro-Synthetic-Aperture-Radar (SAR) operating at X-band and Ku-band (10-18 GHz). To miniaturize SAR, GaN-based amplifiers are necessary to replace bulky traveling wave tubes. Specifically, for micro-SAR development, highly reliable GaN high electron mobility transistors (HEMTs), which have delivered a factor of 10 times improvement in power performance compared to GaAs, need to be developed. Despite the great promise of GaN HEMTs, problems associated with nitride materials growth currently limit gain, linearity, power-added-efficiency, reproducibility, and reliability. These material quality issues are primarily due to heteroepitaxial growth of GaN on lattice mismatched substrates. Because SiC provides the best lattice match and thermal conductivity, SiC is currently the substrate of choice for GaN-based microwave amplifiers. Obviously for GaN-based HEMTs to fully realize their tremendous promise, several challenges related to GaN heteroepitaxy on SiC must be solved. For this LDRD, we conducted a concerted effort to resolve materials issues through in-depth research on GaN/AlGaN growth on SiC. Repeatable growth processes were developed which enabled basic studies of these device layers as well as full fabrication of microwave amplifiers. Detailed studies of the GaN and AlGaN growth of SiC were conducted and techniques to measure the structural and electrical properties of the layers were developed. Problems that limit device performance were investigated, including electron traps, dislocations, the quality of semi-insulating GaN, the GaN/AlGaN interface roughness, and surface pinning of the AlGaN gate. Surface charge was reduced by developing silicon nitride passivation. Constant feedback between material properties, physical understanding, and device performance enabled rapid progress which eventually led to the successful fabrication of state of the art HEMT transistors and amplifiers.

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Novel in situ mechanical testers to enable integrated metal surface micro-machines

Hearne, Sean J.; De Boer, Maarten P.; Foiles, Stephen M.; Kotula, Paul G.; Dyck, Christopher; Follstaedt, David M.; Buchheit, Thomas E.

The ability to integrate metal and semiconductor micro-systems to perform highly complex functions, such as RF-MEMS, will depend on developing freestanding metal structures that offer improved conductivity, reflectivity, and mechanical properties. Three issues have prevented the proliferation of these systems: (1) warpage of active components due to through-thickness stress gradients, (2) limited component lifetimes due to fatigue, and (3) low yield strength. To address these issues, we focus on developing and implementing techniques to enable the direct study of the stress and microstructural evolution during electrodeposition and mechanical loading. The study of stress during electrodeposition of metal thin films is being accomplished by integrating a multi-beam optical stress sensor into an electrodeposition chamber. By coupling the in-situ stress information with ex-situ microstructural analysis, a scientific understanding of the sources of stress during electrodeposition will be obtained. These results are providing a foundation upon which to develop a stress-gradient-free thin film directly applicable to the production of freestanding metal structures. The issues of fatigue and yield strength are being addressed by developing novel surface micromachined tensile and bend testers, by interferometry, and by TEM analysis. The MEMS tensile tester has a ''Bosch'' etched hole to allow for direct viewing of the microstructure in a TEM before, during, and after loading. This approach allows for the quantitative measurements of stress-strain relations while imaging dislocation motion, and determination of fracture nucleation in samples with well-known fatigue/strain histories. This technique facilitates the determination of the limits for classical deformation mechanisms and helps to formulate a new understanding of the mechanical response as the grain sizes are refined to a nanometer scale. Together, these studies will result in a science-based infrastructure to enhance the production of integrated metal--semiconductor systems and will directly impact RF MEMS and LIGA technologies at Sandia.

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Relaxation of compressively strained AlGaN by inclined threading dislocations

Proposed for publication in Applied Physics Letters.

Follstaedt, David M.; Provencio, P.N.; Allerman, A.A.; Floro, Jerrold A.; Crawford, Mary H.

Transmission electron microscopy and x-ray diffraction were used to assess the microstructure and strain of Al{sub x}Ga{sub 1?x}N(x = 0.61-0.64) layers grown on AlN. The compressively-strained AlGaN is partially relaxed by inclined threading dislocations, similar to observations on Si-doped AlGaN by P. Cantu, F. Wu, P. Waltereit, S. Keller, A. E. Romanov, U. K. Mishra, S. P. DenBaars, and J. S. Speck [Appl. Phys. Lett. 83, 674 (2003) ]; however, in our material, the dislocations bend before the introduction of any Si. The bending may be initiated by the greater lattice mismatch or the lower dislocation density of our material, but the presence of Si is not necessarily required. The relaxation by inclined dislocations is quantitatively accounted for with the model of A. E. Romanov and J. S. Speck [Appl. Phys. Lett. 83, 2569 (2003)], and we demonstrate the predicted linear dependence of relaxation on layer thickness. Notably, such relaxation was not found in tensile strained AlGaN grown on GaN [J. A. Floro, D. M. Follstaedt, P. Provencio, S. J. Hearne, and S. R. Lee, J. Appl. Phys. 96, 7087 (2004)], even though the same mechanism appears applicable.

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Response to comment on "grain boundary mediated plasticity in nanocrystalline nickel"

Proposed for publication in Science.

Follstaedt, David M.; Knapp, J.A.

Our study (1) reported on the deformation response of nanocrystalline Ni during in situ dark-field transmission electron microscopy (DFTEM) straining experiments and showed what we view as direct and compelling evidence of grain boundary-mediated plasticity. Based on their analysis of the limited experimental data we presented, however, Chen and Yan (2) propose that the reported contrast changes more likely resulted from grain growth caused by electron irradiation and applied stress rather than from plastic deformation. Here, we give specific reasons why their assertions are incorrect and discuss how the measurement approaches they have used are inappropriate. Additionally, we present further evidence that supports our original conclusions. The method Chen and Yan employed to measure displacement merely probes the in-plane (two-dimensional) components of incremental strain occurring during the very short time interval shown [figure 3 in (1)] instead of the accumulated strain. As we noted explicitly in the supporting online material in (1), the loading was applied by pulsing the displacement manually. After each small displacement pulse, the monitored area always moved significantly within or even out of the field of view. Clear images could be obtained only when the sample position stabilized within the field of view, and at that time severe deformation was nearly complete. Thus, little incremental strain occurs during this short image sequence [figure 3 in (1)], as one might expect. We believe that the images shown in figure 3 of (1) are particularly valuable in understanding deformation in nanocrystalline materials. In general, the formation process of grain agglomerates simply occurred too fast to be recorded clearly. Moreover, instead of remaining constant after formation, the sizes of the grain agglomerates changed in a rather irregular manner in responding to the deformation and fracture process (see, for example, Fig. 1, B to D). This indicates that strong grain boundary-related activity occurred inside the grain agglomerates. Figure 3 in (1), a short (0.5 s) extract from more than 6 hours of videotaped experimentation (imaged ahead of cracks), not only reveals the formation process of a grain agglomerate, but also shows conclusive evidence for grain rotation and excludes the effect of overall sample rotation. It should be noted that other small grains still exhibit some minor contrast changes in figure 3 in (1). Hence, using them as reference points yields measurements that may not be accurate to {+-}1 nm [as Chen and Yan (2) claim in their analysis] and limits the accuracy of their conclusions. Chen and Yan also claim that no deformation has occurred, yet simultaneously state that the analysis has a deformation measurement error of 0.5%. This is simply not consistent; even small strains of this order may cause plastic deformation. In contrast with previous in situ TEM experiments (3-5), the special sample design adopted in our investigation (1) ensured that all deformation was primarily concentrated in a bandlike area ahead of the propagating crack. We found that these grain agglomerates were observed only in this bandlike thinning area as a response to the applied loads (Fig. 1B). No similar phenomena were detected under the electron beam alone or in stressed areas apart from the main deformation area, and these phenomena have not been reported during in situ observations of this same material made by other researchers (5). Subsequent cracks were always observed to follow this deformation area upon further displacement pulses (Fig. 1, C and D). This clearly indicates that the enlarged agglomerates do not result simply from electron irradiation plus stress, but rather from stress-induced deformation. In their comment, Chen and Yan claimed a linear relation between 'grain' area and time based on their measurements made from figure 3 in (1) and claimed that these measurements are exactly consistent with the classical grain growth equation. However, as we noted (1), the growth in size of this agglomerate is not isotropic and occurs in an irregular manner. For example, after bright contrast emerged from a grain about 6 nm in diameter, it remained well defined in size as a single, approximately equiaxed grain until t = 0.1 s (fig. S1). We have reproduced the 'grain growth' plot of Chen and Yan (Fig. 2) using our entire video image sequence (fig. S1). Clearly, the growth in area of the agglomerate is not consistent with linear grain growth. (Unfortunately, only a portion of these data could be included in the original paper for reasons of space.) Notably, Chen and Yan did not apply a similar 'grain growth' analysis to nearby grains; this would have yielded no information in support of their argument, as those grains show essentially no growth.

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Effect of threading dislocations on the Bragg peakwidths of GaN, AIGaN, and AIN heterolayers

Proposed for publication in Applied Physics Letters.

Allerman, A.A.; West, Allen W.; Waldrip, Karen E.; Follstaedt, David M.; Provencio, P.N.; Koleske, Daniel

We develop a reciprocal-space model that describes the (hkl) dependence of the broadened Bragg peakwidths produced by x-ray diffraction from a dislocated epilayer. We compare the model to experiments and find that it accurately describes the peakwidths of 16 different Bragg reflections in the [010] zone of both GaN and AlN heterolayers. Using lattice-distortion parameters determined by fitting the model to selected reflections, we estimate threading-dislocation densities for seven different GaN and AlGaN samples and find improved agreement with transmission electron microscopy measurements.

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Final report on LDRD project : outstanding challenges for AlGaInN MOCVD

Creighton, James R.; Koleske, Daniel; Wang, George T.; Coltrin, Michael E.; Allerman, A.A.; Russell, Michael J.; Mitchell, Christine C.; Lee, Stephen R.; Follstaedt, David M.

The AlGaInN material system is used for virtually all advanced solid state lighting and short wavelength optoelectronic devices. Although metal-organic chemical vapor deposition (MOCVD) has proven to be the workhorse deposition technique, several outstanding scientific and technical challenges remain, which hinder progress and keep RD&A costs high. The three most significant MOCVD challenges are: (1) Accurate temperature measurement; (2) Reliable and reproducible p-doping (Mg); and (3) Low dislocation density GaN material. To address challenge (1) we designed and tested (on reactor mockup) a multiwafer, dual wavelength, emissivity-correcting pyrometer (ECP) for AlGaInN MOCVD. This system simultaneously measures the reflectance (at 405 and 550 nm) and emissivity-corrected temperature for each individual wafer, with the platen signal entirely rejected. To address challenge (2) we measured the MgCp{sub 2} + NH{sub 3} adduct condensation phase diagram from 65-115 C, at typical MOCVD concentrations. Results indicate that it requires temperatures of 80-100 C in order to prevent MgCp{sub 2} + NH{sub 3} adduct condensation. Modification and testing of our research reactor will not be complete until FY2005. A new commercial Veeco reactor was installed in early FY2004, and after qualification growth experiments were conducted to improve the GaN quality using a delayed recovery technique, which addresses challenge (3). Using a delayed recovery technique, the dislocation densities determined from x-ray diffraction were reduced from 2 x 10{sup 9} cm{sup -2} to 4 x 10{sup 8} cm{sup -2}. We have also developed a model to simulate reflectance waveforms for GaN growth on sapphire.

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Direct single ion machining of nanopores

Follstaedt, David M.; Norman, Adam K.; Doyle, B.L.

The irradiation of thin insulating films by high-energy ions (374 MeV Au{sup +25} or 241 MeV I{sup +19}) was used to attempt to form nanometer-size pores through the films spontaneously. Such ions deposit a large amount of energy into the target materials ({approx}20 keV/nm), which significantly disrupts their atomic lattice and sputters material from the surfaces, and might produce nanopores for appropriate ion-material combinations. Transmission electron microscopy was used to examine the resulting ion tracks. Tracks were found in the crystalline oxides quartz, sapphire, and mica. Sapphire and mica showed ion tracks that are likely amorphous and exhibit pits 5 nm in diameter on the surface at the ion entrance and exit points. This suggests that nanopores might form in mica if the film thickness is less than {approx}10 nm. Tracks in quartz showed strain in the matrix around them. Tracks were not found in the amorphous thin films examined: 20 nm-SiN{sub x}, deposited SiOx, fused quartz (amorphous SiO{sub 2}), formvar and 3 nm-C. Other promising materials for nanopore formation were identified, including thin Au and SnO{sub 2} layers.

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High-energy ion tracks in thin films

Follstaedt, David M.; Norman, Adam K.; Rossi, Paolo; Doyle, B.L.

High-energy ion tracks (374 MeV Au{sup 26+}) in thin films were examined with transmission electron microscopy to investigate nanopore formation. Tracks in quartz and mica showed diffraction contrast. Tracks in sapphire and mica showed craters formed at the positions of ion incidence and exit, with a lower-density track connecting them. Direct nanopore formation by ions (without chemical etching) would appear to require film thicknesses less than 10 nm.

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Growth and design of deep-UV (240-290nm) light emitting diodes using AlGaN alloys

Proposed for publication in Journal of Crystal Growth.

Allerman, A.A.; Crawford, Mary H.; Fischer, Arthur J.; Bogart, Katherine H.A.; Follstaedt, David M.; Provencio, P.N.; Koleske, Daniel

Solid-state light sources emitting at wavelengths less than 300 nm would enable technological advances in many areas such as fluorescence-based biological agent detection, non-line-of-sight communications, water purification, and industrial processing including ink drying and epoxy curing. In this paper, we present our recent progress in the development of LEDs with emission between 237 and 297 nm. We will discuss growth and design issues of deep-UV LEDs, including transport in Si-doped AlGaN layers. The LEDs are designed for bottom emission so that improved heat sinking and light extraction can be achieved by flip chipping. To date, we have demonstrated 2.25 mW of output power at 295 nm from 1 mm x 1 mm LEDs operated at 500 mA. Shorter wavelength LEDs emitting at 276 nm have achieved an output power of 1.3 mW at 400 mA. The heterostructure designs that we have employed have suppressed deep level emission to intensities that are up to 330 x lower than the primary quantum well emission.

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Grain boundary mediated plasticity in nanocrystalline nickel

Proposed for publication in Science.

Follstaedt, David M.; Knapp, J.A.

The plastic behavior of crystalline materials is mainly controlled by the nucleation and motion of lattice dislocations. We report in situ dynamic transmission electron microscope observations of nanocrystalline nickel films with an average grain size of about 10 nanometers, which show that grain boundary-mediated processes have become a prominent deformation mode. Additionally, trapped lattice dislocations are observed in individual grains following deformation. This change in the deformation mode arises from the grain size-dependent competition between the deformation controlled by nucleation and motion of dislocations and the deformation controlled by diffusion-assisted grain boundary processes.

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Final report on grand challenge LDRD project : a revolution in lighting : building the science and technology base for ultra-efficient solid-state lighting

Simmons, Jerry A.; Fischer, Arthur J.; Crawford, Mary H.; Abrams, B.L.; Biefeld, Robert M.; Koleske, Daniel; Allerman, A.A.; Figiel, Jeffrey J.; Creighton, James R.; Coltrin, Michael E.; Tsao, Jeffrey Y.; Mitchell, Christine C.; Kerley, Thomas M.; Wang, George T.; Bogart, Katherine H.A.; Seager, Carleton H.; Campbell, J.; Follstaedt, David M.; Moran, Michael P.; Norman, Adam K.; Kurtz, S.R.; Wright, Alan F.; Myers, Samuel M.; Missert, Nancy; Copeland, Robert; Provencio, P.N.; Wilcoxon, Jess P.; Hadley, G.R.; Wendt, Joel R.; Kaplar, Robert; Shul, Randy J.; Rohwer, Lauren E.S.; Tallant, David R.; Simpson, Regina L.; Moffat, Harry K.; Salinger, Andrew G.; Pawlowski, Roger; Emerson, John A.; Thoma, Steven T.; Cole, Phillip J.; Boyack, Kevin W.; Elliott, Russell D.; Garcia, Marie L.; Allen, Mark S.; Burdick, Brent; Rahal, Nabeel R.; Monson, Mary A.; Chow, Weng W.; Waldrip, Karen E.; Lee, Stephen R.

This SAND report is the final report on Sandia's Grand Challenge LDRD Project 27328, 'A Revolution in Lighting -- Building the Science and Technology Base for Ultra-Efficient Solid-state Lighting.' This project, which for brevity we refer to as the SSL GCLDRD, is considered one of Sandia's most successful GCLDRDs. As a result, this report reviews not only technical highlights, but also the genesis of the idea for Solid-state Lighting (SSL), the initiation of the SSL GCLDRD, and the goals, scope, success metrics, and evolution of the SSL GCLDRD over the course of its life. One way in which the SSL GCLDRD was different from other GCLDRDs was that it coincided with a larger effort by the SSL community - primarily industrial companies investing in SSL, but also universities, trade organizations, and other Department of Energy (DOE) national laboratories - to support a national initiative in SSL R&D. Sandia was a major player in publicizing the tremendous energy savings potential of SSL, and in helping to develop, unify and support community consensus for such an initiative. Hence, our activities in this area, discussed in Chapter 6, were substantial: white papers; SSL technology workshops and roadmaps; support for the Optoelectronics Industry Development Association (OIDA), DOE and Senator Bingaman's office; extensive public relations and media activities; and a worldwide SSL community website. Many science and technology advances and breakthroughs were also enabled under this GCLDRD, resulting in: 55 publications; 124 presentations; 10 book chapters and reports; 5 U.S. patent applications including 1 already issued; and 14 patent disclosures not yet applied for. Twenty-six invited talks were given, at prestigious venues such as the American Physical Society Meeting, the Materials Research Society Meeting, the AVS International Symposium, and the Electrochemical Society Meeting. This report contains a summary of these science and technology advances and breakthroughs, with Chapters 1-5 devoted to the five technical task areas: 1 Fundamental Materials Physics; 2 111-Nitride Growth Chemistry and Substrate Physics; 3 111-Nitride MOCVD Reactor Design and In-Situ Monitoring; 4 Advanced Light-Emitting Devices; and 5 Phosphors and Encapsulants. Chapter 7 (Appendix A) contains a listing of publications, presentations, and patents. Finally, the SSL GCLDRD resulted in numerous actual and pending follow-on programs for Sandia, including multiple grants from DOE and the Defense Advanced Research Projects Agency (DARPA), and Cooperative Research and Development Agreements (CRADAs) with SSL companies. Many of these follow-on programs arose out of contacts developed through our External Advisory Committee (EAC). In h s and other ways, the EAC played a very important role. Chapter 8 (Appendix B) contains the full (unedited) text of the EAC reviews that were held periodically during the course of the project.

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Plan-view image contrast of dislocations in GaN

Proposed for publication in Applied Physics Letters.

Follstaedt, David M.; Missert, Nancy; Koleske, Daniel; Mitchell, Christine C.; Cross, Karen C.

We demonstrate that when vertical threading dislocations in (0001) GaN are imaged in plan-view by transmission electron microscopy, a surface-relaxation contrast operates in addition to that due to the strain fields of dislocations passing through the specimen. We show that all three dislocation types (edge, screw, and mixed) can be detected in the same image using g = (11{bar 2}0) and 18{sup o} specimen tilt from [0001], allowing total densities to be assessed properly. The type of an individual dislocation can also be readily identified.

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Hall-Petch relationship in pulsed laser deposited nickel films

Proposed for publication in Journal of Materials Research.

Knapp, J.A.; Follstaedt, David M.

Thin-film mechanical properties can be measured using nanoindentation combined with detailed finite element modeling. This technique was used for a study of very fine grained Ni films, formed using pulsed-laser deposition on fused silica, sapphire, and Ni substrates. The grain sizes in the films were characterized by electron microscopy, and the mechanical properties were determined by ultra-low load indentation, analyzed using finite element modeling to separate the mechanical properties of the thin layers from those of the substrates. Some Ni films were deposited at high temperature or annealed after deposition to enlarge the grain sizes. The observed hardnesses and grain sizes in these thin Ni films are consistent with the empirical Hall-Petch relationship for grain sizes ranging from a few micrometers to as small as 10 nm, suggesting that deformation occurs preferentially by dislocation movement even in such nanometer-size grains.

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Surface Hardening by Nanoparticle Precipitation in Ni(Al,O)

Myers, Samuel M.; Follstaedt, David M.; Knapp, J.A.

Ion implantation of O and Al were used to form nanometer-size precipitates of NiO or Al{sub 2}O{sub 3} in the near-surface of Ni. The yield strengths of the treated layers were determined by nanoindentation testing in conjunction with finite-element modeling. The strengths range up to {approximately}5 GPa, substantially above values for hard bearing steels. These results agree quantitatively with predictions of dispersion-hardening theory based on the precipitate microstructures observed by transmission electron microscopy. Such surface hardening by ion implantation may be beneficial for Ni components in micro-electromechanical systems.

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AlGaN Materials Engineering for Integrated Multi-Function Systems

Lee, Stephen R.; Casalnuovo, Stephen A.; Mani, Seethambal; Mitchell, Christine C.; Waldrip, Karen E.; Guilinger, Terry R.; Kelly, Michael J.; Fleming, J.G.; Santa Tsao, Sylviaines; Follstaedt, David M.; Wampler, William R.

This LDRD is aimed to place Sandia at the forefront of GaN-based technologies. Two important themes of this LDRD are: (1) The demonstration of novel GaN-based devices which have not yet been much explored and yet are coherent with Sandia's and DOE's mission objectives. UV optoelectronic and piezoelectric devices are just two examples. (2) To demonstrate front-end monolithic integration of GaN with Si-based microelectronics. Key issues pertinent to the successful completion of this LDRD have been identified to be (1) The growth and defect control of AlGaN and GaN, and (2) strain relief during/after the heteroepitaxy of GaN on Si and the separation/transfer of GaN layers to different wafer templates.

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Hall-Petch hardening in pulsed laser deposited nickel and copper thin films

Materials Research Society Symposium - Proceedings

Knapp, J.A.; Follstaedt, David M.; Banks, James C.; Myers, Samuel M.

Very fine-grained Ni and Cu films were formed using pulsed laser deposition onto fused silica substrates. The grain sizes in the films were characterized by electron microscopy, and the mechanical properties were determined by ultra-low load indentation, with finite-element modeling used to evaluate the properties of the layers separately from those of the substrate. Some Ni films were also examined after annealing to 350 and 450 °C to enlarge the grain sizes. These preliminary results show that the observed hardnesses are consistent with a simple extension of the Hall-Petch relationship to grain sizes as small as 11 nm for Ni and 32 nm for Cu.

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Low-Dislocation-Density GaN from a Single Growth on a Textured Substrate

Applied Physics Letters

Ashby, Carol I.H.; Mitchell, Christine C.; Han, J.; Missert, Nancy; Provencio, P.N.; Follstaedt, David M.; Peake, Gregory M.; Griego, Leonardo

The density of threading dislocations (TD) in GaN grown directly on flat sapphire substrates is typically greater than 10{sup 9}/cm{sup 2}. Such high dislocation densities degrade both the electronic and photonic properties of the material. The density of dislocations can be decreased by orders of magnitude using cantilever epitaxy (CE), which employs prepatterned sapphire substrates to provide reduced-dimension mesa regions for nucleation and etched trenches between them for suspended lateral growth of GaN or AlGaN. The substrate is prepatterned with narrow lines and etched to a depth that permits coalescence of laterally growing III-N nucleated on the mesa surfaces before vertical growth fills the etched trench. Low dislocation densities typical of epitaxial lateral overgrowth (ELO) are obtained in the cantilever regions and the TD density is also reduced up to 1 micrometer from the edge of the support regions.

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Optical properties of spontaneous lateral composition modulations in AlAs/InAs short-period superlattices

Applied Physics Letters

Jones, Eric D.; Reno, John L.; Lee, Stephen R.; Follstaedt, David M.

The effect of lateral composition modulation, spontaneously generated during the epitaxial growth of a AlAs/InAs short-period superlattice, on the electronic band structure is investigated using photo-transmission and photoluminescence spectroscopy. Compared with uniform layers of similar average composition, the presence of the composition modulation considerably reduces the band gap energy and produces strongly polarized emission and absorption spectra. The authors demonstrate that the dominant polarization can selectively be aligned along the [{bar 1}10] or [010] crystallographic directions. In compressively strained samples, the use of (001) InP substrates slightly miscut toward [111]A or [101] resulted in modulation directions along [110] or [100], respectively, and dominant polarizations along a direction orthogonal to the respective composition modulation. Band gap reduction as high as 350 meV and 310 meV are obtained for samples with composition modulation along [110] and [100], respectively. Polarization ratios up to 26 are observed in transmission spectra.

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Effect of surface steps on the microstructure of lateral composition modulation

Applied Physics Letters

Follstaedt, David M.; Reno, John L.; Jones, Eric D.; Lee, Stephen R.

Growth of InAs/AlAs short-period superlattices on appropriately miscut (001) InP substrates is shown to alter the microstructure of composition modulation from a 2D organization of short compositionally enriched wires to a single dominant modulation direction and wire lengths up to {approximately}1 {micro}m. The effects of miscut are interpreted in terms of surface step orientation and character. The material is strongly modulated and exhibits intense optical emission. The 1D modulations appear potentially useful for new devices that take advantage of the preferred direction formed in the growth plane.

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Compliant substrate technology for dissimilar epitaxy

Floro, Jerrold A.; Lee, Stephen R.; Follstaedt, David M.; Klem, John F.

Strained-layer semiconductor films offer tremendous potential with regards to optoelectronic applications for high speed communications, mobile communications, sensing, and novel logic devices. It is an unfortunate reality that many of the possible film/substrate combinations that could be exploited technologically are off limits because of large differences in lattice parameters, chemical compatibilities, or thermal expansion rates. These mechanical, chemical, and thermal incompatibilities manifest themselves primarily in terms of lattice defects such as dislocations and antiphase boundaries, and in some cases through enhanced surface roughness. An additional limitation, from a production point of view, is money. Device manufacturers as a rule want the cheapest substrate possible. Freeing the heteroepitaxial world of the bonds of (near) lattice matching would vastly expand the types of working devices that could be grown. As a result, a great deal of effort has been expended finding schemes to integrate dissimilar film/substrate materials while preserving the perfection of the film layer. One such scheme receiving significant attention lately is the so-called compliant substrate approach.

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The nature and origin of lateral composition modulations in short-period strained-layer superlattices

Jones, Eric D.; Follstaedt, David M.; Lee, Stephen R.; Reno, John L.

The nature and origin of lateral composition modulations in (AlAs){sub m}(InAs){sub n} SPSs grown by MBE on InP substrates have been investigated by XRD, AFM, and TEM. Strong modulations were observed for growth temperatures between {approx} 540 and 560 C. The maximum strength of modulations was found for SPS samples with InAs mole fraction x (=n/(n+m)) close to {approx} 0.50 and when n {approx} m {approx} 2. The modulations were suppressed at both high and low values of x. For x >0.52 (global compression) the modulations were along the <100> directions in the (001) growth plane. For x < 0.52 (global tension) the modulations were along the two <310> directions rotated {approx} {+-} 27{degree} from [110] in the growth plane. The remarkably constant wavelength of the modulations, between {approx} 20--30 nm, and the different modulation directions observed, suggest that the origin of the modulations is due to surface roughening associated with the high misfit between the individual SPS layers and the InP substrate. Highly uniform unidirectional modulations have been grown, by control of the InAs mole fraction and growth on suitably offcut substrates, which show great promise for application in device structures.

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Reciprocal-space and real-space analyses of compositional modulation in InAs/AlAs short-period superlattices

Follstaedt, David M.; Lee, Stephen R.; Reno, John L.; Jones, Eric D.

The microstructure of lateral composition modulation in InAs/AlAs superlattices grown by MBE on InP is examined. The use of x-ray diffraction, TEM, AFM, and STEM to characterize the modulations is discussed. Combining the information from these techniques gives increased insight into the phenomenon and how to manipulate it. Diffraction measures the intensity of modulation and its wavelength, and is used to identify growth conditions giving strong modulation. The TEM and STEM analyses indicate that local compositions are modulated by as much as 0.38 InAs mole fraction. Plan-view images show that modulated structures consists of short ({approx_lt}0.2 {micro}m) In-rich wires with a 2D organization in a (001) growth plane. However, growth on miscut substrates can produce a single modulation along the miscut direction with much longer wires ({approx_gt}0.4 {micro}m), as desired for potential applications. Photoluminescence studies demonstrate that the modulation has large effects on the bandgap energy of the superlattice.

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Role of defects in III-nitride based electronics

Han, J.; Myers, Samuel M.; Follstaedt, David M.; Wright, Alan F.; Crawford, Mary H.; Lee, Stephen R.; Seager, Carleton H.; Shul, Randy J.; Baca, Albert G.

The LDRD entitled ``Role of Defects in III-Nitride Based Devices'' is aimed to place Sandia National Laboratory at the forefront of the field of GaN materials and devices by establishing a scientific foundation in areas such as material growth, defect characterization/modeling, and processing (metalization and etching) chemistry. In this SAND report the authors summarize their studies such as (1) the MOCVD growth and doping of GaN and AlGaN, (2) the characterization and modeling of hydrogen in GaN, including its bonding, diffusion, and activation behaviors, (3) the calculation of energetic of various defects including planar stacking faults, threading dislocations, and point defects in GaN, and (4) dry etching (plasma etching) of GaN (n- and p-types) and AlGaN. The result of the first AlGaN/GaN heterojunction bipolar transistor is also presented.

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Brittle-Ductile Relaxation Kinetics of Strained AlGaN/GaN

Applied Physics Letters

Hearne, Sean J.; Han, J.; Lee, Stephen R.; Floro, Jerrold A.; Follstaedt, David M.

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.

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Characterizing Composition Modulations in InAs/AIAs Short-Period Superlattices

Physical Review B

Follstaedt, David M.

The formation of quantum wires has much interest due to their novel electronic properties which may lead to enhanced optoelectronic device performance and greater photovoltaic efficiencies. One method of forming these structures is through spontaneous lateral modulation found during the epitaxial growth of III/V alloys. In this paper, we report and summarize our investigations on the formation of lateral moduation in the MBE grown InAlAs/InP(001) system. This system was grown as a short-period superlattice where n-monolayers of InAs are deposited followed by m-Monolayers of AlAs (with n and m~2) and this sequence is repeated to grown a low strain InAlAs ternary alloy on InP(001) that exhibits lateral modulation. Films were grown under a variety of condition (growth temperature, effective alloy composition, superlattice period, and growth rate). These films have been extensively analyzed using X-ray diffraction, atomic force microscopy, and transmission electron microscopy (TEM) and microcharacterization, in addition to photon-based spectroscopes. Here we present results of several microstructural characterizations using a wide range of TEM-based techniques, and compare them to results from the other methods to obtain a unified understanding of composition modulation. Two strong points consistently emerge: 1) The lateral modulation wavelength is insensitive to growth temperature and effective alloy composition, but the strength of the lateral modulation is greatest near an effective alloy composition of In(0.46)Al(0.54)As, which corresponds to a slightly tensile global strain with respect to InP. 2) The composition variation for the strongly modulated films is as much as 0.38 InAs mole fraction. In addition, for these strongly modulated films, the modulation wave is asymmetric showing strongly peaked, narrower InAs-rich regions separated by flat AlAs-rich regions. We discuss these results and their possible implications in addition to detailing the techniques used to obtain them.

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Microstructures of cubic Al sub 2 O sub 3 precipitates in oxygen-implanted aluminum

Follstaedt, David M.

The microstructure of Al ion-implanted at room temperature with 17 at. % 0 has been characterized with TEM. The alloy has extremely small (1.5--3.5 nm) oxide precipitates whose crystal structure is interpreted to be a disordered version of {gamma}-Al{sub 2}O{sub 3} having a fcc lattice of O{sup 2{minus}} ions with Al{sup 3+} ions in random interstitial sites. The small sizes can account for the exceptionally high strength of as-implanted alloys: 2500--3300 MPa. Larger precipitates are found when the alloy is annealed 1/2 hour at 550{degree}C, which is consistent with its somewhat lower strength: 800--1600 MPa. 4 figs.

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