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Record quantum efficiency from strain compensated superlattice GaAs/GaAsP photocathode for spin polarized electron source

AIP Advances

Biswas, Jyoti; Cultrera, Luca; Liu, Wei; Wang, Erdong; Skaritka, John; Kisslinger, Kim; Hawkins, Samuel D.; Lee, Stephen R.; Klem, John F.

Photocathodes based on GaAs and other III-V semiconductors are capable of producing highly spin-polarized electron beams. GaAs/GaAsP superlattice photocathodes exhibit high spin polarization; however, the quantum efficiency (QE) is limited to 1% or less. To increase the QE, we fabricated a GaAs/GaAsP superlattice photocathode with a Distributed Bragg Reflector (DBR) underneath. This configuration creates a Fabry-Pérot cavity between the DBR and GaAs surface, which enhances the absorption of incident light and, consequently, the QE. These photocathode structures were grown using molecular beam epitaxy and achieved record quantum efficiencies exceeding 15% and electron spin polarization of about 75% when illuminated with near-bandgap photon energies.

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Heteroepitaxy of Dirac semimetal Cd3As2 by metal-organic chemical-vapor deposition

Journal of Crystal Growth

Wheeler-Tait, Christopher; Lee, Stephen R.; Deitz, Julia D.; Rodriguez, Mark A.; Alliman, Darrell L.; Gunning, Brendan P.; Peake, Gregory M.; Sandoval, Annette S.; Valdez, Nichole R.; Sharps, Paul

We present progress on the synthesis of semimetal Cd3As2 by metal–organic chemical-vapor deposition (MOCVD). Specifically, we have optimized the growth conditions needed to obtain technologically useful growth rates and acceptable thin-film microstructures, with our studies evaluating the effects of varying the temperature, pressure, and carrier-gas type for MOCVD of Cd3As2 when performed using dimethylcadmium and tertiary-butylarsine precursors. In the course of the optimization studies, exploratory Cd3As2 growths are attempted on GaSb substrates, strain-relaxed InAs buffer layers grown on GaSb substrates, and InAs substrates. Notably, only the InAs-terminated substrate surfaces yield desirable results. Extensive microstructural studies of Cd3As2 thin films on InAs are performed by using multiple advanced imaging microscopies and x-ray diffraction modalities. The studied films are 5–75 nm in thickness and consist of oriented, coalesced polycrystals with lateral domain widths of 30–80 nm. The most optimized films are smooth and specular, exhibiting a surface roughness as low as 1.0 nm rms. Under cross-sectional imaging, the Cd3As2-InAs heterointerface appears smooth and abrupt at a lower film thickness, ~30 nm, but becomes quite irregular as the average thickness increases to ~55 nm. The films are strain-relaxed with a residual biaxial tensile strain (ϵxx = +0.0010) that opposes the initially compressive lattice-mismatch strain of Cd3As2 coherent on InAs (ϵxx = - 0.042). Importantly, phase-identification studies find a thin-film crystal structure consistent with the P42/nbc space group, placing MOCVD-grown Cd3As2 among the Dirac semimetals of substantial interest for topological quantum materials studies.

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Zero-bias conductance peak in Dirac semimetal-superconductor devices

Physical Review Research

W Yu, Rafael H.; Rodriguez, Mark A.; Lee, Stephen R.; Zhang, F.; Franz, M.; Pikulin, D.I.; Pan, Wei P.

Majorana zero modes (MZMs), fundamental building blocks for realizing topological quantum computers, can appear at the interface between a superconductor and a topological material. One of the experimental signatures that has been widely pursued to confirm the existence of MZMs is the observation of a large, quantized zero-bias conductance peak (ZBCP) in the differential conductance measurements. In this Letter, we report observation of such a large ZBCP in junction structures of normal metal (titanium/gold Ti/Au)-Dirac semimetal (cadmium-arsenide Cd3As2)-conventional superconductor (aluminum Al), with a value close to four times that of the normal state conductance. Our detailed analyses suggest that this large ZBCP is most likely not caused by MZMs. We attribute the ZBCP, instead, to the existence of a supercurrent between two far-separated superconducting Al electrodes, which shows up as a zero-bias peak because of the circuitry and thermal fluctuations of the supercurrent phase, a mechanism conceived by Ivanchenko and Zil'berman more than 50 years ago [Ivanchenko and Zil'berman, JETP 28, 1272 (1969)]. Our results thus call for extreme caution when assigning the origin of a large ZBCP to MZMs in a multiterminal semiconductor or topological insulator/semimetal setup. We thus provide criteria for identifying when the ZBCP is definitely not caused by an MZM. Furthermore, we present several remarkable experimental results of a supercurrent effect occurring over unusually long distances and clean perfect Andreev reflection features.

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Topological Quantum Materials for Quantum Computation

Nenoff, T.M.; Chou, Stanley S.; Dickens, Peter D.; Modine, N.A.; Yu, Wenlong; Lee, Stephen R.; Sapkota, Keshab R.; Wang, George T.; Wendt, J.R.; Medlin, Douglas L.; Leonard, Francois L.; Pan, Wei P.

Recent years have seen an explosion in research efforts discovering and understanding novel electronic and optical properties of topological quantum materials (TQMs). In this LDRD, a synergistic effort of materials growth, characterization, electrical-magneto-optical measurements, combined with density functional theory and modeling has been established to address the unique properties of TQMs. Particularly, we have carried out extensive studies in search for Majorana fermions (MFs) in TQMs for topological quantum computation. Moreover, we have focused on three important science questions. 1) How can we controllably tune the properties of TQMs to make them suitable for quantum information applications? 2) What materials parameters are most important for successfully observing MFs in TQMs? 3) Can the physical properties of TQMs be tailored by topological band engineering? Results obtained in this LDRD not only deepen our current knowledge in fundamental quantum physics but also hold great promise for advanced electronic/photonic applications in information technologies.

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Topological Quantum Materials for Realizing Majorana Quasiparticles

Chemistry of Materials

Nenoff, T.M.; Pan, Wei P.; Sharma, Peter A.; Lima-Sharma, Ana L.; Lee, Stephen R.

In the past decade, basic physics, chemistry, and materials science research on topological quantum materials - and their potential use to implement reliable quantum computers - has rapidly expanded to become a major endeavor. A pivotal goal of this research has been to realize materials hosting Majorana quasiparticles, thereby making topological quantum computing a technological reality. While this goal remains elusive, recent data-mining studies, performed using topological quantum chemistry methodologies, have identified thousands of potential topological materials - some, and perhaps many, with potential for hosting Majoranas. We write this Review for advanced materials researchers who are interested in joining this expanding search, but who are not currently specialists in topology. The first half of the Review addresses, in readily understood terms, three main areas associated with topological sciences: (1) a description of topological quantum materials and how they enable quantum computing; (2) an explanation of Majorana quasiparticles, the important topologically endowed properties, and how it arises quantum mechanically; and (3) a description of the basic classes of topological materials where Majoranas might be found. The second half of the Review details selected materials systems where intense research efforts are underway to demonstrate nontrivial topological phenomena in the search for Majoranas. Specific materials reviewed include the groups II-V semiconductors (Cd3As2), the layered chalcogenides (MX2, ZrTe5), and the rare-earth pyrochlore iridates (A2Ir2O7, A = Eu, Pr). In each case, we describe crystallographic structures, bulk phase diagrams, materials synthesis methods (bulk, thin film, and/or nanowire forms), methods used to characterize topological phenomena, and potential evidence for the existence of Majorana quasiparticles.

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Electrical-current-induced magnetic hysteresis in self-assembled vertically aligned La2/3Sr1/3MnO3:ZnO nanopillar composites

Physical Review Materials

Pan, Wei P.; Lu, Ping L.; Ihlefeld, J.F.; Lee, Stephen R.; Choi, E.S.; Jiang, Y.; Jia, Q.X.

Magnetoresistive random-access memory (MRAM) is poised to become a next-generation information storage device. Yet, many materials challenges remain unsolved before it can become a widely used memory storage solution. Among them, an urgent need is to identify a material system that is suitable for downscaling and is compatible with low-power logic applications. Self-assembled, vertically aligned La2/3Sr1/3MnO3: ZnO nanocomposites, in which La2/3Sr1/3MnO3 (LSMO) matrix and ZnO nanopillars form an intertwined structure with coincident-site-matched growth occurring between the LSMO and ZnO vertical interfaces, may offer new MRAM applications by combining their superior electric, magnetic ( B ), and optical properties. Here, in this Rapid Communication, we show the results of electrical current induced magnetic hysteresis in magnetoresistance measurements in these nanopillar composites. We observe that when the current level is low, for example, 1 µA, the magnetoresistance displays a linear, negative, nonhysteretic B field dependence. Surprisingly, when a large current is used, I > 10 µA, a hysteretic behavior is observed when the B field is swept in the up and down directions. This hysteresis weakens as the sample temperature is increased. Finally, a possible spin-valve mechanism related to this electrical current induced magnetic hysteresis is proposed and discussed.

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Molecular dynamics studies of InGaN growth on nonpolar (112¯0) GaN surfaces

Physical Review Materials

Zhou, Xiaowang Z.; Jones, Reese E.; Gruber, J.; Tucker, G.J.; Chu, K.; Lee, Stephen R.

In this study, we have performed direct molecular dynamics (MD) simulations of heteroepitaxial vapor deposition of InxGa1-xN films on nonpolar (112¯0) wurtzite-GaN surfaces to investigate strain relaxation by misfit-dislocation formation. The simulated growth is conducted on an atypically large scale by sequentially injecting nearly a million individual vapor-phase atoms towards a fixed GaN substrate. We apply time-and-position-dependent boundary constraints to affect the appropriate environments for the vapor phase, the near-surface solid phase, and the bulklike regions of the growing layer. The simulations employ a newly optimized Stillinger-Weber In-Ga-N system interatomic potential wherein multiple binary and ternary structures are included in the underlying density-functional theory and experimental training sets to improve the treatment of the In-Ga-N related interactions. To examine the effect of growth conditions, we study a matrix of 63 different MD-growth simulations spanning seven InxGa1-xN-alloy compositions ranging from x = 0.0 to x = 0.8 and nine growth temperatures above half the simulated melt temperature. We found a composition dependent temperature range where all kinetically trapped defects were eliminated, leaving only quasiequilibrium misfit and threading dislocations present in the simulated films. Based on the MD results obtained in this temperature range, we observe the formation of interfacial misfit and threading dislocation arrays with morphologies strikingly close to those seen in experiments. In addition, we compare the MD-observed thickness-dependent onset of misfit-dislocation formation to continuum-elasticity-theory models of the critical thickness and find reasonably good agreement. Lastly, we use the three-dimensional atomistic details uniquely available in the MD-growth histories to directly observe the nucleation of dislocations at surface pits in the evolving free surface.

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Emergent Phenomena in Oxide Nanostructures

Pan, Wei P.; Ihlefed, Jon F.; Lu, Ping L.; Lee, Stephen R.

The field of oxide electronics has seen tremendous growth over two decades and oxide materials find wide-ranging applications in information storage, fuel cells, batteries, and more. Phase transitions, such as magnetic and metal-to-insulator transitions, are one of the most important phenomena in oxide nanostructures. Many novel devices utilizing these phase transitions have been proposed, ranging from ultrafast switches for logic applications to low power memory structures. Yet, despite this promise and many years of research, a complete understanding of phase transitions in oxide nanostructures remains elusive. In this LDRD, we report two important observations of phase transitions. We conducted a systematic study of these transitions. Moreover, emergent quantum phenomena due to the strong correlations and interactions among the charge, orbital, and spin degrees of freedom inherent in transition metal oxides were explored. In addition, a new, fast atomic-scale chemical imaging technique developed through the characterization of these oxides is presented.

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Compact Models for Defect Diffusivity in Semiconductor Alloys

Wright, Alan F.; Modine, N.A.; Lee, Stephen R.; Foiles, Stephen M.

Predicting transient effects caused by short - pulse neutron irradiation of electronic devices is an important part of Sandia's mission. For example , predicting the diffusion of radiation - induced point defects is needed with in Sandia's Qualification Alternative to the Sandia Pulsed Reactor (QASPR) pro gram since defect diffusion mediates transient gain recovery in QASPR electronic devices. Recently, the semiconductors used to fabricate radiation - hard electronic devices have begun to shift from silicon to III - V compounds such as GaAs, InAs , GaP and InP . An advantage of this shift is that it allows engineers to optimize the radiation hardness of electronic devices by using alloy s such as InGaAs and InGaP . However, the computer codes currently being used to simulate transient radiation effects in QASP R devices will need to be modified since they presume that defect properties (charge states, energy levels, and diffusivities) in these alloys do not change with time. This is not realistic since the energy and properties of a defect depend on the types of atoms near it and , therefore, on its location in the alloy. In particular, radiation - induced defects are created at nearly random locations in an alloy and the distribution of their local environments - and thus their energies and properties - evolves with time as the defects diffuse through the alloy . To incorporate these consequential effects into computer codes used to simulate transient radiation effects, we have developed procedures to accurately compute the time dependence of defect energies and properties and then formulate them within compact models that can be employed in these computer codes. In this document, we demonstrate these procedures for the case of the highly mobile P interstitial (I P ) in an InGaP alloy. Further dissemination only as authorized to U.S. Government agencies and their contractors; other requests shall be approved by the originating facility or higher DOE programmatic authority.

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Molecular dynamics studies of defect formation during heteroepitaxial growth of InGaN alloys on (0001) GaN surfaces

Journal of Applied Physics

Zhou, Xiaowang Z.; Jones, Reese E.; Gruber, Jacob G.; Lee, Stephen R.; Tucker, G.J.

We investigate the formation of extended defects during molecular-dynamics (MD) simulations of GaN and InGaN growth on (0001) and ( 11 2 ¯ 0 ) wurtzite-GaN surfaces. The simulated growths are conducted on an atypically large scale by sequentially injecting nearly a million individual vapor-phase atoms towards a fixed GaN surface; we apply time-and-position-dependent boundary constraints that vary the ensemble treatments of the vapor-phase, the near-surface solid-phase, and the bulk-like regions of the growing layer. The simulations employ newly optimized Stillinger-Weber In-Ga-N-system potentials, wherein multiple binary and ternary structures are included in the underlying density-functional-theory training sets, allowing improved treatment of In-Ga-related atomic interactions. To examine the effect of growth conditions, we study a matrix of >30 different MD-growth simulations for a range of InxGa1-xN-alloy compositions (0 ≤ x ≤ 0.4) and homologous growth temperatures [0.50 ≤ T/T*m(x) ≤ 0.90], where T*m(x) is the simulated melting point. Growths conducted on polar (0001) GaN substrates exhibit the formation of various extended defects including stacking faults/polymorphism, associated domain boundaries, surface roughness, dislocations, and voids. In contrast, selected growths conducted on semi-polar ( 11 2 ¯ 0 ) GaN, where the wurtzite-phase stacking sequence is revealed at the surface, exhibit the formation of far fewer stacking faults. We discuss variations in the defect formation with the MD growth conditions, and we compare the resulting simulated films to existing experimental observations in InGaN/GaN. While the palette of defects observed by MD closely resembles those observed in the past experiments, further work is needed to achieve truly predictive large-scale simulations of InGaN/GaN crystal growth using MD methodologies.

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Phase degradation in BxGa1−xN films grown at low temperature by metalorganic vapor phase epitaxy

Journal of Crystal Growth

Gunning, Brendan P.; Moseley, Michael; Koleske, Daniel K.; Allerman, A.A.; Lee, Stephen R.

Using metalorganic vapor phase epitaxy, a comprehensive study of BxGa1−xN growth on GaN and AlN templates is described. BGaN growth at high-temperature and high-pressure results in rough surfaces and poor boron incorporation efficiency, while growth at low-temperature and low-pressure (750–900 °C and 20 Torr) using nitrogen carrier gas results in improved surface morphology and boron incorporation up to ~7.4% as determined by nuclear reaction analysis. However, further structural analysis by transmission electron microscopy and x-ray pole figures points to severe degradation of the high boron composition films, into a twinned cubic structure with a high density of stacking faults and little or no room temperature photoluminescence emission. Films with <1% triethylboron (TEB) flow show more intense, narrower x-ray diffraction peaks, near-band-edge photoluminescence emission at ~362 nm, and primarily wurtzite-phase structure in the x-ray pole figures. For films with >1% TEB flow, the crystal structure becomes dominated by the cubic phase. Only when the TEB flow is zero (pure GaN), does the cubic phase entirely disappear from the x-ray pole figure, suggesting that under these growth conditions even very low boron compositions lead to mixed crystalline phases.

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Phase degradation in BxGa1–xN films grown at low temperature by metalorganic vapor phase epitaxy

Journal of Crystal Growth

Gunning, Brendan P.; Moseley, Michael; Koleske, Daniel K.; Allerman, A.A.; Lee, Stephen R.

Using metalorganic vapor phase epitaxy, a comprehensive study of BxGa1-xN growth on GaN and AlN templates is described. BGaN growth at high-temperature and high-pressure results in rough surfaces and poor boron incorporation efficiency, while growth at low-temperature and low-pressure (750–900 °C and 20 Torr) using nitrogen carrier gas results in improved surface morphology and boron incorporation up to ~7.4% as determined by nuclear reaction analysis. However, further structural analysis by transmission electron microscopy and x-ray pole figures points to severe degradation of the high boron composition films, into a twinned cubic structure with a high density of stacking faults and little or no room temperature photoluminescence emission. Films with <1% triethylboron (TEB) flow show more intense, narrower x-ray diffraction peaks, near-band-edge photoluminescence emission at ~362 nm, and primarily wurtzite-phase structure in the x-ray pole figures. For films with >1% TEB flow, the crystal structure becomes dominated by the cubic phase. As a result, only when the TEB flow is zero (pure GaN), does the cubic phase entirely disappear from the x-ray pole figure, suggesting that under these growth conditions even very low boron compositions lead to mixed crystalline phases.

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Identification of the primary compensating defect level responsible for determining blocking voltage of vertical GaN power diodes

Applied Physics Letters

King, Michael P.; Kaplar, Robert K.; Dickerson, Jeramy R.; Lee, Stephen R.; Allerman, A.A.; Crawford, Mary H.; Marinella, Matthew J.; Flicker, Jack D.; Fleming, Robert M.; Kizilyalli, I.C.; Aktas, O.; Armstrong, Andrew A.

Electrical performance and characterization of deep levels in vertical GaN P-i-N diodes grown on low threading dislocation density (∼104 - 106cm-2) bulk GaN substrates are investigated. The lightly doped n drift region of these devices is observed to be highly compensated by several prominent deep levels detected using deep level optical spectroscopy at Ec-2.13, 2.92, and 3.2 eV. A combination of steady-state photocapacitance and lighted capacitance-voltage profiling indicates the concentrations of these deep levels to be Nt = 3 × 1012, 2 × 1015, and 5 × 1014cm-3, respectively. The Ec-2.92 eV level is observed to be the primary compensating defect in as-grown n-type metal-organic chemical vapor deposition GaN, indicating this level acts as a limiting factor for achieving controllably low doping. The device blocking voltage should increase if compensating defects reduce the free carrier concentration of the n drift region. Understanding the incorporation of as-grown and native defects in thick n-GaN is essential for enabling large VBD in the next-generation wide-bandgap power semiconductor devices. Thus, controlling the as-grown defects induced by epitaxial growth conditions is critical to achieve blocking voltage capability above 5 kV.

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Giant Magneto-Resistance in Epitaxial (La0.7Sr0.3MnO3)0.5: (ZnO)0.5 Nanocomposites

Pan, Wei P.; Jiang, Y.X.; Ihlefeld, Jon I.; Lu, Ping L.; Lee, Stephen R.

A great deal of research has been carried out in oxide material systems. Among them, ZnO and La0.7Sr0.3MnO3 (LSMO) are of particular interest due to their superb optical properties and colossal magneto-resistive effect. Here, we report our recent results of magneto-transport studies in self-assembled, epitaxial (ZnO)0.5:(La0.7Sr0.3MnO3)0.5 nanocomposite films.

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Defect-reduction mechanism for improving radiative efficiency in InGaN/GaN light-emitting diodes using InGaN underlayers

Journal of Applied Physics

Armstrong, Andrew A.; Bryant, Benjamin N.; Crawford, Mary H.; Koleske, Daniel K.; Lee, Stephen R.; Wierer, Jonathan W.

The influence of a dilute InxGa1-xN (x ∼ 0.03) underlayer (UL) grown below a single In0.16Ga0.84N quantum well (SQW), within a light-emitting diode (LED), on the radiative efficiency and deep level defect properties was studied using differential carrier lifetime (DCL) measurements and deep level optical spectroscopy (DLOS). DCL measurements found that inclusion of the UL significantly improved LED radiative efficiency. At low current densities, the non-radiative recombination rate of the LED with an UL was found to be 3.9 times lower than the LED without an UL, while the radiative recombination rates were nearly identical. This suggests that the improved radiative efficiency resulted from reduced non-radiative defect concentration within the SQW. DLOS measurement found the same type of defects in the InGaN SQWs with and without ULs. However, lighted capacitance-voltage measurements of the LEDs revealed a 3.4 times reduction in a SQW-related near-mid-gap defect state for the LED with an UL. Quantitative agreement in the reduction of both the non-radiative recombination rate (3.9×) and deep level density (3.4×) upon insertion of an UL corroborates deep level defect reduction as the mechanism for improved LED efficiency.

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Density Functional Theory Calculations of Activation Energies for Non-radiative Carrier Capture by Deep Defect Levels in Semiconductors

Sandia journal manuscript; Not yet accepted for publication

Modine, N.A.; Wright, Alan F.; Lee, Stephen R.

Carrier recombination due to defects can have a major impact on device performance. The rate of defect-induced carrier recombination is determined by both defect levels and carrier capture cross-sections. Kohn-Sham density functional theory (DFT) has been widely and successfully used to predict defect levels in semiconductors and insulators, but only recently has work begun to focus on using DFT to determine carrier capture cross-sections. Lang and Henry worked out the fundamental theory of carrier-capture cross-sections in the 1970s and showed that, in most cases, room temperature carrier-capture cross-sections differ between defects primarily due to differences in the carrier capture activation energies. Here, we present an approach to using DFT to calculate carrier capture activation energies that does not depend on perturbation theory or an assumed configuration coordinate, and we demonstrate this approach for the -3/-2 level of the Ga vacancy in wurtzite GaN.

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Semi-polar GaN materials technology for high IQE green LEDs

Koleske, Daniel K.; Lee, Stephen R.; Crawford, Mary H.; Coltrin, Michael E.

The goal of this NETL funded program was to improve the IQE in green (and longer wavelength) nitride- based LEDs structures by using semi-polar GaN planar orientations for InGaN multiple quantum well (MQW) growth. These semi-polar orientations have the advantage of significantly reducing the piezoelectric fields that distort the QW band structure and decrease electron-hole overlap. In addition, semipolar surfaces potentially provide a more open surface bonding environment for indium incorporation, thus enabling higher indium concentrations in the InGaN MQW. The goal of the proposed work was to select the optimal semi-polar orientation and explore wafer miscuts around this orientation that produced the highest quantum efficiency LEDs. At the end of this program we had hoped to have MQWs active regions at 540 nm with an IQE of 50% and an EQE of 40%, which would be approximately twice the estimated current state-of-the-art.

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Final LDRD report : science-based solutions to achieve high-performance deep-UV laser diodes

Crawford, Mary H.; Allerman, A.A.; Armstrong, Andrew A.; Miller, Mary A.; Smith, Michael L.; Cross, Karen C.; Lee, Stephen R.; Henry, Tania A.; Alessi, Leonard J.

We present the results of a three year LDRD project that has focused on overcoming major materials roadblocks to achieving AlGaN-based deep-UV laser diodes. We describe our growth approach to achieving AlGaN templates with greater than ten times reduction of threading dislocations which resulted in greater than seven times enhancement of AlGaN quantum well photoluminescence and 15 times increase in electroluminescence from LED test structures. We describe the application of deep-level optical spectroscopy to AlGaN epilayers to quantify deep level energies and densities and further correlate defect properties with AlGaN luminescence efficiency. We further review our development of p-type short period superlattice structures as an approach to mitigate the high acceptor activation energies in AlGaN alloys. Finally, we describe our laser diode fabrication process, highlighting the development of highly vertical and smooth etched laser facets, as well as characterization of resulting laser heterostructures.

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Nanoengineering for solid-state lighting

Crawford, Mary H.; Fischer, Arthur J.; Koleske, Daniel K.; Lee, Stephen R.; Missert, Nancy A.

This report summarizes results from a 3-year Laboratory Directed Research and Development project performed in collaboration with researchers at Rensselaer Polytechnic Institute. Our collaborative effort was supported by Sandia's National Institute for Nanoengineering and focused on the study and application of nanoscience and nanoengineering concepts to improve the efficiency of semiconductor light-emitting diodes for solid-state lighting applications. The project explored LED efficiency advances with two primary thrusts: (1) the study of nanoscale InGaN materials properties, particularly nanoscale crystalline defects, and their impact on internal quantum efficiency, and (2) nanoscale engineering of dielectric and metal materials and integration with LED heterostructures for enhanced light extraction efficiency.

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Nanostructural engineering of nitride nucleation layers for GaN substrate dislocation reduction

Koleske, Daniel K.; Lee, Stephen R.; Coltrin, Michael E.; Cross, Karen C.

With no lattice matched substrate available, sapphire continues as the substrate of choice for GaN growth, because of its reasonable cost and the extensive prior experience using it as a substrate for GaN. Surprisingly, the high dislocation density does not appear to limit UV and blue LED light intensity. However, dislocations may limit green LED light intensity and LED lifetime, especially as LEDs are pushed to higher current density for high end solid state lighting sources. To improve the performance for these higher current density LEDs, simple growth-enabled reductions in dislocation density would be highly prized. GaN nucleation layers (NLs) are not commonly thought of as an application of nano-structural engineering; yet, these layers evolve during the growth process to produce self-assembled, nanometer-scale structures. Continued growth on these nuclei ultimately leads to a fully coalesced film, and we show in this research program that their initial density is correlated to the GaN dislocation density. In this 18 month program, we developed MOCVD growth methods to reduce GaN dislocation densities on sapphire from 5 x 10{sup 8} cm{sup -2} using our standard delay recovery growth technique to 1 x 10{sup 8} cm{sup -2} using an ultra-low nucleation density technique. For this research, we firmly established a correlation between the GaN nucleation thickness, the resulting nucleation density after annealing, and dislocation density of full GaN films grown on these nucleation layers. We developed methods to reduce the nuclei density while still maintaining the ability to fully coalesce the GaN films. Ways were sought to improve the GaN nuclei orientation by improving the sapphire surface smoothness by annealing prior to the NL growth. Methods to eliminate the formation of additional nuclei once the majority of GaN nuclei were developed using a silicon nitride treatment prior to the deposition of the nucleation layer. Nucleation layer thickness was determined using optical reflectance and the nucleation density was determined using atomic force microscopy (AFM) and Nomarski microscopy. Dislocation density was measured using X-ray diffraction and AFM after coating the surface with silicon nitride to delineate all dislocation types. The program milestone of producing GaN films with dislocation densities of 1 x 10{sup 8} cm{sup -2} was met by silicon nitride treatment of annealed sapphire followed by the multiple deposition of a low density of GaN nuclei followed by high temperature GaN growth. Details of this growth process and the underlying science are presented in this final report along with problems encountered in this research and recommendations for future work.

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Issues associated with the metalorganic chemical vapor deposition of ScGaN and YGaN alloys

Koleske, Daniel K.; Creighton, J.R.; Lee, Stephen R.; Crawford, Mary H.; Cross, Karen C.; Knapp, J.A.

The most energy efficient solid state white light source will likely be a combination of individually efficient red, green, and blue LED. For any multi-color approach to be successful the efficiency of deep green LEDs must be significantly improved. While traditional approaches to improve InGaN materials have yielded incremental success, we proposed a novel approach using group IIIA and IIIB nitride semiconductors to produce efficient green and high wavelength LEDs. To obtain longer wavelength LEDs in the nitrides, we attempted to combine scandium (Sc) and yttrium (Y) with gallium (Ga) to produce ScGaN and YGaN for the quantum well (QW) active regions. Based on linear extrapolation of the proposed bandgaps of ScN (2.15 eV), YN (0.8 eV) and GaN (3.4 eV), we expected that LEDs could be fabricated from the UV (410 nm) to the IR (1600 nm), and therefore cover all visible wavelengths. The growth of these novel alloys potentially provided several advantages over the more traditional InGaN QW regions including: higher growth temperatures more compatible with GaN growth, closer lattice matching to GaN, and reduced phase separation than is commonly observed in InGaN growth. One drawback to using ScGaN and YGaN films as the active regions in LEDs is that little research has been conducted on their growth, specifically, are there metalorganic precursors that are suitable for growth, are the bandgaps direct or indirect, can the materials be grown directly on GaN with a minimal defect formation, as well as other issues related to growth. The major impediment to the growth of ScGaN and YGaN alloys was the low volatility of metalorganic precursors. Despite this impediment some progress was made in incorporation of Sc and Y into GaN which is detailed in this report. Primarily, we were able to incorporate up to 5 x 10{sup 18} cm{sup -3} Y atoms into a GaN film, which are far below the alloy concentrations needed to evaluate the YGaN optical properties. After a no-cost extension was granted on this program, an additional more 'liquid-like' Sc precursor was evaluated and the nitridation of Sc metals on GaN were investigated. Using the Sc precursor, dopant level quantities of Sc were incorporated into GaN, thereby concluding the growth of ScGaN and YGaN films. Our remaining time during the no-cost extension was focused on pulsed laser deposition of Sc metal films on GaN, followed by nitridation in the MOCVD reactor to form ScN. Finally, GaN films were deposited on the ScN thin films in order to study possible GaN dislocation reduction.

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AlGaN Materials Engineering for Integrated Multi-Function Systems

Lee, Stephen R.; Casalnuovo, Stephen A.; Mani, Seethambal S.; Mitchell, Christine C.; Waldrip, Karen E.; Guilinger, Terry R.; Kelly, M.; Fleming, J.G.; Santa Tsao, Sylviaines; Follstaedt, D.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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Control and Elimination of Cracking of AlGaN Using Low-Temperature AlGaN Interlayers

Applied Physics Letters

Han, J.; Waldrip, Karen E.; Lee, Stephen R.; Figiel, J.J.; Peterscn, G.A.; Myers, S.M.

We demonstrate that the insertion of low-temperature (LT) AlGaN interlayers is effective in reducing mismatch-induced tensile stress and suppressing the formation of cracks during growth of AlGaN directly upon GaN epilayers., Stress evolution and relaxation is monitored using an in-situ optical stress sensor. The combination of in-situ and ex-situ. characterization techniques enables us to determine the degree of pseudomorphism in the interlayers. It is observed that the elastic tensile mismatch between AlGaN and GaN is mediated by the relaxation of interlayers; the use of interlayers offers tunability in the in-plane lattice parameters.

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

Applied Physics Letters

Jones, E.D.; Reno, J.L.; Lee, Stephen R.; Follstaedt, D.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, D.M.; Reno, J.L.; Jones, E.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, D.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, E.D.; Follstaedt, D.M.; Lee, Stephen R.; Reno, J.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, D.M.; Lee, Stephen R.; Reno, J.L.; Jones, E.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, S.M.; Follstaedt, D.M.; Wright, Alan F.; Crawford, Mary H.; Lee, Stephen R.; Seager, Carleton H.; Shul, Randy J.; Baca, A.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, D.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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Metalorganic Vapor-Phase Epitaxial Growth and Characterization of Quaternary AlGaInN

Applied Physics Letters

Han, J.; Figiel, J.J.; Crawford, Mary H.; Banas, Michael A.; Peterson, Gary D.; Myers, S.M.; Lee, Stephen R.

In this letter we report the growth (by MOVPE) and characterization of quaternary AlGaInN. A combination of PL, high-resolution XRD, and RBS characterizations enables us to explore and delineate the contours of equil-emission energy and lattice parameters as functions of the quaternary compositions. The observation of room temperature PL emission as short as 351nm (with 20% Al and 5% In) renders initial evidence that the quaternary could be used to provide confinement for GaInN (and possibly GaN). AlGaInN/GdnN MQW heterostructures have also been grown; both x-ray diffraction and PL measurement suggest the possibility of incorporating this quaternary into optoelectronic devices.

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The Band Gap of AlGaN Alloys

Applied Physics Letters

Lee, Stephen R.

The band gap of AlXGal.XN is measured for the composition range 0s<0.45; the resulting bowing parameter, b=+O.69 eV, is compared to 20 previous works. A correlation is found between the measured band gaps and the methods used for epitaxial growth of the AlXGal_XN: directly nucleated or buffered growths of AlXGal-XN initiated at temperatures T>800 C on sapphire usually lead to stronger apparent bowing (b> +1.3 eV); while growths initiated using low-temperature buffers on sapphire, followed by high-temperature growth, lead to weaker bowing (b<+ 1.3 eV). Extant data suggests that the correct band-gap bowing parameter for AlXGal-XN is b=+O.62 (N.45) eV.

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Reciprocal-Space Analysis of Compositional Modulation in Short-Period Superlattices Using Position-Sensitive X-Ray Detection

Journal of Materials Science: Materials in Electronics

Lee, Stephen R.

Epitaxial growth of AlAs-InAs short-period superlattices on (001) InP can lead to heterostructures exhibiting strong, quasi-periodic, lateral modulation of the alloy composition; transverse satellites arise in reciprocal space as a signature of the compositional modulation. Using an x-ray diffractometer equipped with a position-sensitive x-ray detector, we demonstrate reciprocal-space mapping of these satellites as an efficient, nondestructive means for detecting and characterizing the occurrence of compositional modulation. Systematic variations in the compositional modulation due to the structural design and the growth conditions of the short-period superlattice are characterized by routine mapping of the lateral satellites. Spontaneous compositional modulation occurs along the growth front during molecular-beam epitaxy of (AlAs) (InAs)n short-period superlattices. The modulation is quasi-periodic and forms a lateral superlattice superimposed on the intended SPS structure. Corresponding transverse satellites arise about each reciprocal lattice point, and x-ray diffraction can be routinely used to map their local reciprocal-space structure. The integrated intensity, spacing, orientation, and shape of these satellites provide a reliable means for nondestructively detecting and characterizing the compositional modulation in short-period superlattices. The analytical efficiency afforded by the use of a PSD has enabled detailed study of systematic vacations in compositional modulation as a function of the average composition, the period, and the growth rate of the short- period superlattice

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Evaluation of factors affecting the timing capabilities of the MC3858 sprytron

Lee, Stephen R.

The switch delay time of the MC3858 sprytron was measured using a test matrix consisting of 36 different trigger circuit configurations. The test matrix allowed the measurement of switch delay times for peak trigger voltages ranging from 47 V to 1340 V and for stored trigger energies ranging from 0.023 mJ to 2.7 mJ. The average switch delay time was independent of peak trigger voltage above approximately 800 V. Similarly, the average switch delay was independent of trigger stored energy above approximately 0.5 mJ. Below these saturation values, the average switch delay increases rapidly with decreasing trigger voltage or esergy. In contrast to the average switch delay time, the shot-to-shot variability in switch delay time does not appear to be strongly affected by peak trigger voltage as long as the trigger voltage is groater than 100 V. Below 100 V, the variability in switch delay time rises rapidly due to failure of the trigger to undergo immediate high voltage breakdown when trigger voltage is applied. The effect of an abnormally-high-resistance trigger probe on switch delay time was also investigated. It was found that a high-resistance probe behaved as a second overvoltage gap in the trigger circuit. Operation with a peak trigger voltage greater than the breakdown voltage of this second gap yielded delay times comparable to operation with a normal trigger. Operation with a peak trigger voltage less than the breakdown voltage of this second gap increased the switch delay time by an amount comparable to the time required to ramp the trigger circuit output up to the breakdown voltage of the second gap. Finally, the effect that varying the bias voltage applied to the sprytron has on switch delay time was measured. The switch delay time did not appear to depend on bias voltage for bias voltages between 725 V and 2420 V.

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98 Results
98 Results