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DOE OSTI2026

Oxide-nitride heteroepitaxy for low-loss dielectrics in superconducting quantum circuits

Superconducting qubits show great promise for the realization of fault-tolerant quantum computing, but lossy, amorphous dielectrics limit current technology. Identifying highly crystalline and stoichiometric dielectrics with intrinsically low microwave loss is therefore a central materials challenge, yet experimentally validated platforms remain scarce. In this work, we integrate a crystalline dielectric into a heteroepitaxial TiN/$γ$-Al$_2$O$_3$/TiN trilayer grown via pulsed laser deposition. Correlative high-resolution imaging, diffraction, and spectroscopy measurements confirm the single-crystal quality and chemical integrity of all layers, with minimal defects and limited anion interdiffusion across the oxide-nitride interfaces. Using microwave lumped-element resonators with parallel-plate capacitors, we report the first direct measurement of the dielectric loss of epitaxial $γ$-Al$_2$O$_3$, for which we find a low intrinsic two-level system loss, $δ_{\text{TLS}}^0 = (2.8 \pm 0.1) \times 10^{-5}$. These results establish heteroepitaxial oxides on transition metal nitrides as an attractive materials platform for superconducting quantum circuits, particularly for integration into compact device architectures such as merged-element transmons and microwave kinetic inductance detectors.

Garcia-Wetten, David A. [Northwestern U.]↗

NASA NTRS2000

Study of Doped ZnO Films Synthesized by Combining Vapor Gases and Pulsed Laser Deposition

The properties and structure of the ZnO material are similar to those of the GaN. Since an excitonic binding energy of ZnO is about 60 meV, it has strong potential for excitonic lasing at the room temperature. This makes synthesizing ZnO films for applications attractive. However, there are several hurdles in fabricating electro-optical devices from ZnO. One of those is in growing doped p-type ZnO films. Although techniques have been developed for the doping of both p-type and n-type ZnO, this remains an area that can be improved. In this presentation, we will report the experimental results of using both thermal vapor and pulsed laser deposition to grow doped ZnO films. The films are deposited on (0001) sapphire, (001) Si and quartz substrates by ablating a ZnO target. The group III and V elements are introduced into the growth chamber using inner gases. Films are characterized by x-ray diffraction, scanning probe microscopy, energy dispersive spectroscopy, Auger electron spectroscopy, and electrical measurements. The full width at half maximum of theta rocking curves for epitaxial films is less than 0.5 deg. In textured films, it rises to several degrees. Film surface morphology reveals an island growth pattern, but the size and density of these islands vary with the composition of the reactive gases. The electrical resistivity also changes with the doped elements. The relationship between the doping elements, gas composition, and film properties will be discussed.

Zhu, Shen↗

DOE OSTI2021

High-Brightness Ultraviolet Lasers for Leap-Ahead National Security Applications

In this project we endeavored to improve the state-of-the-art in UV lasers diodes. We made important advancements in several fronts from modeling, to epitaxial growth, to fabrication, and testing. Throughout the project it became clear that polarization doping would be able to help advance the state of laser diode design in terms of electrical performance, but the optical design would need to be investigated to ensure that a 2D guided mode would be supported. New capability in optical modeling using commercial software demonstrated that the new polarization doped structures would be viable. New capability in pulsed testing was established to reach the current and voltage required. Our fabricated devices had some parasitic electrical paths which hindered performance that we were ultimately unable to overcome in the project timeframe. We do believe that future projects will be able to leverage the advancements made under this project.

36 MATERIALS SCIENCE↗

NASA NTRS1976

Development of a high capacity bubble domain memory element and related epitaxial garnet materials for application in spacecraft data recorders. Item 2: The optimization of material-device parameters for application in bubble domain memory elements for spacecraft data recorders

Bubble domain materials and devices are discussed. One of the materials development goals was a materials system suitable for operation of 16 micrometer period bubble domain devices at 150 kHz over the temperature range -10 C to +60 C. Several material compositions and hard bubble suppression techniques were characterized and the most promising candidates were evaluated in device structures. The technique of pulsed laser stroboscopic microscopy was used to characterize bubble dynamic properties and device performance at 150 kHz. Techniques for large area LPE film growth were developed as a separate task. Device studies included detector optimization, passive replicator design and test and on-chip bridge evaluation. As a technology demonstration an 8 chip memory cell was designed, tested and delivered. The memory elements used in the cell were 10 kilobit serial registers.

Besser, P. J.↗

DOE OSTI2024

Growth of ultra-flat ultra-thin alkali antimonide photocathode films

Ultra-flat, ultra-thin alkali antimonide photocathodes with high crystallinity can exhibit high quantum efficiency and low mean transverse energy of outgoing electrons, which are essential requirements for a variety of applications for photocathode materials. Here, we investigate the growth of Cs 3 Sb on graphene-coated 4H–SiC (Gr/4H–SiC), 3C–SiC, and Si 3 N 4 substrates. Sb is deposited using pulsed laser deposition, while Cs is deposited thermally and simultaneously. We demonstrate, employing x-ray analysis and quantum efficiency measurements, that this growth method yields atomically smooth Cs 3 Sb photocathodes with a high quantum efficiency (>10%), even in the ultra-thin limit (<30 nm). For the Si 3 N 4 substrate, film growth is shown to be polycrystalline, while films grown on Gr/4H–SiC show a high degree of ordering with signs of epitaxy.

36 MATERIALS SCIENCE↗

NASA NTRS1982

Studies of single-mode injection lasers and of quaternary materials. Volume 1: Single-mode constricted double-heterojunction AlGaAs diode lasers

Constricted double-heterojunction (CDH) lasers are presented as the class of single-mode nonplanar-substrate devices for which the lasing cavity is on the least resistive electrical path between the contact and the substrate. Various types of CDH structures are considered under three general topics: liquid-phase epitaxy over channeled substrates, lateral mode control, and current control in nonplanar-substrate devices. Ridge-guide CDH lasers have positive-index lateral-mode confinement and provide: single-mode CW operation to 7 mW/facet at room temperature and to 3 mW/facet at 150 C; light-current characteristics with second-harmonic distortion as low as -57 dB below the fundamental level; threshold-current temperature coefficients, as high as 375 C (pulsed) and 310 C (CW); constant external differential quantum efficiency to 100 C; and lasing operation to 170 C CW and 280 C pulsed. Semileakyguide CDH lasers have an asymmetric leaky cavity for lateral-mode confinement and provide single-mode operation to 15 to 20 mW/facet CW and to 50 mW/facet at 50% duty cycle. Modulation characteristics and preliminary reliability data are discussed.

Botez, D.↗

NASA NTRS1987

InGaAs/GaAs multiquantum-well electroabsorption modulator with integrated waveguide

A monolithically integrated guided-wave modulator has been realized by using molecular-beam epitaxial regrowth and ion-milling techniques. The guiding and modulating regions consist, respectively, of In-doped GaAs and GaAs/In(0.34)Ga(0.66)As strained-layer multiquantum wells. Modulation is achieved by field-enhanced electroabsorption in the multiquantum wells. The insertion loss of the modulator is 0.9 dB, and the transmission loss in the guides is less than or equal to 1 dB/cm. The temporal response of similar GaAs/InGaAs as-grown photodiodes to pulsed laser excitation is characterized by a rise time of 115 psec.

Das, Utpal↗

DOE OSTI2020

Unconventional crystal-field splitting in noncentrosymmetric BaTiO 3 thin films

Understanding the crystal-field splitting and orbital polarization in noncentrosymmetric systems such as ferroelectric materials is fundamentally important. In this work, taking BaTiO 3 as a representative material, we investigate titanium crystal-field splitting and orbital polarization in noncentrosymmetric TiO 6 octahedra with resonant x-ray linear dichroism at the Ti L 2,3 edge. The high-quality BaTiO 3 thin films were deposited on DyScO 3 (110) single crystal substrates in a layer-by-layer way by pulsed laser deposition. The reflection high-energy electron diffraction and element specific x-ray absorption spectroscopy were performed to characterize the structural and electronic properties of the films. In sharp contrast to conventional crystal-field splitting and orbital configuration (d xz /d yz < d xy < d 3z 2 -r 2 < d x 2 -y 2 or d xy < d xz /d yz < d x 2 -y 2 < d 3z 2 -r 2 ) expected from compressive or tensile epitaxial strain, respectively, it is revealed that d xz , d yz , and d xy orbitals are nearly degenerate, whereas d 3z 2 -r 2 and d x 2 -y 2 orbitals are split with an energy gap ~100 meV in the epitaxial BaTiO 3 films. We find that the unexpected degenerate orbitals d xz /d yz /d xy result from the competition between the orbital splitting induced by epitaxial strain and that induced by polar distortions of BaTiO 3 films. Our results provide a route to manipulate orbital degree of freedom by switching electric polarization in ferroelectric materials.

36 MATERIALS SCIENCE↗

NASA NTRS2003

Low threshold interband cascade lasers operating above room temperature

Mid-IR type-II interband cascade lasers were demonstrated in pulsed mode at temperatures up to 325 K and in continuous mode up to 200 K. At 80 K, the threshold current density was 8.9 A/cm2 and a cw outpout power of ~140 mW/facet was obtained.

interband cascade lasers GaSb molecular beam epita↗

NASA NTRS1992

Room-temperature operation of MOCVD-grown GaInAs/InP strained-layer multiquantum well lasers in 1.8 micron range

The first successful room-temperature pulsed operation is reported of InGaAs strained layer multiquantum well injection lasers grown by MOVPE on InP substrates in the 1.8 micron range. The threshold current density and the external differential quantum efficiency of the 10 micron wide ridge waveguide lasers were 2.5 kA/sq cm (cavity length = 1 mm) and 5 percent (cavity length = 400 microns), respectively. Broad-area lasers, 100 microns wide and 1 mm long, had a reverse leakage current of less than 10 microamps at -1 V indicating high quality of the epitaxial layers.

Forouhar, S.↗

NASA NTRS1975

Semiconductor diode laser material and devices with emission in visible region of the spectrum

Two alloy systems, (AlGa)As and (InGa)P, were studied for their properties relevant to obtaining laser diode operation in the visible region of the spectrum. (AlGa)As was prepared by liquid-phase epitaxy (LPE) and (InGa)P was prepared both by vapor-phase epitaxy and by liquid-phase epitaxy. Various schemes for LPE growth were applied to (InGa)P, one of which was found to be capable of producing device material. All the InGaP device work was done using vapor-phase epitaxy. The most successful devices were fabricated in (AlGa)As using heterojunction structures. At room temperature, the large optical cavity design yielded devices lasing in the red (7000 A). Because of the relatively high threshold due to the basic band structure limitation in this alloy, practical laser diode operation is presently limited to about 7300 A. At liquid-nitrogen temperature, practical continuous-wave operation was obtained at a wavelength of 6500 to 6600 A, with power emission in excess of 50 mW. The lowest pulsed lasing wavelength is 6280 A. At 223 K, lasing was obtained at 6770 A, but with high threshold currents. The work dealing with CW operation at room temperature was successful with practical operation having been achieved to about 7800 A.

Ladany, I.↗

DOE OSTI2020

Enhanced magnetocaloric performance in manganite bilayers

Bilayer films of La 0.8 Sr 0.2 MnO 3 and La 0.7 Ca 0.3 MnO 3 with different layer thicknesses and stacking sequences were synthesized via pulsed laser deposition. The magnetic properties and magnetocaloric effects were systematically investigated. We found that the phase transition associated with the layers tends to merge together at an optimal thickness and a stacking sequence. The operating temperature span of the entropy change broadens at the expense of its magnitude, leading to an enhancement of the refrigerant capacity by over 40%. The optimized bilayer film possesses a refrigerant capacity of ~6.0J/kg, compared to a value of ~4.2J/kg for the single-phase films. The phase transition broadening induced by epitaxial strain is responsible for the enhanced window of operating temperature as well as refrigerant capacity. Finally, the design principle developed here may be applied to ferroelastic and ferroelectric materials to enhance elastocaloric and electrocaloric effects.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Recent Advances in Vertically Aligned Nanocomposites with Tunable Optical Anisotropy: Fundamentals and Beyond

Developing reliable and tunable metamaterials is fundamental to next-generation optical-based nanodevices and computing schemes. In this review, an overview of recent progress made with a unique group of ceramic-based functional nanocomposites, i.e., vertically aligned nanocomposites (VANs), is presented, with the focus on the tunable anisotropic optical properties. Using a self-assembling bottom-up deposition method, the as-grown VANs present great promise in terms of structural flexibility and property tunability. Such broad tunability of functionalities is achieved through VAN designs, material selection, growth control, and strain coupling. The as-grown multi-phase VAN films also present enormous advantages, including wafer scale integration, epitaxial quality, sharp atomic interface, as well as designable materials and geometries. This review also covers the research directions with practical device potentials, such as multiplex sensing, high-temperature plasmonics, magneto-optical switching, as well as photonic circuits.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Enhancement in electro-optic performance of InAlGaAs/GaAs quantum dot lasers by ex situ thermal annealing

Here, this Letter reports the growth, fabrication, and characterization of molecular beam epitaxy (MBE)-grown quaternary InAlGaAs/GaAs quantum dot (QD) lasers emitting at sub-900 nm. The presence of Al in QD-based active regions acts as the origin of defects and non-radiative recombination centers. Applying optimized thermal annealing annihilates the defects in p-i-n diodes, thus lowering the reverse leakage current by six orders of magnitude compared to as-grown devices. A systematic improvement in the optical properties of the devices is also observed in the laser devices with increasing annealing time. At an annealing temperature of 700°C for 180 s, Fabry–Pérot lasers exhibit a lower pulsed threshold current density at infinite length of 570 A/cm 2 .

42 ENGINEERING↗

NASA NTRS2012

Terahertz Quantum Cascade Laser With Efficient Coupling and Beam Profile

Quantum cascade lasers (QCLs) are unipolar semiconductor lasers, where the wavelength of emitted radiation is determined by the engineering of quantum states within the conduction band in coupled multiple-quantum-well heterostructures to have the desired energy separation. The recent development of terahertz QCLs has provided a new generation of solid-state sources for radiation in the terahertz frequency range. Terahertz QCLs have been demonstrated from 0.84 to 5.0 THz both in pulsed mode and continuous wave mode (CW mode). The approach employs a resonant-phonon depopulation concept. The metal-metal (MM) waveguide fabrication is performed using Cu-Cu thermo-compression bonding to bond the GaAs/AlGaAs epitaxial layer to a GaAs receptor wafer.

Chattopadhyay, Goutam↗

DOE OSTI2025

Ultra-Fast Non-Volatile Resistive Switching Devices with Over 512 Distinct and Stable Levels for Memory and Neuromorphic Computing

Low-current multilevel programmability with inherent non-volatility and high stability of resistance states is required for both multi-bit memory storage and deep learning accelerators but is difficult to achieve. Here, in a resistive switching system, this work realizes >512 (>9 bits) distinct non-volatile conductance levels with stable retention for each state with current levels down to the nanoampere range, highly promising for potential integration with small processing nodes with ultra-low power consumption requirements. This is achieved by demonstrating a new thin film design concept that encompasses three key features: an ultra-thin epitaxial oxygen ionic switching layer that provides a tunable energy barrier at the bottom electrode, an overcoat amorphous layer that acts as an ion migration barrier for stable state retention, and a partial conductive filament as a localized electronic transport channel to the epitaxial switching layer. A large dynamic resistance range of up to seven orders of magnitude is achieved with reset-free transitions among intermediate states, and programmability is demonstrated with ultra-fast (20 ns) pulses. Artificial neural network (ANN) simulations, based on the experimental performance and its non-idealities, demonstrate close-to-ideal inference accuracies for various Modified National Institute of Standards and Technology (MNIST) data sets.

36 MATERIALS SCIENCE↗

NASA NTRS1990

Superconductivity applications for infrared and microwave devices; Proceedings of the Meeting, Orlando, FL, Apr. 19, 20, 1990

Various papers on superconductivity applications for IR and microwave devices are presented. The individual topics addressed include: pulsed laser deposition of Tl-Ca-Ba-Cu-O films, patterning of high-Tc superconducting thin films on Si substrates, IR spectra and the energy gap in thin film YBa2Cu3O(7-delta), high-temperature superconducting thin film microwave circuits, novel filter implementation utilizing HTS materials, high-temperature superconductor antenna investigations, high-Tc superconducting IR detectors, high-Tc superconducting IR detectors from Y-Ba-Cu-O thin films, Y-Ba-Cu0-O thin films as high-speed IR detectors, fabrication of a high-Tc superconducting bolometer, transition-edge microbolometer, photoresponse of YBa2Cu3O(7-delta) granular and epitaxial superconducting thin films, fast IR response of YBCO thin films, kinetic inductance effects in high-Tc microstrip circuits at microwave frequencies.

Bhasin, Kul B.↗

NASA NTRS1979

Laser Techniques in Photovoltaic Research

High-power laser pulses were used to replace the conventional high temperature furnace processing for the p-n junction formation step in high speed, low cost solar cell fabrication. Three different approaches to junction formation were tested: (1) laser annealing of ion-implanted Si in which laser radiation is used to remove the radiation damage and to recover the electrical activity in the implanted layer; (2) a process in which a thin film of dopant is first deposited on the substrate and then incorporated into the near-surface region by laser-induced diffusion; and (3) a process in which a heavily doped amorphous silicon layer is deposited on the Si substrate and epitaxially regrown from the melted substrate layer by laser radiation. All three methods were found to provide suitable candidates for high efficiency Si solar cells.

Young, R. T.↗