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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 307 records · Page 17

Synchronous detection of cosmic rays and correlated errors in superconducting qubit arrays

Quantum information processing at scale will require sufficiently stable and long-lived qubits, likely enabled by error-correction codes. Several recent superconducting-qubit experiments, however, reported observing intermittent spatiotemporally correlated errors that would be problematic for conventional codes, with ionizing radiation being a likely cause. Here, we directly measured the cosmic-ray contribution to spatiotemporally correlated qubit errors. We accomplished this by synchronously monitoring cosmic-ray detectors and qubit energy-relaxation dynamics of 10 transmon qubits distributed across a 5 × 5 × 0.35 mm 3 silicon chip. Cosmic rays caused correlated errors at a rate of $1/\left(592\begin{array}{c}+48\\ -41\end{array}\,{\rm{s}}\right)$, accounting for 17.1 ± 1.3% of all such events. Our qubits responded to essentially all of the cosmic rays and their secondary particles incident on the chip, consistent with the independently measured arrival flux. Moreover, we observed that the landscape of the superconducting gap in proximity to the Josephson junctions dramatically impacts the qubit response to cosmic rays. Given the practical difficulties associated with shielding cosmic rays, our results indicate the importance of radiation hardening—for example, superconducting gap engineering—to the realization of robust quantum error correction.

Science & Technology - Other Topics↗

Bridging the gap between molecules and materials in quantum chemistry with localized active spaces

The number of materials that “bridge the gap” between single molecules and extended solids, such as metal-organic frameworks and organic semiconductors, has been increasing. Consequently, there is a growing need for modeling approaches that effectively integrate the real-space molecular perspective employed by computational chemists and the reciprocal-space dispersive perspective employed by computational physicists. Here, we propose the localized active space (LAS) approach as a promising method to successfully bridge this gap. The LAS approach extends the active space concept from multiconfigurational methods such as complete active space self-consistent field theory to multiple molecular fragments via a product-form wave function ansatz. Here, we apply this method to solid state phenomena by treating each unit cell as a fragment with different sets of local quantum numbers (e.g., charge and excitation number). State interaction between these LAS states (LASSI) thus provides a comprehensive basis for the study of charge and energy transfer, meeting and surpassing the capabilities of single-reference fragmentation approaches such as constrained density functional theory (cDFT). Most centrally, we show how combining this LASSI approach with multiconfigurational pair-density functional theory (MC-PDFT) provides an elegant and efficient method to compute band structures that capture multiconfigurational character. We apply the LASSI band structure approach to the computation of band gaps in stretched hydrogen chain, polyacetylene, and bulk nickel oxide (NiO), finding good or excellent quantitative agreement with reference values in all cases. Additionally, we use the LAS basis in one-dimensional model systems to demonstrate its ability to treat difficult solid-state phenomena such as exciton transfer and excitation at p-n junctions.

method development↗

Ferroelectrically switched valley-dependent transmission in SnTe-PbTe-SnTe monolayer lateral heterostructures

A special class of valleytronic two-dimensional (2D) semiconductors possesses carrier pockets (i.e., valleys) along certain directions in the first Brillouin zone, which can be applied as a new degree of freedom for information storage and processing. Here we show that members of this family that are ferroelectric allow the location of these valleys to be switched by rotating the ferroelectric polarization. This makes possible the control of electronic state transmission probability through an energy barrier by ferroelectrically switching the polarization direction, thereby creating or eliminating valley matching in reciprocal space. We apply molecular beam epitaxy to grow lateral sandwich heterostructures with monolayer-thick ferroelectric SnTe separated by nanometer-wide paraelectric PbTe as the barriers. Using scanning tunneling microscopy, we show that the transmission probability of the 2D hole states at the valence band maximum of SnTe monolayer strongly relies on the relative orientation between the polarization directions of the two SnTe electrodes. The transmission can be switched from a suppressed state to a permitted state by rotating the ferroelectric polarization of one SnTe electrode by 90 degrees. Our work demonstrates the electric-field-control of valley locations and its potential for tunnel junction valleytronic devices.

electronic devices↗

Observation of interface piezoelectricity in superconducting devices on silicon

The development of superconducting quantum processors relies on understanding and mitigating decoherence in superconducting qubits. Piezoelectric coupling contributes to decoherence by mediating energy exchange between microwave photons and acoustic phonons. Although bulk centrosymmetric materials like silicon and sapphire are non-piezoelectric and commonly used as qubit substrates, the lack of centrosymmetry at interfaces may induce piezoelectric losses. This effect was predicted decades ago but never experimentally observed in superconducting devices. Here, we report interface piezoelectricity at aluminum-silicon junctions and demonstrate it as a significant loss channel in superconducting devices. Using aluminum interdigital transducers on silicon, we observe piezoelectric transduction from room to millikelvin temperatures, with an effective electromechanical coupling factor K 2 ≈ (3 ± 0.4) × 10−5%, comparable to weakly piezoelectric substrates. Modeling shows this mechanism limits qubit quality factors to Q ~ 10 4 − 10 8 , depending on surface participation and mode matching. These findings reveal interface piezoelectricity as a major dissipation channel and highlight the need for heterostructure and phononic engineering in next-generation superconducting qubits.

Zhou, Haoxin [University of California, Berkeley, ↗

Chain entanglements enable regeneration of high-performance thermosets

Thermoset plastics underpin structural materials, electronics and transportation, yet the permanent covalent networks that prevent flow and provide dimensional stability also make them difficult to recycle without sacrificing performance. In this work we show that high-performance thermosets can be built around dense chain entanglements, the physical interlacing of long polymer strands, rather than dense permanent crosslinks, with only a small number of selectively cleavable junctions preserving connectivity. Long, rigid, entangled polyolefin backbones generated by frontal polymerization form glassy polymers with high stiffness, high toughness and excellent creep suppression yet can be fully deconstructed into soluble, linear oligomers. Varying oligomer length and end-group chemistry enables their reuse as re-entangling building blocks that regenerate thermosets with thermal and mechanical properties that remain unchanged across generations. The strategy further extends to high-temperature fibre-reinforced composite matrices and additively manufactured structures, establishing chain entanglement as a design principle for durable, regenerable thermosets.

36 MATERIALS SCIENCE↗

Nanoscopic cross-grain cation homogenization in perovskite solar cells

Multiscale cation inhomogeneity has been a major hurdle in state-of-the-art formamidinium–caesium (FA–Cs) mixed-cation perovskites for achieving perovskite solar cells with optimal power conversion efficiencies and durability. Although the field has attempted to homogenize the overall distributions of FA–Cs in perovskite films from both plan and cross-sectional views, our understanding of grain-to-grain cation inhomogeneity and ability to tailor it—that is, spatially resolving the FA–Cs compositional difference between individual grains down to the nanoscale—are lacking. Here we reveal that as fundamental building blocks of a perovskite film, individual grains exhibit cationic compositions deviating from the prescribed ideal composition, severely limiting the interfacial optoelectronic properties and perovskite layer durability. This performance-limiting nanoscopic factor is linked to thermodynamic-driven morphological grooving, leading to a segmented surface landscape. At the grain triple junctions, grooves form nanoscale groove traps that hinder the mixing of solid-state cations across grains and thus retard inter-grain FA–Cs mixing. By rationally modulating the heterointerfacial energies, we reduced the depth of these nanoscale groove traps by a factor of three, significantly improving cation homogeneity. Perovskite solar cells with shallower nanoscale groove traps demonstrate enhanced power conversion efficiencies (25.62%) and improved stability under various standardized international protocols. In conclusion, our work highlights the significance of resolving surface nano-morphologies for homogeneous properties of perovskites.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Direct experimental constraints on the spatial extent of a neutrino wavepacket

Despite their high relative abundance in our Universe, neutrinos are the least understood fundamental particles of nature. In fact, the quantum properties of neutrinos emitted in experimentally relevant sources are theoretically contested and the spatial extent of the neutrino wavepacket is only loosely constrained by reactor neutrino oscillation data with a spread of 13 orders of magnitude. Here we present a method to directly access this quantity by precisely measuring the energy width of the recoil daughter nucleus emitted in the radioactive decay of beryllium-7. The final state in the decay process contains a recoiling lithium-7 nucleus, which is entangled with an electron neutrino at creation. The lithium-7 energy spectrum is measured to high precision by directly embedding beryllium-7 radioisotopes into a high-resolution superconducting tunnel junction that is operated as a cryogenic sensor. Under this approach, we set a lower limit on the Heisenberg spatial uncertainty of the recoil daughter of 6.2 pm, which implies that the final-state system is localized at a scale more than a thousand times larger than the nucleus itself. From this measurement, the first, to our knowledge, direct lower limit on the spatial extent of a neutrino wavepacket is extracted. These results may have implications in several areas including the theoretical understanding of neutrino properties, the nature of localization in weak nuclear decays and the interpretation of neutrino physics data.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Strain engineering of doped hydrogen passivated silicon quantum dots

Silicon quantum dots are nanomaterials that are attractive candidates for photovoltaic applications. Doping of these materials creates p-n junctions and is important for solar cells. In this work, we present a first-principles study of the coupled influence of doping and strain on the stability, energy gap, Fermi level, electronic density, and density of states of hydrogen-passivated silicon quantum dots. We find that the cohesive energy and the energy gap decrease with increasing quantum dot size and are strongly influenced by strain. Furthermore, the response to strain also depends on the size of the quantum dot and dopant type. We present expressions of cohesive energy and energy gap as power-law of size and polynomial dependence on strain. We also show that the Fermi energy increases with size for pristine and p-type doping but decreases with size for n-type doping. We also discuss the influence of strain and dopant type on the density of states and electron density of the quantum dots.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Magnetic flux imaging in a 3D superconductor integrated circuit

We report on imaging magnetic flux distributions in a multilayered superconductor integrated circuit which emerge during magnetization and after field cooling of the circuit in the DC magnetic field. The obtained complicated field maps expose the flux propagation across the patterned superconducting ground planes sandwiching layers with Josephson junction-based logic cells, fine wire grid around the functional units, and multiple superconducting fill structures located in different inner layers. The observed intricate flux distributions are explained by specific patterns of Meissner screening currents and superconducting critical currents in different mutually interacting parts of the integrated circuit. Our results provide important insights into possible ways of improving the protection of superconductor integrated circuits from magnetic fields and their resilience against flux trapping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

An antiferromagnetic diode effect in even-layered MnBi 2 Te 4

In a p–n junction, the separation of positive and negative charges leads to diode transport, in which charge flows in only one direction. Non-centrosymmetric polar conductors are intrinsic diodes that could be of use in the development of nonlinear applications. Such systems have recently been extended to non-centrosymmetric superconductors, and the superconducting diode effect has been observed. Here, in this paper, we report an antiferromagnetic diode effect in a centrosymmetric crystal without directional charge separation. We observed large second-harmonic transport in a nonlinear electronic device enabled by the compensated antiferromagnetic state of even-layered MnBi 2 Te 4 . We show that this antiferromagnetic diode effect can be used to create in-plane field-effect transistors and microwave-energy-harvesting devices. We also show that electrical sum-frequency generation can be used as a tool to detect nonlinear responses in quantum materials.

electronic properties and materials↗

Facets control charge separation during photoelectrochemical water oxidation with strontium titanate (SrTiO 3 ) single crystals

The photocatalytic overall water splitting reaction provides a pathway to hydrogen fuel from sunlight. Photocatalysts must achieve the reaction without the application of an external bias, which requires an effective charge separation mechanism. Photolabeling studies and electrostatic simulations for the well-known CoOOH/Al:SrTiO 3 /Rh/Cr 2 O 3 photocatalyst suggest that charge separation is driven by work function differences at the (100) and (110) facets of SrTiO 3 , which are electron and hole selective, respectively. Here we use hydrogen annealed SrTiO 3–x single crystals to obtain the first quantitative assessment of the charge separation ability of the (100), or (110), or (111) facets during oxygen evolution. Under UV illumination (60 mW cm –2 ), the crystals exhibit variable water oxidation photocurrents (0.34, 0.82, 1.36 mA cm –2 at 1.23 V versus RHE) and photovoltage values of 1.40, 1.52 and 1.52 V for (100), (110), and (111) SrTiO 3–x , respectively. A surface photovoltage increase in that same order (0.31 V < 0.57 V < 0.67 V) is confirmed independently with vibrating Kelvin probe surface photovoltage spectroscopy (VKP-SPV) under 375 nm (1.91 mW cm –2 ) illumination. Mott Schottky measurements in aqueous K 3/4 [Fe(CN) 6 ] reveal facet-dependent flatband positions of –0.58, –0.71, and –0.74 V RHE for the (100), (110), and (111) crystals respectively. This confirms that the photoelectrochemical water oxidation performance of SrTiO 3–x crystals is controlled by the work function of each facet, which determines the electron transfer barrier height of the respective solid–liquid junctions. After correcting for differences in electron donor concentrations, barriers are found to increase in the order (100) < (111) < (110) and differ by as much as 0.16 eV, similar to an earlier prediction. Altogehter, these results explain the charge separation mechanism in SrTiO 3 photocatalysts and highlight the need for faceted semiconductor crystals as light absorbers in particle-based photocatalysts.

08 HYDROGEN↗

Integrating magnetic Co-nanopillars in a NbN-based VAN thin film as a multifunctional hybrid metamaterial

NbN thin films are considered as a promising alternative candidate to conventional Al superconducting electrodes for Josephson junction devices, superconducting qubits and quantum logic circuits. Herein, by co-growing ferromagnetic Co with superconducting NbN, self-assembled NbN–Co vertically aligned nanocomposite (VAN) thin films have been successfully deposited on a MgO substrates, with NbN in its cubic superconducting phase. The obtained VAN metamaterials exhibit epitaxial growth of NbN with uniformly dispersed Co nanoplates. Further physical property characterization reveals that the NbN–Co VAN presents ferromagnet properties with strong out-of-plane magnetic anisotropy and optical anisotropy. This hybrid metamaterial system could find future applications in superconducting spintronic devices and quantum computing devices.

Zhang, Yizhi [Purdue Univ., West Lafayette, IN (Un↗

Bandgap engineering of SrZrS 3 chalcogenide perovskite via substitutional doping for photovoltaic applications: a first-principles DFT study

Strontium zirconium sulfide (SrZrS 3 ) has garnered significant attention for photovoltaic (PV) applications due to its excellent optoelectronic properties, high chemical and moisture stability, and non-toxicity. However, the bandgaps of both the α- and β-phases lie outside the optimum ranges for both single-junction solar cells (SJSCs) and tandem solar cells (TSCs), thereby limiting their applications in PV technologies. In this study, we employed hybrid density functional theory to engineer the band gaps of α- and β-SrZrS 3 through substitutional doping. We considered three dopants (Hf, Sn, and Ti) at the Zr site of SrZrS 3 with varying doping concentrations and investigated their effects on the structural, electronic, and optical properties of the materials. We found that Sn and Ti doping effectively lowers the band gaps of both α- and β-SrZrS 3 , whereas Hf doping increases them. For x values up to 0.25, the band gaps of the α-SrZr 1−x Sn x S 3 and α-SrZr 1−x Ti x S 3 are within the optimum range for SJSCs, and those of β-SrZr 1−x Sn x S 3 and β-SrZr 1−x Ti x S 3 lie within the optimum range for Si/perovskite as well as perovskite/perovskite TSCs. The three dopants exhibited significant effects on the optical properties of both α- and β-SrZrS 3 , including the absorption coefficient, energy-loss functions, reflectivity, and refractivity spectra. Thermodynamic stability analysis revealed that for both phases, SrZr 1−x Hf x S 3 can be synthesized via exothermic processes, whereas the formation of SrZr 1−x Ti x S 3 and SrZr1−xSn x S 3 is endothermic and hence, not thermodynamically favorable. Further analysis showed that SrZr 1−x Ti x S 3 in both α- and β-phases are stable under thermodynamic equilibrium conditions, whereas SrZr 1−x Sn x S 3 is prone to dissociation into ternary phases (SrZrS 3 and SrSnS 3 ), especially at higher doping concentrations. These results show that Ti doping is effective in tuning the band gaps of α- and β-SrZrS 3 toward the optimal values for PV applications.

14 SOLAR ENERGY↗

Oxygen vacancy-induced ferroelectric effect in (111) strontium titanate single crystals controls photoelectrochemical water oxidation

Ferroelectric materials, such as tetragonal BaTiO 3 , have a permanent electric polarization that can be controlled with an external electric field, however, a ferroelectric polarization in cubic SrTiO 3 is forbidden by the higher symmetry of the lattice. Here we demonstrate that hydrogen annealed SrTiO 3−x single crystals can be polarized electrically, and that the polarization controls the activity for photoelectrochemical water oxidation, a pathway to solar hydrogen fuel. Specifically, it is observed that the anodic water oxidation photocurrent increases from 0.99 to 2.22 mA cm −2 at 1.23 V RHE (60 mW cm −2 , UV illumination) or decreases to 0.50 mA cm −2 after electric polarization of hydrogen-annealed (111) SrTiO 3−x single crystals in forward or reverse direction. The polarization also modifies the surface photovoltage signal of the material and its flat band potential, based on Mott–Schottky measurements. These observations are attributed to the formation of an electric dipole at the (111) SrTiO 3−x surface, which alters the potential drop across the depletion layer at the solid–liquid junction, and with it the electron transfer barrier. Density functional theory calculations confirm that an electric dipole can result from the movement of oxygen vacancies between the surface or sub-surface layers of SrTiO 3−x . The filling of these surface oxygen vacancies is the probable cause for the observed disappearance of the electric polarization after 24 h storage in air and 48 h in argon. Overall, this work establishes a new surface-based ferroelectric effect in SrTiO 3−x and its use for solar energy conversion during photoelectrochemical water oxidation. Because oxygen vacancy defects are common, similar electric polarization effects are to be expected in other metal oxides.

Assavachin, Samutr [University of California, Davi↗

Tunable and Robust Optical and Structural Properties of a Cooperative Squaraine-Dye Aggregate-DNA DX-DAE Tile System

Molecular excitons, which are excitations delocalized over multiple dyes in a wavelike manner, are of interest for a wide range of applications, including quantum information science. Numerous studies have templated a variety of synthetic dyes via a DNA scaffold to induce dye aggregation to create molecular excitons upon photoexcitation. Dye aggregate optical properties are critically dependent on relative dye geometry and local environment; therefore, an understanding of dye-dye and DNA-dye interactions is critical for advancing toward more complex DNA-dye systems. The extensively studied DNA Holliday junction (HJ) and less-studied double-crossover (DX) tile motif are fundamental test beds for designing complex and ultimately modular DNA-dye architectures. Here, we report the first study of single-linked squaraine dye aggregation and exciton delocalization on a larger and more stable (compared with the HJ) DX tile motif. We first highlight a few DNA-dye constructs that support single dyes and aggregates with distinct optical properties that are both tunable—through sample design, buffer conditions, and heat treatment—and robust to environment changes, including transfer to solid phase. Next, we assess several experimental and design considerations that demonstrate directed dye-driven assembly of a novel double-tile DNA configuration. Our results demonstrate that single-linked squaraine dyes templated to DX tiles provide a viable research path to design and evaluate dye aggregate networks that support exciton delocalization. We include herein the first report of exciton delocalization in the solid phase in a DNA-dye construct. Additionally, our findings indicate that dye aggregation impacts the assembly of the DNA-dye construct, and, in some cases, thereby cooperates with the DNA to determine a final robust system configuration. Finally, we show that a controlled annealing schedule can be employed to promote the homogeneous assembly of DNA-dye constructs. The findings in this study contribute to the understanding of DNA-dye systems and the relevant factors involved in their directed assembly to achieve specific constructs with desirable properties.

36 MATERIALS SCIENCE↗

Photosynthesis of CO from CO 2 with an iron polypyridyl catalyst at a passivated silicon photoelectrode

A first-row transition metal catalyst, [Fe(tpy)(Mebim-py)(NCCH 3 )] 2+ (tpy = 2,2′:6′,2′′-terpyridine, Mebim-py = 1-methylbenzimidazol-2-ylidene-3-(2′-pyridine)) mediates CO 2 reduction to CO at passivated p-Si photoelectrodes with applied potentials 240 mV positive of the standard CO 2 /CO reduction potential. The molecular catalyst's selectivity for CO was retained under photoelectrochemical conditions, with negligible direct proton reduction promoted by the photoelectrode. The faradaic efficiency for CO (44 ± 6%) was slightly enhanced relative to the catalyst performance in the dark (33%). A photosynthetic cell based on this photocathode system, coupled with ferrocene oxidation at the anode, successfully operated at a cell voltage of −1.2 V. The photovoltage generated by illumination of p-Si–CH 3 met and surpassed the potential required for CO 2 reduction when coupled with ferrocene oxidation. By leveraging a low-overpotential CO 2 reduction electrocatalyst, a photo-assisted electrochemical efficiency of 0.15% and applied bias photon-to-current efficiency of 0.05% was achieved for this single-junction cell, ultimately storing 46 kJ mol −1 (11 kcal mol −1 ) of photon energy.

Carbon Dioxide Reduction↗

Single-event burnout in homojunction GaN vertical PiN diodes with hybrid edge termination design

GaN devices play a major role in modern electronics, providing high-power handling, efficient high-frequency operation, and resilience in harsh environments. However, electric field crowding at the edge of the anode often limits its full potential, leading to single-event effects (SEEs) at lower bias voltages under heavy ion radiation. Here, in this work, we report on the performance of homojunction GaN vertical PiN diodes with a hybrid edge termination design under heavy ion irradiation, specifically, oxygen ions, chlorine ions, Cf-252 fission fragments, and alpha particles from an Am-241 source. The unique hybrid edge termination (HET) design provides better electric field management, preventing breakdown from occurring at the edge of the anode at lower voltages. The results of this study reveal that these devices exhibit excellent tolerance to 12-MeV oxygen and 16-MeV chlorine ions, owing to their low linear energy transfer (LET) and range in GaN. However, single-event burnout (SEB) is observed during the Cf-252 exposure at about 50% of the diodes' electrical breakdown voltage due to the presence of higher LET and longer-range ions. Optical and scanning electron microscopy (SEM) reveal that the damage that caused by SEB lies close to the center of these devices rather than the anode edge. Devices with junction termination extension (JTE) instead of HET edge termination also show similar SEB when irradiated with Cf-252 fission fragments. Physical damage due to SEB occurs at the edge of the anode for these devices. These comparative results show the benefits of HET for enhancing the resistance of GaN-based PiN diodes to heavy ion irradiation.

42 ENGINEERING↗