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DOE OSTI2024

High mass loading potassium ion stabilized manganese dioxide nanowire forests for rechargeable Zn batteries

Manganese dioxide (MnO 2 ) represents an ideal cathode material for rechargeable aqueous Zn batteries due to its high theoretical capacity (308 mAh g -1 ), suitable potential (1.4 V vs. Zn 2+ /Zn), natural abundance, and negligible toxicity. However, the capacity and rate capability of MnO 2 deteriorate significantly in thick electrodes owing to its low electrical and ionic conductivities. Herein, we report the design of high mass loading potassium ion stabilized α-MnO 2 (K 0.133 MnO 2 ) nanowire forests on carbon cloth through a seed-assisted hydrothermal method for Zn batteries. Further, the vertically aligned K 0.133 MnO 2 nanowire forests with uninterrupted charge transport afford a high area capacity of 3.54 mAh cm -2 and a capacity retention of 79.2% over 1000 cycles in aqueous electrolyte. Moreover, the high area capacity and cyclability can be readily transferred to quasi-solid-state devices.

25 ENERGY STORAGE↗

DOE OSTI2022

A review of zirconia oxygen, NO x , and mixed potential gas sensors – History and current trends

Zirconia-based electrochemical sensors have revolutionized oxygen monitoring and combustion control. Here, these robust, solid-state devices are found in virtually every internal combustion engine today providing feedback information for tight air to fuel ratio control thus minimizing unwanted emissions and improving engine efficiency. Variations on the sensor design and operational mode enable the measurement of nitrogen oxides to part per million levels, providing control information for exhaust after-treatment systems. Emerging designs include the development of "gas analyzers on a chip" capable of monitoring oxygen, carbon monoxide, nitrogen oxides, ammonia and hydrocarbons.

47 OTHER INSTRUMENTATION↗

DOE OSTI2017

Programmable Colloidal Approach to Hierarchical Structures of Methylammonium Lead Bromide Perovskite Nanocrystals with Bright Photoluminescent Properties

Here, systematic tailoring of nanocrystal architecture could provide unprecedented control over their electronic, photophysical, and charge transport properties for a variety of applications. However, at present, manipulation of the shape of perovskite nanocrystals is done mostly by trial-and-error-based experimental approaches. Here, we report systematic colloidal synthetic strategies to prepare methylammonium lead bromide quantum platelets and quantum cubes. In order to control the nucleation and growth processes of these nano crystals, we appropriately manipulate the solvent system, surface ligand chemistry, and reaction temperature causing syntheses into anisotropic shapes. We demonstrate that both the presence of chlorinated solvent and a long chain aliphatic amine in the reaction mixture are crucial for the formation of ultrathin quantum platelets (similar to 1.5 nm in thickness), which is driven by mesoscale-assisted growth of spherical seed nanocrystals (similar to 1.6 nm in diameter) through attachment of monomers onto selective crystal facets. A combined surface and structural characterization, along with small-angle X-ray scattering analysis, confirm that the long hydrocarbon of the aliphatic amine is responsible for the well ordered hierarchical stacking of the quantum platelets of 3.5 nm separation. In contrast, the formation of similar to 12 nm edge-length quantum cubes is a kinetically driven process in which a high flux of monomers is achieved by supplying thermal energy. The photoluminescence quantum yield of our quantum platelets (similar to 52%) is nearly 2-fold higher than quantum cubes. Moreover, the quantum platelets display a lower nonradiative rate constant than that found with quantum cubes, which suggests less surface trap states. Together, our research has the potential both to improve the design of synthetic methods for programmable control of shape and assembly and to provide insight into optoelectronic properties of these materials for solid-state device fabrication, e.g., light-emitting diodes, solar cells, and lasing materials.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Dehydrogenation vs Apparent Hydrogenation: Unraveling the Mechanisms of He and O 2 Plasma Etching on Colloidal Nanocrystal Films

Removing organic ligands from colloidal nanoparticles is critical for fabricating solid-state devices, yet accurately quantifying this removal remains a significant analytical challenge. Here, we establish a robust and accessible method for this quantification by calibrating Raman spectroscopy against precise ion beam analysis (IBA) for nanoparticle assemblies (CNAs) processed by helium (He) and oxygen (O 2 ) plasmas. We demonstrate that the calibration curves are remarkably independent of plasma power and pressure, depending critically only on the choice of feed gas. He plasma induces rapid dehydrogenation and cross-linking, evidenced by a much faster decrease in the C–H Raman signal relative to the actual carbon loss. Conversely, O 2 plasma leads to a surprising “apparent hydrogenation”, where the carbon backbone is removed significantly faster than the C–H signal diminishes. This counterintuitive effect is explained by a serial mechanism of oxidative fragmentation; β-scission cleaves the alkyl chains, and subsequent stabilization steps enrich the remaining film with hydrogen-rich methyl-terminated fragments, while carbon is efficiently removed as volatile CO. This work provides calibrated functions that enable the rapid determination of absolute carbon content in processed CNAs using simple Raman spectroscopy with uncertainties of ∼8% for O 2 and ∼12% for He plasma, offering a vital tool for both process diagnostics and fundamental studies of plasma–matter interactions in colloidal nanocrystal films.

Animal feed↗

DOE OSTI2011

Effect of Concentration on the Energetics and Dynamics of Li Ion Transport in Anatase and Amorphous TiO2

We report on the energetics and dynamics of Li diffusion in bulk anatase and amorphous TiO2 using molecular dynamics (MD) simulations and density functional theory (DFT) calculations. Using MD simulations, for both anatase and amorphous TiO2, diffusion characteristics are first studied for an isolated Li ion, followed by simulations of Li concentrations ranging from 10% to 100% in order to explore the concentration effect on the diffusivity. The isolated Li diffusion mechanism, revealed from the MD simulations, occurs via zigzag hops between the octahedral sites in anatase. The corresponding barrier for this process obtained fromDFT-NEB calculations is 480 meV.MDsimulations also show that isolated Li ion diffusivity is much slower in the amorphous TiO2 than in anatase TiO2. DFT-NEB results for the diffusion in amorphous titania indicate that Li encounters deep energy wells within the amorphous network that are in the electronvolt range, confirming our MD observation of low Li diffusivity. A monotonic decrease in diffusion barriers with increasing Li concentration is observed in the case of amorphous titania whereas a non-monotonic variation is seen in anatase, with the lowest barrier observed at 50% Li concentration. At low Li concentrations (<50%), we find that the barriers in anatase are lower than in amorphous titania. However, at the maximum Li intercalation ratios, which are experimentally known to be 50% for anatase and >75% for amorphous titania, the Li diffusivity in amorphous is found to be much higher than in anatase. Our MD simulations suggest that the underlying reason for these differences is related to changes in diffusion mechanism. Our simulations therefore indicate a strong correlation between Li ion concentration and the observed transport characteristics, offering new insights into ion conduction mechanisms that are of importance to solid-state devices used for energy storage applications.

Environmental Molecular Sciences Laboratory↗

DOE OSTI2015

Restricted Photochemistry in the Molecular Solid State: Structural Changes on Photoexcitation of Cu(I) Phenanthroline Metal-to-Ligand Charge Transfer (MLCT) Complexes by Time-Resolved Diffraction

The excited-state structure of Cu{sup I}[(1,10-phenanthroline-N,N') bis(triphenylphosphine)] cations in their crystalline [BF{sub 4}] salt has been determined at both 180 and 90 K by single-pulse time-resolved synchrotron experiments with the modified polychromatic Laue method. The two independent molecules in the crystal show distortions on MLCT excitation that differ in magnitude and direction, a difference attributed to a pronounced difference in the molecular environment of the two complexes. As the excited states differ, the decay of the emission is biexponential with two strongly different lifetimes, the longer lifetime, assigned to the more restricted molecule, becoming more prevalent as the temperature increases. Standard deviations in the current Laue study are very much lower than those achieved in a previous monochromatic study of a Cu(I) 2,9-dimethylphenanthroline substituted complex (J. Am. Chem. Soc. 2009, 131, 6566), but the magnitudes of the shifts on excitation are similar, indicating that lattice restrictions dominate over the steric effect of the methyl substitution. Above all, the study illustrates emphatically that molecules in solids have physical properties different from those of isolated molecules and that their properties depend on the specific molecular environment. This conclusion is relevant for the understanding of the properties of molecular solid-state devices, which are increasingly used in current technology.

Makal, Anna↗

DOE OSTI2012

Decoherence-protected quantum gates for a hybrid solid-state spin register

Protecting the dynamics of coupled quantum systems from decoherence by the environment is a key challenge for solid-state quantum information processing. An idle quantum bit (qubit) can be efficiently insulated from the outside world by dynamical decoupling, as has recently been demonstrated for individual solid-state qubits. However, protecting qubit coherence during a multi-qubit gate is a non-trivial problem in general, the decoupling disrupts the interqubit dynamics and hence conflicts with gate operation. This problem is particularly salient for hybrid systems, in which different types of qubit evolve and decohere at very different rates. Here we present the integration of dynamical decoupling into quantum gates for a standard hybrid system, the electron-nuclear spin register. Our design harnesses the internal resonance in the coupled-spin system to resolve the conflict between gate operation and decoupling. We experimentally demonstrate these gates using a two-qubit register in diamond operating at room temperature. Quantum tomography reveals that the qubits involved in the gate operation are protected as accurately as idle qubits. We also perform Grover's quantum search algorithm, and achieve fidelities of more than 90% even though the algorithm run-time exceeds the electron spin dephasing time by two orders of magnitude. Our results directly allow decoherence-protected interface gates between different types of solid-state qubit. Ultimately, quantum gates with integrated decoupling may reach the accuracy threshold for fault-tolerant quantum information processing with solid-state devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

A chiral molecular propeller designed for unidirectional rotations on a surface

Abstract Synthetic molecular machines designed to operate on materials surfaces can convert energy into motion and they may be useful to incorporate into solid state devices. Here, we develop and characterize a multi-component molecular propeller that enables unidirectional rotations on a material surface when energized. Our propeller is composed of a rotator with three molecular blades linked via a ruthenium atom to a ratchet-shaped molecular gear. Upon adsorption on a gold crystal surface, the two dimensional nature of the surface breaks the symmetry and left or right tilting of the molecular gear-teeth induces chirality. The molecular gear dictates the rotational direction of the propellers and step-wise rotations can be induced by applying an electric field or using inelastic tunneling electrons from a scanning tunneling microscope tip. By means of scanning tunneling microscope manipulation and imaging, the rotation steps of individual molecular propellers are directly visualized, which confirms the unidirectional rotations of both left and right handed molecular propellers into clockwise and anticlockwise directions respectively.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Hydrogen-induced tunable remanent polarization in a perovskite nickelate

Materials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO 3 into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors. The space-charge polarization caused by long-range movement and trapping of protons dominates when the electric field exceeds the threshold value. First-principles calculations suggest the polarization originates from the polar structure created by H doping. We find that polarization decays within ~1 second which is an interesting temporal regime for neuromorphic computing hardware design, and we implement the transient characteristics in a neural network to demonstrate unsupervised learning. These discoveries open new avenues for designing ferroelectric materials and electrets using light-ion doping.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Adiabatic two-qubit gates in capacitively coupled quantum dot hybrid qubits

Abstract The ability to tune qubits to flat points in their energy dispersions (“sweet spots”) is an important tool for mitigating the effects of charge noise and dephasing in solid-state devices. However, the number of derivatives that must be simultaneously set to zero grows exponentially with the number of coupled qubits, making the task untenable for as few as two qubits. This is a particular problem for adiabatic gates, due to their slower speeds. Here, we propose an adiabatic two-qubit gate for quantum dot hybrid qubits, based on the tunable, electrostatic coupling between distinct charge configurations. We confirm the absence of a conventional sweet spot, but show that controlled-Z (CZ) gates can nonetheless be optimized to have fidelities of ~99% for a typical level of quasistatic charge noise ( σ ε ≃ 1 μeV). We then develop the concept of a dynamical sweet spot (DSS), for which the time-averaged energy derivatives are set to zero, and identify a simple pulse sequence that achieves an approximate DSS for a CZ gate, with a 5× improvement in the fidelity. We observe that the results depend on the number of tunable parameters in the pulse sequence, and speculate that a more elaborate sequence could potentially attain a true DSS.

Frees, Adam (ORCID:0000000324711096)↗

DOE OSTI2023

Remarkable heat conduction mediated by non-equilibrium phonon polaritons

Surface waves can lead to intriguing transport phenomena. In particular, surface phonon polaritons (SPhPs), which result from coupling between infrared light and optical phonons, have been predicted to contribute to heat conduction along polar thin films and nanowires. However, experimental efforts so far suggest only very limited SPhP contributions. Through systematic measurements of thermal transport along the same 3C-SiC nanowires with and without a gold coating on the end(s) that serves to launch SPhPs, here we show that thermally excited SPhPs can substantially enhance the thermal conductivity of the uncoated portion of these wires. The extracted pre-decay SPhP thermal conductance is more than two orders of magnitude higher than the Landauer limit predicted on the basis of equilibrium Bose–Einstein distributions. Here, we attribute the notable SPhP conductance to the efficient launching of non-equilibrium SPhPs from the gold-coated portion into the uncoated SiC nanowires, which is strongly supported by the observation that the SPhP-mediated thermal conductivity is proportional to the length of the gold coating(s). The reported discoveries open the door for modulating energy transport in solids by introducing SPhPs, which can effectively counteract the classical size effect in many technologically important films and improve the design of solid-state devices.

42 ENGINEERING↗

DOE OSTI2013

Ion irradiation synthesis of Ag–Au bimetallic nanospheroids in SiO{sub 2} glass substrate with tunable surface plasmon resonance frequency

Ag–Au bimetallic nanospheroids with tunable localized surface plasmon resonance (LSPR) were synthesized by 100 keV Ar–ion irradiation of 30 nm Ag–Au bimetallic films deposited on SiO{sub 2} glass substrates. A shift of the LSPR peaks toward shorter wavelengths was observed up to an irradiation fluence of 1.0 × 10{sup 17} cm{sup −2}, and then shifted toward the longer wavelength because of the increase of fragment volume under ion irradiation. Further control of LSPR frequency over a wider range was realized by modifying the chemical components. The resulting LSPR frequencies lie between that of the pure components, and an approximate linear shift of the LSPR toward the longer wavelength with the Au concentration was achieved, which is in good agreement with the theoretical calculations based on Gans theory. In addition, the surface morphology and compositions were examined with a scanning electron microscope equipped with an energy dispersive spectrometer, and microstructural characterizations were performed using a transmission electron microscope. The formation of isolated photosensitive Ag–Au nanospheroids with a FCC structure partially embedded in the SiO{sub 2} substrate was confirmed, which has a potential application in solid-state devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2014

Optical detection of spin-filter effect for electron spin polarimetry

We have monitored the cathodoluminescence (CL) emitted upon injection of free electrons into a hybrid structure consisting of a thin magnetic Fe layer deposited on a p-GaAs substrate, in which InGaAs quantum wells are embedded. Electrons transmitted through the unbiased metal/semiconductor junction recombine radiatively in the quantum wells. Because of the electron spin-filtering across the Fe/GaAs structure, the CL intensity, collected from the backside, is found to depend on the relative orientation between the injected electronic spin polarization and the Fe layer magnetization. The spin asymmetry of the CL intensity in such junction provides a compact optical method for measuring spin polarization of free electrons beams or of hot electrons in solid-state devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Millimeter wave traveling wave tubes for the 21st Century

Traveling wave tubes are rapidly evolving to provide unprecedented power level in comparison to solid state devices in the millimeter waves region of the spectrum (80–300 GHz) thus enabling a wide range of applications. Wireless communications, imaging, plasma diagnostics, healthcare and many others will gain substantial features if high power at millimeter waves would be available from compact sources. The development of fabrication technologies is proving crucial for introducing new topologies and structures for millimeter wave vacuum electronic devices, compatible with the dimensions dictated by the short wavelength that poses substantial manufacturing challenges due to tight tolerances. This review paper will provide an overview of the principles, evolution and state of the art of one of the most widely utilized vacuum electronic device, the traveling wave tube (TWT). The wide band, high gain features of TWTs make those devices the most promising solutions for high power at millimeter waves and THz frequencies.

42 ENGINEERING↗

DOE OSTI2020

Selective acoustic control of photon-mediated qubit-qubit interactions

Quantum technologies such as quantum sensing, quantum imaging, quantum communications, and quantum computing rely on the ability to actively manipulate the quantum state of light and matter. Quantum emitters, such as color centers trapped in solids, are a useful platform for the realization of elementary building blocks (qubits) of quantum information systems. In particular, the modular nature of such solid-state devices opens up the possibility to connect them into quantum networks and create nonclassical states of light shared among many qubits. The function of a quantum network relies on efficient and controllable interactions among individual qubits. In this context, we present a scheme where optically active qubits of differing excitation energies are mutually coupled via a dispersive interaction with a shared mode of an optical cavity. This generally off-resonant interaction is prohibitive of direct exchange of information among the qubits. However, we propose a scheme in which by acoustically modulating the qubit excitation energies it is, in fact, possible to tune to resonance a preselected pair of qubits and thus open a communication channel between them. This method potentially enables fast (approximately nanoseconds) and parallelizable on-demand control of a large number of physical qubits. In this work, we develop an analytical and a numerical theoretical model demonstrating this principle and suggest feasible experimental scenarios to test the theoretical predictions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

A Low-Power and In Situ Annealing Mitigation Technique for Fast Neutrons Irradiation of Integrated Temperature Sensing Diodes

High doses of fast neutrons is detrimental to the performance of most common solid-state devices such as diodes and transistors. The ionizing effect is observed in particular for diodes used as simple integrated temperature sensors, or thermo-diodes, when their junction voltage is measured at constant current bias. In this work, we present a low-power and in situ mitigation technique based on Silicon-on-Insulator (SOI) micro-hot-plates to recover thermo-diodes. The basic operating principle consists in annealing the temperature-sensitive diodes integrated on the membrane during or after their irradiation in order to restore similar sensing characteristics over time. We measured thermo-diodes integrated to micro-hot-plates during their irradiation by fast neutrons (23 MeV peak) with total doses about 2.97±0.08 kGy. The membrane annealing is taking place at 450 deg. C using 40 mW of electrical power. Thanks to the annealing, the diode keeps a total measurement error below 0.5 deg. C. In this harsh radiation environment and beside the good tolerance of the thermo-diodes and the membrane materials to the total ionizing dose, the thermo-diode located on the heating membrane keeps a constant sensitivity. The demonstrated resistance of micro-hot-plates and the integrated thermo-diodes to fast neutron radiations can extend their use in nuclear plants and for radiation detectors. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

Chameleon: An Adaptive Wear Balancer for Flash Clusters

NAND flash-based Solid State Devices (SSDs) offer the desirable features of high performance, energy efficiency, and fast growing capacity. Thus, the use of SSDs is increasing in distributed storage systems. A key obstacle in this context is that the natural unbalance in distributed I/O workloads can result in wear imbalance across the SSDs in a distributed setting. This, in turn can have significant impact on the reliability, performance, and lifetime of the storage deployment. Extant load balancers for storage systems do not consider SSD wear imbalance when placing data, as the main design goal of such balancers is to extract higher performance. Consequently, data migration is the only common technique for tackling wear imbalance, where existing data is moved from highly loaded servers to the least loaded ones. In this paper, we explore an innovative holistic approach, Chameleon, that employs data redundancy techniques such as replication and erasure-coding, coupled with endurance-aware write offloading, to mitigate wear level imbalance in distributed SSD-based storage. Chameleon aims to balance the wear among different flash servers while meeting desirable objectives of: extending life of flash servers; improving I/O performance; and avoiding bottlenecks. Evaluation with a 50 node SSD cluster shows that Chameleon reduces the wear distribution deviation by 81% while improving the write performance by up to 33%.

Zhao, Nannan↗

DOE OSTI2025

Dopant Optimization of Donors in Semiconductor Opening Switches to Eliminate Prepulse

Semiconductor opening switches are solid-state devices capable of delivering nanosecond, hundreds of kilovolts pulses by interrupting kiloamps of current. The interruption of the current occurs in a moderately doped p-region when a high electric field region (HFR) is formed. The HFR occurs because the reverse pumping current cannot be supported by the saturation velocity and majority carrier concentration of the doping level. However, the donor profile also significantly affects the pulse performance. A secondary prepulse occurs if a secondary HFR is formed at the interface of the background n-doping and N+ doping (X n ) . By moving the location of X n deeper into the diode, the effect of the prepulse is reduced. This article investigates the effect of the donor doping profile on the performance metrics of semiconductor opening switches through technology computer-aided design (TCAD) simulations and experimental results. Through a SILVACO TCAD optimization, we designed a P + /p/n - base/n/N + where the intersection of the moderate p-region and intrinsic n-base region (X p ) is at 160 μm and X n is at 220 μm. This profile is fabricated via silicon epitaxy. Experimentally, it is shown that a deep X n (220 μm) compared with a shallow X n (300 μm) reduces the rise time by >5× . In addition, the magnitude of current density during interruption affects the prepulse foot and pulse shape. At lower current densities without the graded donor profile, high peak voltages are not achieved. Comparing the experimental results to the TCAD simulations shows that the model is predictive under high-current densities in the semiconductor opening switch (SOS) regime.

nanosecond pulse power↗