We examine the DC and radio frequency (RF) response of superconducting transmission line resonators comprised of very thin NbTiN films, [Formula: see text] in thickness, in the high-temperature limit, where the photon energy is less than the thermal energy. The resonant frequencies of these superconducting resonators show a significant nonlinear response as a function of RF input power, which can approach a frequency shift of [Formula: see text] in a [Formula: see text] span in the thinnest film. The strong nonlinear response allows these very thin film resonators to serve as high kinetic inductance parametric amplifiers.
Capacitance-voltage ( {C} - {V} ) characteristics and carrier transport properties of 2-D electron gases (2DEGs) in an undoped Si/SiGe heterostructure at {T}= {4} - {35} K are presented. Two capacitance plateaus due to density saturation of the 2DEG in the buried Si quantum well (QW) are observed and explained by a model of surface tunneling. The peak mobility at 4 K is 4.1 \times 10^{{5}} cm2/ \text{V}\cdot \text{s} and enhanced by a factor of 1.97 at an even lower carrier density compared to the saturated carrier density, which is attributed to the effect of remote carrier screening. At {T}\,\,=35 K, the mobility enhancement with a factor of 1.35 is still observed, which suggests the surface tunneling is still dominant.
Defects in materials are an ongoing challenge for quantum bits, so called qubits. Solid state qubits—both spins in semiconductors and superconducting qubits—suffer from losses and noise caused by two-level-system (TLS) defects thought to reside on surfaces and in amorphous materials. Understanding and reducing the number of such defects is an ongoing challenge to the field. Superconducting resonators couple to TLS defects and provide a handle that can be used to better understand TLS. We develop noise measurements of superconducting resonators at very low temperatures (20 mK) compared to the resonant frequency, and low powers, down to single photon occupation.
We investigate the thermoelectric transport properties of the half-filled lowest Landau level v=1/2 in a gated two-dimensional hole system in a strained Ge/SiGe heterostructure. The electron-diffusion dominated regime is achieved below 600 mK, where the diffusion thermopower Sxxd at v=1/2 shows a linear temperature dependence. In contrast, the diffusion-dominated Nernst signal Sxyd of v=1/2 is found to approach zero, which is independent of the measurement configuration (sweeping magnetic field at a fixed hole density or sweeping the density by a gate at a fixed magnetic field).
Terahertz (THz) photoconductive devices are used for generation, detection, and modulation of THz waves, and they rely on the ability to switch electrical conductivity on a subpicosecond time scale using optical pulses. However, fast and efficient conductivity switching with high contrast has been a challenge, because the majority of photoexcited charge carriers in the switch do not contribute to the photocurrent due to fast recombination. Here, we improve efficiency of electrical conductivity switching using a network of electrically connected nanoscale GaAs resonators, which form a perfectly absorbing photoconductive metasurface. We achieve perfect absorption without incorporating metallic elements, by breaking the symmetry of cubic Mie resonators. As a result, the metasurface can be switched between conductive and resistive states with extremely high contrast using an unprecedentedly low level of optical excitation. We integrate this metasurface with a THz antenna to produce an efficient photoconductive THz detector. The perfectly absorbing photoconductive metasurface opens paths for developing a wide range of efficient optoelectronic devices, where required optical and electronic properties are achieved through nanostructuring the resonator network.
High-mobility two-dimensional (2D) holes residing in a Ge quantum well are a new electronic system with potentials in quantum computing and spintronics. Since for any electronic material, the effective mass and the g factor are two fundamental material parameters that determine the material response to electric and magnetic fields, measuring these two parameters in this material system is thus an important task that needs to be completed urgently. Because of the quantum confinement in the crystal growth direction (z), the biaxial strain of epitaxial Ge on SiGe, and the valance band nature, both the effective mass and the g factor can show very strong anisotropy. In particular, the in-plane g factor (gip) can be vanishingly small while the perpendicular g factor (gz) can be much larger than 2. Here we report the measurement of gip at very low hole densities using in-plane magneto-resistance measurement performed at the NHMFL.
Battery cycle life is directly influenced by the microstructural changes occurring in the electrodes during charge and discharge cycles. Here, we image in situ the nanoscale phase evolution in negative electrode materials for Li-ion batteries using a fully enclosed liquid cell in a transmission electron microscope (TEM) to reveal early degradation that is not evident in the charge-discharge curves. To compare the electrochemical phase transformation behavior between three model materials, thin films of amorphous Si, crystalline Al, and crystalline Au were lithiated and delithiated at controlled rates while immersed in a commercial liquid electrolyte. This method allowed for the direct observation of lithiation mechanisms in nanoscale negative electrodes, revealing that a simplistic model of a surface-to-interior lithiation front is insufficient. For the crystalline films, a lithiation front spread laterally from a few initial nucleation points, with continued grain nucleation along the growing interface. The intermediate lithiated phases were identified using electron diffraction, and high-resolution postmortem imaging revealed the details of the final microstructure. Our results show that electrochemically induced solid-solid phase transformations can lead to highly concentrated stresses at the laterally propagating phase boundary which should be considered for future designs of nanostructured electrodes for Li-ion batteries.
Demir, Muslum; Kahveci, Zafer; Aksoy, Burak; Palapati, Naveen K.R.; Subramanian, Arunkumar; Cullinan, Harry T.; El-Kaderi, Hani M.; Harris, Charles T.; Gupta, Ram B.
Lignin is a high-volume byproduct from the pulp and paper industry and is currently burned to generate electricity and process heat. The industry has been searching for high value-added uses of lignin to improve the process economics. In addition, battery manufacturers are seeking nonfossil sources of graphitic carbon for environmental sustainability. In this work, lignin (which is a cross-linked polymer of phenols, a component of biomass) is converted into graphitic porous carbon using a two-step conversion. Lignin is first carbonized in water at 300°C and 1500 psi to produce biochar, which is then graphitized using a metal nitrate catalyst at 900-1100°C in an inert gas at 15 psi. Graphitization effectiveness of three different catalysts - iron, cobalt, and manganese nitrates - is examined. The product is analyzed for morphology, thermal stability, surface properties, and electrical conductivity. Both temperature and catalyst type influenced the degree of graphitization. A good quality graphitic carbon was obtained using catalysis by Mn(NO3)2 at 900°C and Co(NO3)2 at 1100°C.
Three-dimensional (3D) network structure has been envisioned as a superior architecture for lithium ion battery (LIB) electrodes, which enhances both ion and electron transport to significantly improve battery performance. Herein, a 3D carbon nano-network is fabricated through chemical vapor deposition of carbon on a scalably manufactured 3D porous anodic alumina (PAA) template. As a demonstration on the applicability of 3D carbon nano-network for LIB electrodes, the low conductivity active material, TiO2, is then uniformly coated on the 3D carbon nano-network using atomic layer deposition. High power performance is demonstrated in the 3D C/TiO2 electrodes, where the parallel tubes and gaps in the 3D carbon nano-network facilitates fast Li ion transport. A large areal capacity of ~0.37mAh·cm-2 is achieved due to the large TiO2 mass loading in the 60μm-thick 3D C/TiO2 electrodes. At a test rate of C/5, the 3D C/TiO2 electrode with 18nm-thick TiO2 delivers a high gravimetric capacity of ~240mAhg-1, calculated with the mass of the whole electrode. A long cycle life of over 1000 cycles with a capacity retention of 91% is demonstrated at 1C. The effects of the electrical conductivity of carbon nano-network, ion diffusion, and the electrolyte permeability on the rate performance of these 3D C/TiO2 electrodes are systematically studied.
This report documents work that was performed under the Laboratory Directed Research and Development project, Science of Battery Degradation. The focus of this work was on the creation of new experimental and theoretical approaches to understand atomistic mechanisms of degradation in battery electrodes that result in loss of electrical energy storage capacity. Several unique approaches were developed during the course of the project, including the invention of a technique based on ultramicrotoming to cross-section commercial scale battery electrodes, the demonstration of scanning transmission x-ray microscopy (STXM) to probe lithium transport mechanisms within Li-ion battery electrodes, the creation of in-situ liquid cells to observe electrochemical reactions in real-time using both transmission electron microscopy (TEM) and STXM, the creation of an in-situ optical cell utilizing Raman spectroscopy and the application of the cell for analyzing redox flow batteries, the invention of an approach for performing ab initio simulation of electrochemical reactions under potential control and its application for the study of electrolyte degradation, and the development of an electrochemical entropy technique combined with x-ray based structural measurements for understanding origins of battery degradation. These approaches led to a number of scientific discoveries. Using STXM we learned that lithium iron phosphate battery cathodes display unexpected behavior during lithiation wherein lithium transport is controlled by nucleation of a lithiated phase, leading to high heterogeneity in lithium content at each particle and a surprising invariance of local current density with the overall electrode charging current. We discovered using in-situ transmission electron microscopy that there is a size limit to lithiation of silicon anode particles above which particle fracture controls electrode degradation. From electrochemical entropy measurements, we discovered that entropy changes little with degradation but the origin of degradation in cathodes is kinetic in nature, i.e. lower rate cycling recovers lost capacity. Finally, our modeling of electrode-electrolyte interfaces revealed that electrolyte degradation may occur by either a single or double electron transfer process depending on thickness of the solid-electrolyte-interphase layer, and this cross-over can be modeled and predicted.
We present the results of a three year LDRD project that focused on understanding the impact of defects on the electrical, optical and thermal properties of GaN-based nanowires (NWs). We describe the development and application of a host of experimental techniques to quantify and understand the physics of defects and thermal transport in GaN NWs. We also present the development of analytical models and computational studies of thermal conductivity in GaN NWs. Finally, we present an atomistic model for GaN NW electrical breakdown supported with experimental evidence. GaN-based nanowires are attractive for applications requiring compact, high-current density devices such as ultraviolet laser arrays. Understanding GaN nanowire failure at high-current density is crucial to developing nanowire (NW) devices. Nanowire device failure is likely more complex than thin film due to the prominence of surface effects and enhanced interaction among point defects. Understanding the impact of surfaces and point defects on nanowire thermal and electrical transport is the first step toward rational control and mitigation of device failure mechanisms. However, investigating defects in GaN NWs is extremely challenging because conventional defect spectroscopy techniques are unsuitable for wide-bandgap nanostructures. To understand NW breakdown, the influence of pre-existing and emergent defects during high current stress on NW properties will be investigated. Acute sensitivity of NW thermal conductivity to point-defect density is expected due to the lack of threading dislocation (TD) gettering sites, and enhanced phonon-surface scattering further inhibits thermal transport. Excess defect creation during Joule heating could further degrade thermal conductivity, producing a viscous cycle culminating in catastrophic breakdown. To investigate these issues, a unique combination of electron microscopy, scanning luminescence and photoconductivity implemented at the nanoscale will be used in concert with sophisticated molecular-dynamics calculations of surface and defect-mediated NW thermal transport. This proposal seeks to elucidate long standing material science questions for GaN while addressing issues critical to realizing reliable GaN NW devices.