Publications

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We demonstrate an InAs-based terahertz (THz) metasurface emitter that can generate and focus THz pulses using a binary-phase Fresnel zone plate concept. The metalens emitter successfully generates a focused THz beam without additional THz optics.

Superconducting qubits have reached the point where system designers are worried about the heat that control wiring brings into the cryostat. To continue scaling cryogenic quantum systems, control solutions that work inside the cold space must be explored. One possibility is to use control electronics that is native to superconductivity, so called single-flux-quantum (SFQ) circuitry, to form an interface between qubits and whatever other electronics is needed to control eventual quantum systems. To begin exploring the utility of SFQ as control circuitry, we performed modeling and experiments on qubit readout using ballistic fluxons which are SFQ in the limit of ballistic fluxon transport. Our modeling results show that a flavor of qubit, the fluxonium, can be read out using ballistic fluxons. We designed test samples to prove some of the key concepts needed for such a readout but were ultimately unable to getting a working demonstration. The lack of testing success was due to challenges in fabrication and running short of time to perform testing rather than a fundamental problem with our analysis.

While radiation is known to degrade AlGaN/GaN high-electron-mobility transistors (HEMTs), the question remains on the extent of damage governed by the presence of an electrical field in the device. In this study, we induced displacement damage in HEMTs in both ON and OFF states by irradiating with 2.8 MeV Au4+ ion to fluence levels ranging from 1.72 × 10 10 to 3.745 × 10 13 ions cm−2, or 0.001-2 displacement per atom (dpa). Electrical measurement is done in situ, and high-resolution transmission electron microscopy (HRTEM), energy dispersive x-ray (EDX), geometrical phase analysis (GPA), and micro-Raman are performed on the highest fluence of Au4+ irradiated devices. The selected heavy ion irradiation causes cascade damage in the passivation, AlGaN, and GaN layers and at all associated interfaces. After just 0.1 dpa, the current density in the ON-mode device deteriorates by two orders of magnitude, whereas the OFF-mode device totally ceases to operate. Moreover, six orders of magnitude increase in leakage current and loss of gate control over the 2-dimensional electron gas channel are observed. GPA and Raman analysis reveal strain relaxation after a 2 dpa damage level in devices. Significant defects and intermixing of atoms near AlGaN/GaN interfaces and GaN layer are found from HRTEM and EDX analyses, which can substantially alter device characteristics and result in complete failure.

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We demonstrate an InAs-based nonlinear dielectric metasurface, which can generate terahertz (THz) pulses with opposite phase in comparison to an unpatterned InAs layer. It enables binary phase THz metasurfaces for generation and focusing of THz pulses.

Aperture near-field microscopy and spectroscopy (a-SNOM) enables the direct experimental investigation of subwavelength-sized resonators by sampling highly confined local evanescent fields on the sample surface. Despite its success, the versatility and applicability of a-SNOM is limited by the sensitivity of the aperture probe, as well as the power and versatility of THz sources used to excite samples. Recently, perfectly absorbing photoconductive metasurfaces have been integrated into THz photoconductive antenna detectors, enhancing their efficiency and enabling high signal-to-noise ratio THz detection at significantly reduced optical pump powers. Here, we discuss how this technology can be applied to aperture near-field probes to improve both the sensitivity and potentially spatial resolution of a-SNOM systems. In addition, we explore the application of photoconductive metasurfaces also as near-field THz sources, providing the possibility of tailoring the beam profile, polarity and phase of THz excitation. Photoconductive metasurfaces therefore have the potential to broaden the application scope of aperture near-field microscopy to samples and material systems which currently require improved spatial resolution, signal-to-noise ratio, or more complex excitation conditions.

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Thin film platinum resistive thermometers are conventionally applied for resistance thermometry techniques due to their stability and proven measurement accuracy. Depending upon the required thermometer thickness and temperature measurement, however, performance benefits can be realized through the application of alternative nanometallic thin films. Herein, a comparative experimental analysis is provided on the performance of nanometallic thin film thermometers most relevant to microelectronics and thermal sensing applications: Al, Au, Cu, and Pt. Sensitivity is assessed through the temperature coefficient of resistance, measured over a range of 10-300 K for thicknesses nominally spanning 25-200 nm. The interplay of electron scattering sources, which give rise to the temperature-dependent TCR properties for each metal, are analyzed in the framework of a Mayadas-Shatzkes based model. Despite the prevalence of evaporated Pt thin film thermometers, Au and Cu films fabricated in a similar manner may provide enhanced sensitivity depending upon thickness. These results may serve as a guide as the movement toward smaller measurement platforms necessitates the use of smaller, thinner metallic resistance thermometers.

We examine the DC and radio frequency (RF) response of superconducting transmission line resonators comprised of very thin NbTiN films, < 12 nm 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 Δ f = - 0.15 % in a - 20 dB span in the thinnest film. The strong nonlinear response allows these very thin film resonators to serve as high kinetic inductance parametric amplifiers.

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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.

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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.

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Despite their wide use in terahertz (THz) research and technology, the application spectra of photoconductive antenna (PCA) THz detectors are severely limited due to the relatively high optical gating power requirement. This originates from poor conversion efficiency of optical gate beam photons to photocurrent in materials with subpicosecond carrier lifetimes. Here we show that using an ultra-thin (160 nm), perfectly absorbing low-temperature grown GaAs metasurface as the photoconductive channel drastically improves the efficiency of THz PCA detectors. This is achieved through perfect absorption of the gate beam in a significantly reduced photoconductive volume, enabled by the metasurface. This Letter demonstrates that sensitive THz PCA detection is possible using optical gate powers as low as 5 μW-three orders of magnitude lower than gating powers used for conventionalPCAdetectors.We show that significantly higher optical gate powers are not necessary for optimal operation, as they do not improve the sensitivity to the THz field. This class of efficient PCA THz detectors opens doors for THz applications with low gate power requirements.

A demonstration of 2D hole gases in GeSn/Ge heterostructures with a mobility as high as 20 000 cm² V^–1 s^–1 is given. Both the Shubnikov–de Haas oscillations and integer quantum Hall effect are observed, indicating high sample quality. The Rashba spin-orbit coupling (SOC) is investigated via magneto-transport. Further, a transition from weak localization to weak anti-localization is observed, which shows the tunability of the SOC strength by gating. The magneto-transport data are fitted to the Hikami–Larkin–Nagaoka formula. The phase-coherence and spin-relaxation times, as well as spin-splitting energy and Rashba coefficient of the k-cubic term, are extracted. Furthermore, the analysis reveals that the effects of strain and confinement potential at a high fraction of Sn suppress the Rashba SOC caused by the GeSn/Ge heterostructures.

Modulation doping is a commonly adopted technique to create two-dimensional (2D) electrons or holes in semiconductor heterostructures. One constraint, however, is that the intentional dopants required for modulation doping are controlled and incorporated during the growth of heterostructures. Using undoped strained germanium quantum wells as the model material system, we show, in this work, that modulation doping can be achieved post-growth of heterostructures by ion implantation and dopant-activation anneals. The carrier density is controlled ex situ by varying the ion fluence and implant energy, and an empirical calibration curve is obtained. While the mobility of the resulting 2D holes is lower than that in undoped heterostructure field-effect transistors built using the same material, the achievable carrier density is significantly higher. Potential applications of this modulation-doping technique are discussed.

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Coherent manipulation of quantum states is at the core of quantum information science (QIS). Many state-of-the-art quantum systems rely on microwave fields for quantum operations. As such, the microwave electromagnetic fields serve as the ideal "quantum bus" to integrate different types of QIS systems into a hybrid quantum system. Superconducting metamaterials are artificial materials consisting of arrays of superconducting resonant microstructures with sizes much smaller than the microwave wavelengths of interest. Superconducting metamaterials are a strong candidate medium for the microwave quantum bus, because the effective impedance, field distributions, and frequency response can all be controlled by engineering the microstructures, electrical bias, and magnetic flux while maintaining extremely low loss. In this project, we investigate the fundamental unit of a superconducting metamaterial - a resonator with physical dimensions much smaller than the microwave wavelengths - using NbTiN as the working superconductor, whose high operating temperatures and magnetic fields are desirable attributes for compatibility with a wide variety of quantum systems. We first studied the properties of sputtered NbTiN thin films by correlating the film thickness with the normal state resistivity, superconducting transition temperature, and resonances of transmission line resonators made from these films. We developed a process flow and designed a coplanar waveguide platform for studying small resonators. The platform significantly shortens the turnaround times of the resonator fabrication and testing cycles. Several resonators with different designs were fabricated and tested at 4 Kelvin. Resonances were observed in some resonator testers. Potential paths for improvements and future directions are discussed.

Superconducting quantum interference devices (SQUIDs) are extraordinarily sensitive to magnetic flux and thus make excellent current amplifiers for cryogenic applications. One such application of high interest to Sandia is the set-up and state read-out of quantum dot based qubits, where a qubit state is read out from a short current pulse (microseconds to milliseconds long) of approximately 100 pA, a signal that is easily corrupted by noise in the environment. A Parametric SQUID Amplifier can be high bandwidth (in the GHz range), low power dissipation (less than 1pW), and can be easily incorporated into multi-qubit systems. In this SAIL LDRD, we will characterize the noise performance of the parametric amplifier front end -- the SQUID -- in an architecture specific to current readout for spin qubits. Noise is a key metric in amplification, and identifying noise sources will allow us to optimize the system to reduce its effects, resulting in higher fidelity readout. This effort represents a critical step in creating the building blocks of a high speed, low power, parametric SQUID current amplifier that will be needed in the near term as quantum systems with many qubits begin to come on line in the next few years.

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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).

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Here we present the development of the building blocks of a Josephson parametric amplifier (JPA), namely the superconducting quantum interference device (SQUID) and the inductive pick-up coil that permits current coupling from a quantum dot into the SQUID. We also discuss our efforts in making depletion mode quantum dots using delta doped GaAs quantum wells. Because quantum dot based spin qubits utilize very low-level (~10 - 100pA), short duration (1ms - 1μs) current signals for state preparation and readout, these systems require close proximity cryogenic amplification to prevent signal corruption. Common amplification methods in these semiconductor quantum dots rely on heterojunction bipolar transistors (HBTs) and high electron mobility transistors (HEMTs) to amplify the readout signal from a single qubit. The state of the art for HBTs and HEMTs produce approximately 10µW of power when operating at high bandwidths. For few-qubit systems this level of heat dissipation is acceptable. However, for scaling up the number of qubits to several hundred or a thousand, the heat load produced in a 1 to 1 amplifier to qubit arrangement would overload the cooling capacity of a common dilution refrigerator, which typically has a cooling power of ~100µW at its base temperature. Josephson parametric amplifiers have been shown to dissipate ~1pW of power with current sensitivies on par with HBTs and HEMTs and with bandwidths 30 times that of HBTs and HEMTs, making them attractive for multi-qubit platforms. In this report we describe in detail the fabrication process flow for developing inductive pick-up coils and the fabrication and measurement of NbTiN and A1/A1Ox/A1 SQUIDs.

We present the fabrication of nano-magnet arrays, comprised of two sets of interleaving SmCo5 and Co nano-magnets, and the subsequent development and implementation of a protocol to program the array to create a one-dimensional rotating magnetic field. We designed the array based on the microstructural and magnetic properties of SmCo5 films annealed under different conditions, also presented here. Leveraging the extremely high contrast in coercivity between SmCo5 and Co, we applied a sequence of external magnetic fields to program the nano-magnet arrays into a configuration with alternating polarization, which based on simulations creates a rotating magnetic field in the vicinity of nano-magnets. Our proof-of-concept demonstration shows that complex, nanoscale magnetic fields can be synthesized through coercivity contrast of constituent magnetic materials and carefully designed sequences of programming magnetic fields.

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.

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Nanowire transistors are typically undoped devices whose characteristics depend strongly on the injection of carriers from the electrical contacts. In this letter, we fabricate and characterize SiGe nanowire transistors with an n-p-n doping profile and with a top gate covering only the p-doped section of the nanowire. For each device, we locate the p-segment with scanning capacitance microscopy, where the p-segment position varies along the channel due to the stochastic nature of our dropcast fabrication technique. The current-voltage characteristics for a series of transistors with different gate positions reveal that the on/off ratios for electrons is the highest when the gated p-type section is closest to the source contact, whereas the on/off ratios for holes is the highest when the gated p-type section is closest to the drain contact.

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Even as today's most prominent spin-based qubit technologies are maturing in terms of capability and sophistication, there is growing interest in exploring alternate material platforms that may provide advantages, such as enhanced qubit control, longer coherence times, and improved extensibility. Recent advances in heterostructure material growth have opened new possibilities for employing hole spins in semiconductors for qubit applications. Undoped, strained Ge/SiGe quantum wells are promising candidate hosts for hole spin-based qubits due to their low disorder, large intrinsic spin-orbit coupling strength, and absence of valley states. Here, we use a simple one-layer gated device structure to demonstrate both a single quantum dot as well as coupling between two adjacent quantum dots. The hole effective mass in these undoped structures, m∗ ∼ 0.08 m 0, is significantly lower than for electrons in Si/SiGe, pointing to the possibility of enhanced tunnel couplings in quantum dots and favorable qubit-qubit interactions in an industry-compatible semiconductor platform.

Performance of terahertz (THz) photoconductive devices, including detectors and emitters, has been improved recently by means of plasmonic nanoantennae and gratings. However, plasmonic nanostructures introduce Ohmic losses, which limit gains in device performance. In this presentation, we discuss an alternative approach, which eliminates the problem of Ohmic losses. We use all-dielectric photoconductive metasurfaces as the active region in THz switches to improve their efficiency. In particular, we discuss two approaches to realize perfect optical absorption in a thin photoconductive layer without introducing metallic elements. In addition to providing perfect optical absorption, the photoconductive channel based on all-dielectric metasurface allows us to engineer desired electrical properties, specifically, fast and efficient conductivity switching with very high contrast. This approach thus promises a new generation of sensitive and efficient THz photoconductive detectors. Here we demonstrate and discuss performance of two practical THz photoconductive detectors with integrated all-dielectric metasurfaces.

Here we present the development of a Zeptocalorimeter. The motivation for designing and implementing such a device is driven, ultimately, by its anticipated exceptional sensitivity (10-21 J/K, at 2K). Such a device would be highly valuable in detecting minute quantities of mass for threat detection, studying fundamental phonon physics, and detecting energetic dissipation events at the attojoule level. To date, the most sensitive calorimeter demonstrated in the literature at 2K has been developed by the Roukes group at Caltech, where they achieved an addendum heat capacity of 10^-15 J/K with a 1/1000 sensitivity to external stimuli. To obtain such a low value of heat capacity requires a very small thermal mass, and thus, one of the greatest challenges in this project is the fabrication of this device, which requires numerous precision nanofabrication techniques. Furthermore, the heat capacity measurement of this device, as performed from room temperature to cryogenic temperatures, is equally challenging, as the transient signals used to determine the platform's thermal time constant require careful attention to the mitigation of feedthrough capacitance and delicate amplifier offsets. In this report we describe in detail the fabrication process flow for developing the calorimeter, including the layout and device design for obtaining a single lumped RC thermal resistance and capacitance, so that the device can be used for quantitative measurements of nanoscale materials with a suitable thermal link. The measurement method and experimental setup are also given, where we explain the heater and thermometer calibration methods, the thermal resistance measurements, the transient measurements, and lastly the cryogenic setup with intermediate frequency cabling and the thermal sinking of those lines.

There has been much interest in leveraging the topological order of materials for quantum information processing. Among the various solid-state systems, one-dimensional topological superconductors made out of strongly spin-orbit-coupled nanowires have been shown to be the most promising material platform. In this project, we investigated the feasibility of turning silicon, which is a non-topological semiconductor and has weak spin-orbit coupling, into a one-dimensional topological superconductor. Our theoretical analysis showed that it is indeed possible to create a sizable effective spin-orbit gap in the energy spectrum of a ballistic one-dimensional electron channel in silicon with the help of nano-magnet arrays. Experimentally, we developed magnetic materials needed for fabricating such nano-magnets, characterized the magnetic behavior at low temperatures, and successfully demonstrated the required magnetization configuration for opening the spin-orbit gap. Our results pave the way toward a practical topological quantum computing platform using silicon, one of the most technologically mature electronic materials.

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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 (g_ip) can be vanishingly small while the perpendicular g factor (g_z) can be much larger than 2. Here we report the measurement of g_ip at very low hole densities using in-plane magneto-resistance measurement performed at the NHMFL.

We investigate carrier transport in silicon-germanium nanowires with an axial p-n junction doping profile by fabricating these wires into transistors that feature separate top gates over each doping segment. By independently biasing each gate, carrier concentrations in the n- and p-side of the wire can be modulated. For these devices, which were fabricated with nickel source-drain electrical contacts, holes are the dominant charge carrier, with more favorable hole injection occurring on the p-side contact. Channel current exhibits greater sensitivity to the n-side gate, and in the reverse biased source-drain configuration, current is limited by the nickel/n-side Schottky contact.

We report the measurements of the effective g factor of low-density two-dimensional holes in a Ge quantum well. Using the temperature dependence of the Shubnikov-de Haas oscillations, we extract the effective g factor in a magnetic field perpendicular to the sample surface. Very large values of the effective g factor, ranging from ∼13 to ∼28, are observed in the density range of 1.4×1010 cm-2- 1.4×1011 cm-2. When the magnetic field is oriented parallel to the sample surface, the effective g factor is obtained from a protrusion in the magneto-resistance data that signify full spin polarization. In the latter orientation, a small effective g factor, ∼1.3-1.4, is measured in the density range of 1.5×1010 cm-2- 2×1010 cm-2. This very strong anisotropy is consistent with theoretical predictions and previous measurements in other 2D hole systems, such as InGaAs and GaSb.

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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.

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This paper reports a diameter-independent Young's modulus of 91.9 ± 8.2 GPa for [111] Germanium nanowires (Ge NWs). When the surface oxide layer is accounted for using a core-shell NW approximation, the YM of the Ge core approaches a near theoretical value of 147.6 ± 23.4 GPa. The ultimate strength of a NW device was measured at 10.9 GPa, which represents a very high experimental-to-theoretical strength ratio of ∼75%. With increasing interest in this material system as a high-capacity lithium-ion battery anode, the presented data provide inputs that are essential in predicting its lithiation-induced stress fields and fracture behavior.

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.

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Electrodeposited metallic lithium is an ideal negative battery electrode, but nonuniform microstructure evolution during cycling leads to degradation and safety issues. A better understanding of the Li plating and stripping processes is needed to enable practical Li-metal batteries. Here we use a custom microfabricated, sealed liquid cell for in situ scanning transmission electron microscopy (STEM) to image the first few cycles of lithium electrodeposition/dissolution in liquid aprotic electrolyte at submicron resolution. Cycling at current densities from 1 to 25 mA/cm² leads to variations in grain structure, with higher current densities giving a more needle-like, higher surface area deposit. The effect of the electron beam was explored, and it was found that, even with minimal beam exposure, beam-induced surface film formation could alter the Li microstructure. The electrochemical dissolution was seen to initiate from isolated points on grains rather than uniformly across the Li surface, due to the stabilizing solid electrolyte interphase surface film. We discuss the implications for operando STEM liquid-cell imaging and Li-battery applications.

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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.

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The thermal conductivity of single crystal silicon was engineered using lithographically formed phononic crystals. Specifically, sub-micron periodic through-holes were patterned in 500nm-thick silicon membranes to construct phononic crystals, and through phonon scattering enhancement, heat transfer was significantly reduced. The thermal conductivity of silicon phononic crystals was measured as low as 32.6W/mK, which is a ∼75% reduction compared to bulk silicon thermal conductivity [1]. This corresponds to a 37% reduction even after taking into account the contributions of the thin-film and volume reduction effects, while the electrical conductivity was reduced only by as much as the volume reduction effect. The demonstrated method uses conventional lithography-based technologies that are directly applicable to diverse micro/nano-scale devices, leading toward huge performance improvements where heat management is important. © 2011 IEEE.

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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.