Publications

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Measurements of the electrical and thermal transport properties of one-dimensional nanostructures (e.g., nanotubes and nanowires) typically are obtained without detailed knowledge of the specimen's atomic-scale structure or defects. To address this deficiency we have developed a microfabricated, chip-based characterization platform that enables both transmission electron microscopy (TEM) of atomic structure and defects as well as measurement of the thermal transport properties of individual nanostructures. The platform features a suspended heater line that contacts the center of a suspended nanostructure/nanowire that was placed using in-situ scanning electron microscope nanomanipulators. One key advantage of this platform is that it is possible to measure the thermal conductivity of both halves of the nanostructure (on each side of the central heater), and this feature permits identification of possible changes in thermal conductance along the wire and measurement of the thermal contact resistance. Suspension of the nanostructure across a through-hole enables TEM characterization of the atomic and defect structure (dislocations, stacking faults, etc.) of the test sample. As a model study, we report the use of this platform to measure the thermal conductivity and defect structure of GaN nanowires. The utilization of this platform for the measurements of other nanostructures will also be discussed.

Although planar heterostructures dominate current solid-state lighting architectures (SSL), 1D nanowires have distinct and advantageous properties that may eventually enable higher efficiency, longer wavelength, and cheaper devices. However, in order to fully realize the potential of nanowire-based SSL, several challenges exist in the areas of controlled nanowire synthesis, nanowire device integration, and understanding and controlling the nanowire electrical, optical, and thermal properties. Here recent results are reported regarding the aligned growth of GaN and III-nitride core-shell nanowires, along with extensive results providing insights into the nanowire properties obtained using cutting-edge structural, electrical, thermal, and optical nanocharacterization techniques. A new top-down fabrication method for fabricating periodic arrays of GaN nanorods and subsequent nanorod LED fabrication is also presented.

We report on the novel room temperature method of synthesizing advanced nuclear fuels; a method that virtually eliminates any volatility of components. This process uses radiolysis to form stable nanoparticle (NP) nuclear transuranic (TRU) fuel surrogates and in-situ heated stage TEM to sinter the NPs. The radiolysis is performed at Sandia's Gamma Irradiation Facility (GIF) 60Co source (3 x 10{sup 6} rad/hr). Using this method, sufficient quantities of fuels for research purposes can be produced for accelerated advanced nuclear fuel development. We are focused on both metallic and oxide alloy nanoparticles of varying compositions, in particular d-U, d-U/La alloys and d-UO2 NPs. We present detailed descriptions of the synthesis procedures, the characterization of the NPs, the sintering of the NPs, and their stability with temperature. We have employed UV-vis, HRTEM, HAADF-STEM imaging, single particle EDX and EFTEM mapping characterization techniques to confirm the composition and alloying of these NPs.

Advances in electrochemical energy storage science require the development of new or the refinement of existing in situ probes that can be used to establish structure - activity relationships for technologically relevant materials. The drive to develop reversible, high capacity electrodes from nanoscale building blocks creates an additional requirement for high spatial resolution probes to yield information of local structural, compositional, and electronic property changes as a function of the storage state of a material. In this paper, we describe a method for deconstructing a lithium ion battery positive electrode into its basic constituents of ion insertion host particles and a carbon current collector. This model system is then probed in an electrochemical environment using a combination of atomic force microscopy and tunneling spectroscopy to correlate local activity with morphological and electronic configurational changes. Cubic spinel Li{sub 1+x}Mn{sub 2-x}O{sub 4} nanoparticles are grown on graphite surfaces using vacuum deposition methods. The structure and composition of these particles are determined using transmission electron microscopy and Auger microprobe analysis. The response of these particles to initial de-lithiation, along with subsequent electrochemical cycling, is tracked using scanning probe microscopy techniques in polar aprotic electrolytes (lithium hexafluorophosphate in ethylene carbonate:diethylcarbonate). The relationship between nanoparticle size and reversible ion insertion activity will be a specific focus of this paper.

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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.

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Nanowires based on the III nitride materials system have attracted attention as potential nanoscale building blocks in optoelectronics, sensing, and electronics. However, before such applications can be realized, several challenges exist in the areas of controlled and ordered nanowire synthesis, fabrication of advanced nanowire heterostructures, and understanding and controlling the nanowire electrical and optical properties. Here, recent work is presented involving the aligned growth of GaN and III-nitride core-shell nanowires, along with extensive results providing insights into the nanowire properties obtained using advanced electrical, optical and structural characterization techniques.

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Reducing battery materials to nano-scale dimensions may improve battery performance while maintaining the use of low-cost materials. However, we need better characterization tools with atomic to nano-scale resolution in order to understand degradation mechanisms and the structural and mechanical changes that occur in these new materials during battery cycling. To meet this need, we have developed a micro-electromechanical systems (MEMS)-based platform for performing electrochemical measurements using volatile electrolytes inside a transmission electron microscope (TEM). This platform uses flip-chip assembly with special alignment features and multiple buried electrode configurations. In addition to this platform, we have developed an unsealed platform that permits in situ TEM electrochemistry using ionic liquid electrolytes. As a test of these platform concepts, we have assembled MnO{sub 2} nanowires on to the platform using dielectrophoresis and have examined their electrical and structural changes as a function of lithiation. These results reveal a large irreversible drop in electronic conductance and the creation of a high degree of lattice disorder following lithiation of the nanowires. From these initial results, we conclude that the future full development of in situ TEM characterization tools will enable important mechanistic understanding of Li-ion battery materials.