Publications

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We investigated error and uncertainty in Raman thermal conductivity measurements via finite element based numerical simulation of two geometries often employed -- Joule-heating of a wire and laser-heating of a suspended wafer. Using this methodology, the accuracy and precision of the Raman-derived thermal conductivity are shown to depend on (1) assumptions within the analytical model used in the deduction of thermal conductivity, (2) uncertainty in the quantification of heat flux and temperature, and (3) the evolution of thermomechanical stress during testing. Apart from the influence of stress, errors of 5% coupled with uncertainties of ±15% are achievable for most materials under conditions typical of Raman thermometry experiments. Error can increase to >20%, however, for materials having highly temperature dependent thermal conductivities or, in some materials, when thermomechanical stress develops concurrent with the heating. A dimensionless parameter -- termed the Raman stress factor -- is derived to identify when stress effects will induce large levels of error. Together, the results compare the utility of Raman based conductivity measurements relative to more established techniques while at the same time identifying situations where its use is most efficacious.

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We study the interplay between the contributions of electron thermal flux and interface scattering to the Kapitza conductance across metal-metal interfaces through measurements of thermal conductivity of copper-niobium multilayers. Thermal conductivities of copper-niobium multilayer films of period thicknesses ranging from 5.4 to 96.2 nm and sample thicknesses ranging from 962 to 2677 nm are measured by time-domain thermoreflectance over a range of temperatures from 78 to 500 K. The Kapitza conductances between the Cu and Nb interfaces in multilayer films are determined from the thermal conductivities using a series resistor model and are in good agreement with the electron diffuse mismatch model. Our results for the thermal boundary conductance between Cu and Nb are compared to literature values for the thermal boundary conductance across Al-Cu and Pd-Ir interfaces, and demonstrate that the interface conductance in metallic systems is dictated by the temperature derivative of the electron energy flux in the metallic layers, rather than electron mean free path or scattering processes at the interface.

Conversion of plane waves to surface waves prior to detection allows key advantages in changes to the architecture of the detector pixels in a focal plane array. We have integrated subwavelength patterned metal nanoantennas with various detector materials to incorporate these advantages: midwave infrared indium gallium arsenide antimonide detectors and longwave infrared graphene detectors. Nanoantennas offer a means to make infrared detectors much thinner by converting incoming plane waves to more tightly bound and concentrated surface waves. Thinner architectures reduce both dark current and crosstalk for improved performance. For graphene detectors, which are only one or two atomic layers thick, such field concentration is a necessity for usable device performance, as single pass plane wave absorption is insufficient. Using III-V detector material, we reduced thickness by over an order of magnitude compared to traditional devices. We will discuss Sandia's motivation for these devices, which go beyond simple improvement in traditional performance metrics. The simulation methodology and design rules will be discussed in detail. We will also offer an overview of the fabrication processes required to make these subwavelength structures on at times complex underlying devices based on III-V detector material or graphene on silicon or silicon carbide. Finally, we will present our latest infrared detector characterization results for both III-V and graphene structures.

Vertically aligned, untangled planarized arrays of multiwall carbon nanotubes (MWNTs) with Ohmic back contacts were grown in nanopore templates on arbitrary substrates. The templates were prepared by sputter depositing Nd-doped Al films onto W-coated substrates, followed by anodization to form an aluminum oxide nanopore array. The W underlayer helps eliminate the aluminum oxide barrier that typically occurs at the nanopore bottoms by instead forming a thin WO3 layer. The WO3 can be selectively etched to enable electrodeposition of Co catalysts with control over the Co site density. This led to control of the site density of MWNTs grown by thermal chemical vapor deposition, with W also serving as a back electrical contact. Ohmic contact to MWNTs was confirmed, even following ultrasonic cutting of the entire array to a uniform height.

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Nanoantennas are an enabling technology for visible to terahertz components and may be used with a variety of detector materials. We have integrated subwavelength patterned metal nanoantennas with various detector materials for infrared detection: midwave infrared indium gallium arsenide antimonide detectors, longwave infrared graphene detectors, and shortwave infrared germanium detectors. Nanoantennas offer a means to make infrared detectors much thinner, thus lowering the dark current and improving performance. The nanoantenna converts incoming plane waves to more tightly bound and concentrated surface waves. The active material only needs to extend as far as these bound fields. In the case of graphene detectors, which are only one or two atomic layers thick, such field concentration is a necessity for usable device performance, as single pass absorption is insufficient. The nanoantenna is thus the enabling component of these thin devices. However nanoantenna integration and fabrication vary considerably across these platforms as do the considerations taken into account during design. Here we discuss the motivation for these devices and show examples for the three material systems. Characterization results are included for the midwave infrared detector. © 2014 SPIE.

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Chemical functionalization is required to adapt graphenes properties to many applications. However, most covalent functionalization schemes are spontaneous or defect driven and are not suitable for applications requiring directed assembly of molecules on graphene substrates. In this work, we demonstrated electrochemically driven covalent bonding of phenyl iodoniums onto epitaxial graphene. The amount of chemisorption was demonstrated by varying the duration of the electrochemical driving potential. Chemical, electronic, and defect states of phenyl-modified graphene were studied by photoemission spectroscopy, spatially resolved Raman spectroscopy, and water contact angle measurement. Covalent attachment rehybridized some of the delocalized graphene sp2 orbitals to localized sp3 states. Control over the relative spontaneity (reaction rate) of covalent graphene functionalization is an important first step to the practical realization of directed molecular assembly on graphene. More than 10 publications, conference presentations, and program highlights were produced (some invited), and follow-on funding was obtained to continue this work.

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