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Devaraj, Arun

Publications and source records attributed to Devaraj, Arun.

165 records · Page 10
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DOE OSTI2013

Subsurface Synthesis and Characterization of Ag Nanoparticles Embedded in MgO

Metal nanoparticles exhibit localized surface plasmon resonance (LSPR) which is very sensitive to the size and shape of the nanoparticle and the dielectric medium surrounding it. LSPR causes field enhancement near the surface of the nanoparticle making them interesting candidates for plasmonic applications. In particular, partially exposed metallic nanoparticles distributed in a dielectric matrix form hotspots which are prime locations for LSPR spectroscopy and sensing. This study involves synthesizing partially buried Ag nanoparticles in MgO and investigating the characteristics of this material system. Ag nanoparticles of different shapes and size distributions were synthesized below the surface of MgO by implanting 200 keV Ag+ ions followed by annealing at 10000C for 10 and 30 hours. A detailed optical and structural characterization was carried out to understand the evolution of Ag nanoparticle microstructure and size distribution inside the MgO matrix. Micro x-ray diffraction (MicroXRD) was employed to investigate the structural properties and estimate the crystallite size. The nanoparticles evolved from a spherical to faceted morphology with annealing time, assuming an octahedral shape truncated at the (001) planes as seen from aberration corrected transmission electron microscopy (TEM) images. The nanoparticles embedded in MgO were shown to be pure metallic Ag using atom probe tomography (APT). The nanoparticles were partially exposed to the surface employing plasma etch techniques to remove the overlaying MgO. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) were employed to study the surface morphology and obtain a height distribution for the partially exposed nanoparticles.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2013

Role of Photoexcitation and Field Ionization in the Measurement of Accurate Oxide Stoichiometry by Laser-Assisted Atom Probe Tomography

Pulsed lasers extend the high spatial and mass resolution of atom probe tomography (APT) to non-conducting materials, such as oxides. For prototypical metal oxide MgO, measured stoichiometry depends strongly upon pulse energy and applied voltage. Very low laser energies (0.02 pJ) and high electric fields yield optimal stoichiometric accuracy, attributed to the field-dependent ionization of photo-desorbed O or O2 neutrals. This emphasizes the importance of considering electronic excitations in APT analysis of oxides ionic materials.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2012

Controlling Axial p-n Heterojunction Abruptness Through Catalyst Alloying in Vapor-Liquid-Solid Grown Semiconductor Nanowires

The p-n junction can be regarded as the most important electronic structure that is responsible for the ubiquity of semiconductor microelectronics today. Efforts to continually scale down the size of electronic components is guiding research to explore the use of nanomaterials synthesized from a bottom-up approach - group-IV semiconductor nanowires being one such material. However, Au-catalyzed synthesis of Si/Si1-x-Gex semiconductor nanowire heterojunctions using the commonly-used vapor-liquid-solid (VLS) growth technique results in diffuse heterojunction interfaces [1], leading to doubts of producing compositionally-sharp p-n junctions using this approach. However, we have recently reported the ability to increase Ge-Si nanowire heterojunction abruptness by VLS synthesis from a Au(1-x)Ga(x) catalyst alloy as shown by EDX analysis in an SEM [2]. In this work, we have extended the use of a AuGa catalyst alloy to produce more compositionally abrupt p-n junction interfaces compared to using pure Au as directly measured by atom probe tomography. As shown in Figure 1(a-b), individual Ge-Si heterostructured nanowires were grown vertically atop Ge(111) microposts. Direct growth on the microposts provides a facile approach to nanowire analysis which circumvents the need to use FIB-based sample preparation techniques. Both nanowires grown from pure Au and a AuGa catalyst alloy were analyzed. The corresponding 3D APT reconstruction of an individual heterostructured nanowire is shown in Figure 1(c) with the corresponding materials labeled. A 1-dimensional composition profile along the analysis direction in Figure 1(d) confirms an increase in heterojunction abruptness for nanowires grown from AuGa (~10nm) compared to nanowires grown from pure Au (~65nm). Analysis of the P distribution within the Si region (Figure 1(e)) indicates that P reaches a constant distribution over approximately 10nm when incorporated through the AuGa catalyst, whereas it continually increases over 100’s of nanometers when incorporated through pure Au. The apparent lower overall P concentration within the nanowire grown from the AuGa alloy suggests that the solubility of P in the alloy is lower compared to pure Au. The ability to controllably increase nanowire p-n junction abruptness is important for nanowire applications as solar cells and tunneling field effect transistors where an increase in device performance is expected from shaper p-n junction interfaces. [1] T.E. Clark et al., Nano Lett. 8 (2008) 1246. [2] D.E. Perea et al., Nano Lett. 11 (2011) 3117. [3] The research was supported through the user program at both the Center for Integrated Nanotechnologies at Los Alamos National Laboratory and the Environmental Molecular Sciences Laboratory at Pacific Northwest National Laboratory.

Environmental Molecular Sciences Laboratory↗