Nick A. Roberts

Competing Liquid Phase Instabilities during Pulsed Laser Induced Self-Assembly of Copper Rings into Ordered Nanoparticle Arrays on SiO2

Nanoscale copper rings of different radii, thicknesses, and widths were synthesized on silicon dioxide thin films and were subsequently liquefied via a nanosecond pulse laser treatment. During the nanoscale liquid lifetimes, the rings experience competing retraction dynamics and thin film and/or Rayleigh-Plateau types of instabilities, which lead to arrays of ordered nanodroplets. Surprisingly, the results are significantly different from those of similar experiments carried out on a Si surface. We use hydrodynamic simulations to elucidate how the different liquid/solid interactions control the different instability mechanisms in the present problem.

Computational Study of Thermal Rectification From Nanostructured Interfaces

Thermal rectification is a phenomenon in which transport is p referred in one direction over the opposite. Though observations of thermal rectification have been elusive, it could be useful in many applications such as thermal management of electronics and improvement of thermoelectr ic devices. The current work explores the possibility of thermally rectifying devices with the use of nanostru ctured interfaces. Interfaces can theoretically result in thermally rectifying behavior because of the difference in phonon frequency content between two dissimilar materials. The current work shows an effective rectification of g reater than 25% in a device composed of two different materials divided equally by a single planar interface.

Hierarchical Nanoparticle Ensembles Synthesized by Liquid Phase Directed Self-Assembly

A liquid metal filament supported on a dielectric substrate was directed to fragment into an ordered, mesoscale particle ensemble. Imposing an undulated surface perturbation on the filament forced the development of a single unstable mode from the otherwise disperse, multimodal Rayleigh-Plateau instability. The imposed mode paved the way for a hierarchical spatial fragmentation of the filament into particles, previously seen only at much larger scales. Ultimately, nanoparticle radius control is demonstrated using a micrometer scale switch.

Purification of nanoscale electron-beam-induced platinum deposits via a pulsed laser-induced oxidation reaction.

Platinum-carbon deposits made via electron-beam-induced deposition were purified via a pulsed laser-induced oxidation reaction and erosion of the amorphous carbon to form pure platinum. Purification proceeds from the top down and is likely catalytically facilitated via the evolving platinum layer. Thermal simulations suggest a temperature threshold of ∼485 K, and the purification rate is a function of the PtC5 thickness (80-360 nm) and laser pulse width (1-100 μs) in the ranges studied. The thickness dependence is attributed to the ∼235 nm penetration depth of the PtC5 composite at the laser wavelength, and the pulse-width dependence is attributed to the increased temperatures achieved at longer pulse widths. Remarkably fast purification is realized at cumulative laser exposure times of less than 1 s.

Directed assembly of one- and two-dimensional nanoparticle arrays from pulsed laser induced dewetting of square waveforms.

The directed assembly of arrayed nanoparticles is demonstrated by dictating the flow of a liquid phase filament on the nanosecond time scale. Results for the assembly of Ni nanoparticles on SiO2 are presented. Previously, we have implemented a sinusoidal perturbation on the edge of a solid phase Ni, thin film strip to tailor nanoparticle assembly. Here, a nonlinear square waveform is explored. This waveform made it possible to expand the range of nanoparticle spacing-radius combinations attainable, which is otherwise limited by the underlying Rayleigh-Plateau type of instability. Simulations of full Navier-Stokes equations based on volume of fluid method were implemented to gain further insight regarding the nature of instability mechanism leading to particle formation in experiments.

Real-time observation of nanosecond liquid-phase assembly of nickel nanoparticles via pulsed-laser heating.

Using pump-probe electron microscopy techniques, the dewetting of thin nickel films exposed to a pulsed nanosecond laser was monitored at tens of nanometers spatial and nanosecond time scales to provide insight into the liquid-phase assembly dynamics. Thickness-dependent and correlated time and length scales indicate that a spinodal instability drives the assembly process. Measured lifetimes of the liquid metal are consistent with finite-difference simulations of the laser-irradiated film and are consistent with estimated and observed spinodal time scales. These results can be used to design improved synthesis and assembly routes toward achieving advanced functional nanomaterials and devices.

Phonon wave-packet simulations of Ar/Kr interfaces for thermal rectification

The frequency and direction dependence of transmission coefficients at interfaces was investigated theoretically. The interfaces are formed by having two Lennard-Jones materials differing in mass and interatomic potential equally divided at the center of an fcc lattice system. A single frequency wave-packet is generated at one end of the system and allowed to propagate through the system until all interactions with the interface are complete. The transmission coefficient is then calculated by comparing the energy of the packet that is transmitted with the original wave-packet. Results show a difference in transmission when the wave-packet originates from opposite sides.

Enhanced by-product desorption via laser assisted electron beam induced deposition of W(CO)6 with improved conductivity and resolution

Nanowires with higher tungsten (W) concentration and enhanced conductivity were grown via the laser assisted electron beam induced deposition (LAEBID) technique using tungsten hexacarbonyl W(CO)6 as the gas precursor. Periodic, pulsed laser irradiation facilitated CO desorption during growth by heating the deposit. Deposit purity improved with laser pulse width up to the threshold for pyrolytic laser chemical vapor deposition (LCVD). Higher resolution was also observed and was attributed to reduced CO incorporation and higher deposit density. The optimal composition and lowest resistivity was achieved by synchronizing the electron beam induced deposition and laser assist such that (1) the electron beam induced deposit is less than a monolayer per cycle and (2) the laser induced heating is just below the LCVD threshold.

In situ laser processing in a scanning electron microscope

Laser delivery probes using multimode fiber optic delivery and bulk focusing optics have been constructed and used for performing materials processing experiments within scanning electron microscope/focused ion beam instruments. Controlling the current driving a 915-nm semiconductor diode laser module enables continuous or pulsed operation down to sub-microsecond durations, and with spot sizes on the order of 50 μm diameter, achieving irradiances at a sample surface exceeding 1 MW/cm2. Localized laser heating has been used to demonstrate laser chemical vapor deposition of Pt, surface melting of silicon, enhanced purity, and resistivity via laser annealing of Au deposits formed by electron beam induced deposition, and in situ secondary electron imaging of laser induced dewetting of Au metal films on SiOx.

Synthesis and electroplating of high resolution insulated carbon nanotube scanning probes for imaging in liquid solutions

High resolution and isolated scanning probe microscopy (SPM) is in demand for continued development of energy storage and conversion systems involving chemical reactions at the nanoscale as well as an improved understanding of biological systems. Carbon nanotubes (CNTs) have large aspect ratios and, if leveraged properly, can be used to develop high resolution SPM probes. Isolation of SPM probes can be achieved by depositing a dielectric film and selectively etching at the apex of the probe. In this paper the fabrication of a high resolution and isolated SPM tip is demonstrated using electron beam induced etching of a dielectric film deposited onto an SPM tip with an attached CNT at the apex.