Adam B. Taylor

Below Melting Point Photothermal Reshaping of Single Gold Nanorods Driven by Surface Diffusion

Plasmonic gold nanorod instability and reshaping behavior below melting points are important for many future applications but are yet to be fully understood, with existing nanoparticle melting theories unable to explain the observations. Here, we have systematically studied the photothermal reshaping behavior of gold nanorods irradiated with femtosecond laser pulses to report that the instability is driven by curvature-induced surface diffusion rather than a threshold melting process, and that the stability dramatically decreases with increasing aspect ratio. We successfully utilized the surface diffusion model to explain the observations and found that the activation energy for surface diffusion was dependent on the aspect ratio of the rods, from 0.6 eV for aspect ratio of 5 to 1.5 eV for aspect ratio less than 3. This result indicates that the surface atoms are much easier to diffuse around in larger aspect ratio rods than in shorter rods and can induce reshaping at any given temperature. Current plasmonics and nanorod applications with the sharp geometric features used for greater field enhancement will therefore need to consider surface diffusion driven shape change even at low temperatures.

Detuned surface plasmon resonance scattering of gold nanorods for continuous wave multilayered optical recording and readout

In a multilayered structure of absorptive optical recording media, continuous-wave laser operation is highly disadvantageous due to heavy beam extinction. For a gold nanorod based recording medium, the narrow surface plasmon resonance (SPR) profile of gold nanorods enables the variation of extinction through mulilayers by a simple detuning of the readout wavelength from the SPR peak. The level of signal extinction through the layers can then be greatly reduced, resulting more efficient readout at deeper layers. The scattering signal strength may be decreased at the detuned wavelength, but balancing these two factors results an optimal scattering peak wavelength that is specific to each layer. In this paper, we propose to use detuned SPR scattering from gold nanorods as a new mechanism for continuous-wave readout scheme on gold nanorod based multilayered optical storage. Using this detuned scattering method, readout using continuous-wave laser is demonstrated on a 16 layer optical recording medium doped with heavily distributed, randomly oriented gold nanorods. Compared to SPR on-resonant readout, this method reduced the required readout power more than one order of magnitude, with only 60 nm detuning from SPR peak. The proposed method will be highly beneficial to multilayered optical storage applications as well as applications using a continuous medium doped heavily with plasmonic nanoparticles.

Electron-beam lithography of plasmonic nanorod arrays for multilayered optical storage

In this paper we demonstrate multilayer fabrication of plasmonic gold nanorod arrays using electron-beam lithography (EBL), and show that this structure could be used for multilayered optical storage media capable of continuous-wave (cw) laser readout. The gold nanorods fabricated using the EBL method are aligned perfectly and homogeneous in size and shape, allowing the polarization response of surface plasmon resonance (SPR) to be observed through ensemble array. This property in turn permits polarization detuned SPR readout possible and other manipulations such as progressively twisted arrays through the multilayers to make cw readout possible through deeper layers without too much extinction loss. The layered gold nanorod arrays are separated by thick spacer layer to enable the optical resolving of individual layers. Using this method, we demonstrated four-fold reduction in extinction loss for cw readout in three-layer structure. The current technique of multilayer fabrication and readout can be useful in 3-dimensional fabrication of plasmonic circuits and structures.

Alignment of gold nanorods by angular photothermal depletion

In this paper, we demonstrate that a high degree of alignment can be imposed upon randomly oriented gold nanorod films by angular photothermal depletion with linearly polarized laser irradiation. The photothermal reshaping of gold nanorods is observed to follow quadratic melting model rather than the threshold melting model, which distorts the angular and spectral hole created on 2D distribution map of nanorods to be an open crater shape. We have accounted these observations to the alignment procedures and demonstrated good agreement between experiment and simulations. The use of multiple laser depletion wavelengths allowed alignment criteria over a large range of aspect ratios, achieving 80% of the rods in the target angular range. We extend the technique to demonstrate post-alignment in a multilayer of randomly oriented gold nanorod films, with arbitrary control of alignment shown across the layers. Photothermal angular depletion alignment of gold nanorods is a simple, promising post-alignment method for creating future 3D or multilayer plasmonic nanorod based devices and structures.

All-optical imaging of gold nanoparticle geometry using super-resolution microscopy

We demonstrate the all-optical reconstruction of gold nanoparticle geometry using super-resolution microscopy. We employ DNA-PAINT to get exquisite control over the (un)binding kinetics by the number of complementary bases and salt concentration, leading to localization accuracies of ∼5 nm. We employ a dye with an emission spectrum strongly blue-shifted from the plasmon resonance to minimize mislocalization due to plasmon-fluorophore coupling. We correlate the all-optical reconstructions with atomic force microscopy images and find that reconstructed dimensions deviate by no more than ∼10%. Numerical modeling shows that this deviation is determined by the number of events per particle, and the signal-to-background ratio in our measurement. We further find good agreement between the reconstructed orientation and aspect ratio of the particles and single-particle scattering spectroscopy. This method may provide an approach to all-optically image the geometry of single particles in confined spaces such as microfluidic circuits and biological cells, where access with electron beams or tip-based probes is prohibited.

Single layer graphene band hybridization with silver nanoplates: Interplay between doping and plasmonic enhancement

In this paper, we report single layer graphene (SLG) hybridized with silver nanoplates, in which nanoplates act as either a charge doping or a field enhancement source for the SLG Raman spectrum. Surprisingly, the stiffening of both G and 2D peaks of more than 10 cm−1 was observed with no plasmonic enhancement of peaks, indicating that p-doping from nanoplates on SLG is occurring. Such observation is explained in terms of the contact separation distance between the graphene and the silver nanoplates being enough (∼4 A) to cause a Fermi level shift in graphene to allow p-doping. When nanoplates were modified in shape with laser irradiation by either photothermal plasmon printing or laser induced ablation, the charge doping was lifted and the strong plasmonic enhancement of Raman signals was observed, indicating that the separation distance is increased. Further, when the nanoplates are oxidized, the two effects on the Raman bands of SLG are turned off, returning the Raman signals back to the original SLG s...

Plasmonic random media based on gold nanorods as an optical storage medium

In this paper, we present our recent study on the plasmonic random media based on gold nanorods doped in polymer matrix using image correlation spectroscopy for noise-free multidimensional optical recording medium.