Teri W. Odom

Atomic structure and electronic properties of single-walled carbon nanotubes

Carbon nanotubes are predicted to be metallic or semiconducting depending on their diameter and the helicity of the arrangement of graphitic rings in their walls. Scanning tunnelling microscopy (STM) offers the potential to probe this prediction, as it can resolve simultaneously both atomic structure and the electronic density of states. Previous STM studies of multi-walled nanotubes and single-walled nanotubes (SWNTs) have provided indications of differing structures and diameter-dependent electronic properties, but have not revealed any explicit relationship between structure and electronic properties. Here we report STM measurements of the atomic structure and electronic properties of SWNTs. We are able to resolve the hexagonal-ring structure of the walls, and show that the electronic properties do indeed depend on diameter and helicity. We find that the SWNT samples exhibit many different structures, with no one species dominating.

Multiscale patterning of plasmonic metamaterials

The interaction of light with surface plasmons--collective oscillations of free electrons--in metallic nanostructures has resulted in demonstrations of enhanced optical transmission, collimation of light through a subwavelength aperture, negative permeability and refraction at visible wavelengths, and second-harmonic generation from magnetic metamaterials. The structures that display these plasmonic phenomena typically consist of ordered arrays of particles or holes with sizes of the order of 100 nm. However, surface plasmons can interact with each other over much longer distances, so the ability to organize nanoscale particles or holes over multiple length scales could lead to new plasmonic metamaterials with novel optical properties. Here, we present a high-throughput nanofabrication technique-soft interference lithography-that combines the ability of interference lithography to produce wafer-scale nanopatterns with the versatility of soft lithography, and use it to create such plasmonic metamaterials. Metal films perforated with quasi-infinite arrays of 100-nm holes were generated over areas greater than 10 cm(2), exhibiting sharp spectral features that changed in relative amplitude and shifted to longer wavelengths when exposed to increased refractive index environments. Moreover, gold nanohole arrays patterned into microscale patches exhibited strikingly different transmission properties; for instance, patches of nanoholes displayed narrow resonances (<14.5 nm full-width-at-half-maximum) that resulted in high refractive index sensitivities far exceeding those reported previously. Soft interference lithography was also used to produce various infinite and finite-area arrays of nanoparticles, including patterns that contained optically distinct particles side by side and arrays that contained both metallic and dielectric materials.

ELECTRONIC DENSITY OF STATES OF ATOMICALLY RESOLVED SINGLE-WALLED CARBON NANOTUBES : VAN HOVE SINGULARITIES AND END STATES

The electronic densities of states of atomically resolved single-walled carbon nanotubes have been investigated using scanning tunneling microscopy. Peaks in the density of states due to the one-dimensional nanotube band structure have been characterized and compared with tight-binding calculations. In addition, tunneling spectroscopy measurements recorded along the axis of an atomically resolved nanotube were found to exhibit new, low-energy peaks in the density of states near the tube end. Calculations suggest that these features arise from the specific arrangement of carbon atoms that close the nanotube end.

Nanofabrication of plasmonic structures.

This review focuses on nanofabrication tools, based on soft lithography, which can generate a wide range of noble-metal structures with exceptional optical properties. These techniques offer a scalable and practical approach for producing arrays of complementary plasmonic structures (nanoholes and nanoparticles) and, in addition, expand the possible architectures of plasmonic materials because the metal building blocks can be organized over multiple length scales. We describe the preparation and characterization of five different systems: subwavelength nanohole arrays, finite arrays of nanoholes, microscale arrays of nanoholes, multiscale arrays of nanoparticles, and pyramidal particles. We also discuss how the surface plasmon resonances of these structures can be tuned across visible and near-infrared wavelengths by varying different parameters. Applications and future prospects of these nanostructured metals are addressed.

Tunable subradiant lattice plasmons by out-of-plane dipolar interactions

Plasmonic nanostructures concentrate optical fields into nanoscale volumes, which is useful for plasmonic nanolasers, surface enhanced Raman spectroscopy and white-light generation. However, the short lifetimes of the emissive plasmons correspond to a rapid depletion of the plasmon energy, preventing further enhancement of local optical fields. Dark (subradiant) plasmons have longer lifetimes, but their resonant wavelengths cannot be tuned over a broad wavelength range without changing the overall geometry of the nanostructures. Also, fabrication of the nanostructures cannot be readily scaled because their complex shapes have subwavelength dimensions. Here, we report a new type of subradiant plasmon with a narrow (∼5 nm) resonant linewidth that can be easily tuned by changing the height of large (>100 nm) gold nanoparticles arranged in a two-dimensional array. At resonance, strong coupling between out-of-plane nanoparticle dipolar moments suppresses radiative decay, trapping light in the plane of the array and strongly localizing optical fields on each nanoparticle. This new mechanism can open up applications for subradiant plasmons because height-controlled nanoparticle arrays can be manufactured over wafer-scale areas on a variety of substrates.

Near-field scanning photocurrent microscopy of a nanowire photodetector

A near-field scanning optical microscope was used to image the photocurrent induced by local illumination along the length of a metal-semiconductor-metal (MSM) photodetector made from an individual CdS nanowire. Nanowire MSM photodetectors exhibited photocurrents ∼105 larger than the dark current (<2pA) under uniform monochromatic illumination; under local illumination, the photoresponse was localized to the near-contact regions. Analysis of the spatial variation and bias dependence of the local photocurrent allowed the mechanisms of photocarrier transport and collection to be identified, highlighting the importance of near-field scanning photocurrent microscopy to elucidating the operating principles of nanowire devices.

Direct observation of nanoparticle-cancer cell nucleus interactions

We report the direct visualization of interactions between drug-loaded nanoparticles and the cancer cell nucleus. Nanoconstructs composed of nucleolin-specific aptamers and gold nanostars were actively transported to the nucleus and induced major changes to the nuclear phenotype via nuclear envelope invaginations near the site of the construct. The number of local deformations could be increased by ultrafast, light-triggered release of the aptamers from the surface of the gold nanostars. Cancer cells with more nuclear envelope folding showed increased caspase 3 and 7 activity (apoptosis) as well as decreased cell viability. This newly revealed correlation between drug-induced changes in nuclear phenotype and increased therapeutic efficacy could provide new insight for nuclear-targeted cancer therapy.

Single-walled carbon nanotube probes for high-resolution nanostructure imaging

Single-walled carbon nanotube (SWNT) tips have been used to image nanostructures with high resolution. Studies of gold nanocrystal standards showed that SWNT tips provide a significant improvement in lateral resolution with respect to multi-walled nanotube tips and microfabricated Si tips. The nanotube tips were also used to resolve substructure within SWNTs deposited on surfaces. These results suggest that observed 1.5 nm high structures can correspond to several SWNTs aligned in parallel. In addition, SWNT tips exhibited superior resolution compared to conventional tips when imaging biological nanostructures, such as double-stranded DNA. The potential and future challenges of SWNT tips are discussed.

Growth and fabrication with single-walled carbon nanotube probe microscopy tips

Single-walled carbon nanotube (SWNT) probe microscopy tips were grown by a surface growth chemical vapor deposition method. Tips consisting of individual SWNTs (1.5–4 nm in diameter) and SWNT bundles (4–12 nm in diameter) have been prepared by design through variations in the catalyst and growth conditions. In addition to high-resolution imaging, these tips have been used to fabricate SWNT nanostructures by spatially controlled deposition of specific length segments of the nanotube tips.

Plasmonic Bowtie Nanolaser Arrays

Plasmonic lasers exploit strong electromagnetic field confinement at dimensions well below the diffraction limit. However, lasing from an electromagnetic hot spot supported by discrete, coupled metal nanoparticles (NPs) has not been explicitly demonstrated to date. We present a new design for a room-temperature nanolaser based on three-dimensional (3D) Au bowtie NPs supported by an organic gain material. The extreme field compression, and thus ultrasmall mode volume, within the bowtie gaps produced laser oscillations at the localized plasmon resonance gap mode of the 3D bowties. Transient absorption measurements confirmed ultrafast resonant energy transfer between photoexcited dye molecules and gap plasmons on the picosecond time scale. These plasmonic nanolasers are anticipated to be readily integrated into Si-based photonic devices, all-optical circuits, and nanoscale biosensors.