Photothermal heterodyne imaging of micron-sized objects.

Micron-sized dye-doped polymer beads were imaged using transmitted/reflected light microscopy and photothermal heterodyne imaging (PHI) measurements. The transmitted/reflected light images show distinct ring patterns that are attributed to diffraction effects and/or internal reflections within the beads. In the PHI experiments pump laser induced heating changes the refractive index and size of the bead, which causes changes in the diffraction pattern and internal reflections. This creates an analogous ring pattern in the PHI images. The ring pattern disappears in both the reflected light and PHI experiments when an incoherent light source is used as a probe. When the beads are imaged in an organic medium heat transfer changes the refractive index of the environment, and gives rise to a ring pattern external to the beads in the PHI images. This causes the beads to appear larger than their physical dimensions in PHI experiments. This external signal does not appear when the beads are imaged in air because the refractive index changes in air are very small.

Chemical interface damping for propagating surface plasmon polaritons in gold nanostripes.

Leakage radiation microscopy has been used to examine chemical interface damping (CID) for the propagating surface plasmon polariton (PSPP) modes of Au nanostripes-nanofabricated structures with heights of 40 or 50 nm, widths between 2 and 4 µm, and 100 µm lengths. Real space imaging was used to determine the propagation lengths LSPP of the leaky PSPP modes, and back focal plane measurements generated ω vs k dispersion curves, which yield the PSPP group velocities vg. The combination of these two experiments was used to calculate the PSPP lifetime via T1 = LSPP/vg. The difference in T1 times between bare and thiol coated nanostripes was used to determine the dephasing rate due to CID ΓCID for the adsorbed thiol molecules. A variety of different thiol molecules were examined, as well as nanostripes with different dimensions. The values of ΓCID are similar for the different systems and are an order-of-magnitude smaller than the typical values observed for the localized surface plasmon resonances (LSPRs) of Au nanoparticles. Scaling the measured ΓCID values by the effective path length for electron-surface scattering shows that the CID effect for the PSPP modes of the nanostripes is similar to that for the LSPR modes of nanoparticles. This is somewhat surprising given that PSPPs and LSPRs have different properties: PSPPs have a well-defined momentum, whereas LSPRs do not. The magnitude of ΓCID for the nanostripes could be increased by reducing their dimensions, principally the height of the nanostructures. However, decreasing dimensions for the leaky PSPP mode increases radiation damping, which would make it challenging to accurately measure ΓCID.

Making waves: Radiation damping in metallic nanostructures.

Metal nanostructures display several types of resonances. In the visible and near-IR spectral regions, there are localized surface plasmon resonances (LSPRs) that involve the coherent oscillation of the conduction electrons. Extended metal nanostructures, such as nanowires or nanoplates, also exhibit propagating surface plasmon polaritons (PSPPs), which are motions of the electrons at the surface of the structure that have a well-defined momentum. In addition, the vibrational normal modes of metal nanostructures give rise to low frequency resonances in the gigahertz to terahertz range. These different types of motions/resonances suffer energy losses from internal effects and from interactions with the environment. The goal of this perspective is to describe the part of the energy relaxation process due to the environment. Even though the plasmon resonances and acoustic vibrational modes arise from very different physics, it turns out that environmental damping is dominated by radiation of waves. The way the rates for radiation damping depend on the size of the nanostructure and the properties of the environment will be discussed for the different processes. For example, it is well known that for LSPRs, the rate of radiation damping increases with particle size. However, the radiation damping rate decreases with increasing dimensions for PSPPs and for the acoustic vibrational modes.

Ultrafast measurements of the dynamics of single nanostructures: a review.

The ability to study single particles has revolutionized nanoscience. The advantage of single particle spectroscopy measurements compared to conventional ensemble studies is that they remove averaging effects from the different sizes and shapes that are present in the samples. In time-resolved experiments this is important for unraveling homogeneous and inhomogeneous broadening effects in lifetime measurements. In this report, recent progress in the development of ultrafast time-resolved spectroscopic techniques for interrogating single nanostructures will be discussed. The techniques include far-field experiments that utilize high numerical aperture (NA) microscope objectives, near-field scanning optical microscopy (NSOM) measurements, ultrafast electron microscopy (UEM), and time-resolved x-ray diffraction experiments. Examples will be given of the application of these techniques to studying energy relaxation processes in nanoparticles, and the motion of plasmons, excitons and/or charge carriers in different types of nanostructures.

Strong Exciton-Plasmon Coupling in Silver Nanowire Nanocavities.

The interaction between plasmonic and excitonic systems and the formation of hybridized states is an area of intense interest due to the potential to create exotic light-matter states. We report herein coupling between the leaky surface plasmon polariton (SPP) modes of single Ag nanowires and excitons of a cyanine dye (TDBC) in an open nanocavity. Silver nanowires were spin-cast onto glass coverslips, and the wavevector of the leaky SPP mode was measured by back focal plane (BFP) microscopy. Performing these measurements at different wavelengths allows the generation of dispersion curves, which show avoided crossings after deposition of a concentrated TDBC-PVA film. The Rabi splitting frequencies (Ω) determined from the dispersion curves vary between nanowires, with a maximum value of Ω = 390 ± 80 meV. The experiments also show an increase in attenuation of the SPP mode in the avoided crossing region. The ability to measure attenuation for the hybrid exciton-SPP states is a powerful aspect of these single nanowire experiments because this quantity is not readily available from ensemble experiments.