Kohei Imura

Near-field optical imaging of plasmon modes in gold nanorods

We have investigated optical properties of single gold nanorods by using an apertured-type scanning near-field optical microscope. Near-field transmission spectrum of single gold nanorod shows several longitudinal surface plasmon resonances. Transmission images observed at these resonance wavelengths show oscillating pattern along the long axis of the nanorod. The number of oscillation increases with decrement of observing wavelength. These spatial characteristics were well reproduced by calculated local density-of-states maps and were attributed to spatial characteristics of plasmon modes inside the nanorods. Dispersion relation for plasmons in gold nanorods was obtained by plotting the resonance frequencies of the plasmon modes versus the wave vectors obtained from the transmission images.

Photoluminescence from gold nanoplates induced by near-field two-photon absorption

We have investigated two-photon-induced photoluminescence (PL) properties of single gold nanoplates by using an apertured scanning near-field optical microscope. The nanoplates show PL much stronger than nanorods. The near-field PL images show characteristic spatial features, which depend on the incident polarization. These PL images are in good agreement with the calculated spatial distribution of the electric fields adjacent to the particles at the excitation wavelength. We attribute the observed images to spatial characteristics of plasmon modes.

Near-field Raman imaging and electromagnetic field confinement in the self-assembled monolayer array of gold nanoparticles.

Spatial distribution of surface enhanced Raman activity is visualized for two-dimensional (2D) nearly close-packed and well-ordered monolayer array of gold nanoparticles by using scanning near-field optical microscope. The 2D arrays exhibit highly nonuniform enhancement in Raman scattering, i.e., the regions along the edge of the 2D array are preferentially enhanced. We demonstrate that the spatial distribution of the localized electric field is also nonuniform and agrees well with that of the Raman enhancement.

Time-resolved scanning near-field optical microscopy with supercontinuum light pulses generated in microstructure fiber

A novel apparatus for time-resolved near-field optical microscopy is described. The apparatus consists of a mode-locked Ti:sapphire laser, a microstructure fiber, and a scanning near-field optical microscope equipped with an apertured optical fiber probe. The probe pulses in visible to near-infrared regions are generated by focusing laser pulses in the microstructure fiber. The broadband continuum can be used as a wavelength-tunable light source for fluorescence excitation as well as for probing absorption of excited states at arbitrary wavelengths by applying pump-probe scheme, in high spatial-resolution (∼100 nm) predominantly determined by the aperture size of the tip. Time resolution obtained with 740–830 nm probe pulses was in 1–2 ps range, while that with 570 nm pulses was 5 ps without precompensation of the group delay dispersion for the probe pulses. Results on the excited-state dynamics of molecular aggregates are presented.

Reciprocity in scanning near-field optical microscopy: illumination and collection modes of transmission measurements

We experimentally investigated the reciprocity of scanning near-field optical microscopy between illumination and collection modes. Near-field transmission images of single gold spheres and nanorods observed by the two modes are found to be equivalent to each other in the region from visible to near infrared. This result shows that reciprocity holds for the near-field scattering problems. We found that the conventional optical selection rule for far-field excitations does not apply not only under illumination mode but also with collection-mode arrangements. The possible origin of this observation might be the near-field probe.

Anomalous light transmission from plasmonic-capped nanoapertures

We report an anomalous light transmission phenomenon for a nanoaperture on an opaque screen when the aperture is covered with an opaque cap. In conventional optics, light transmission must decrease when the aperture is capped. However, we found that light transmission is enhanced when the nanodisk is in close proximity to the aperture at a wavelength close to the plasmon resonance. This effect even occurs when the disk is larger than the aperture.

Raman and near‐field spectroscopic study on localized surface plasmon excitation from the 2D nanostructure of gold nanoparticles

We have studied electromagnetic field on the surface of two‐dimensional nanostructure of gold nanoparticles through two‐photon–induced photoluminescence images by using scanning near‐field optical microscope and far‐field surface‐enhanced Raman scattering measurements. The near‐field two‐photon–induced photoluminescence image shows that strong inhomogeneous enhancement in two‐photon–induced photoluminescence occurs over the two‐dimensional nanostructure, representing localized surface plasmon excitations. The results suggest that the local structure of the two‐dimensional nanostructure influences the distribution of localized surface plasmon excitation.

Plasmon modes in single gold nanodiscs

Optical properties of single gold nanodiscs were studied by scanning near-field optical microscopy. Near-field transmission spectra of a single nanodisc exhibited multiple plasmon resonances in the visible to near-infrared region. Near-field transmission images observed at these resonance wavelengths show wavy spatial features depending on the wavelength of observation. To clarify physical pictures of the images, theoretical simulations based on spatial correlation between electromagnetic fundamental modes inside and outside of the disc were performed. Simulated images reproduced the observed spatial structures excited in the disc. Mode-analysis of the simulated images indicates that the spatial features observed in the transmission images originate mainly from a few fundamental plasmon modes of the disc.

Near-Field Optical Imaging of Nanoscale Optical Fields and Plasmon Waves

Near-field optical microscopy enables spectroscopic and imaging measurements with a spatial resolution far beyond the diffraction limit of light. We show in this review that spatial structures of plasmonic wavefunctions and those of enhanced optical fields are visualized by near-field spectroscopic imaging for gold nanoparticles and their assemblies. A simple formulation for the optical observation of wavefunctions of oscillating polarization modes in nanomaterials is given. We will introduce experimental methods for near-field linear transmission and nonlinear two-photon excitation measurements. We will demonstrate that the wavefunctions of surface plasmons resonant with the incident wavelength are visualized by the near-field methods for gold nanorods. In addition, we will also show for aggregated gold nanospheres that an enhanced optical field is localized in the interstitial gaps between the particles by near-field two-photon excitation measurements.

Sub-20-fs Time-Resolved Measurements in an Apertured Near-Field Optical Microscope Combined with a Pulse-Shaping Technique

We have constructed an ultrafast near-field optical microscope system with near-field pump/probe pulses with a 17 fs duration at the probe tip. The dispersion effects arising from the optical components, especially from the optical fiber, were removed by a pulse-shaping system that consists of passive and adaptive group-velocity dispersion compensators. With this apparatus, we succeeded in measuring dephasing in a single gold nanostructure with a time constant on the order of 10 fs.