Nanoscopic observation of chiro-optical phenomena is an intriguing scientific topic but have large difficulties in the measurements, and hence the physics is still largely unexplored. So far, the chiro-optical physics have not been well unveiled; conventionally, those phenomena have been investigated only through indirect information from the macroscopic far-field optical measurements and/or predictions by theoretical simulations. To fully understand and to utilize the full potential of chiro-optical systems, the local in-situ observation of the effects from individual components is essential, as the macroscopic chiro-optical effect is not straightforward for the analysis of the microscopic phenomena. In the present study, we attempted the imaging of the chiro-optical forces confined in the nanospaces based on a photoinduced force microscopy. On the right-handed gammadion structure, the strong optical gradient force appeared at the edges of the structure under illumination of LCP light at 785 nm. The left-handed gammadion gave the similar result under RCP illumination. This research paves the way for clarifying the physics of nanoscale chiro-optics and application of that.
The chiro-optical effects are measured through the spectroscopic methods typified by optical rotation (OR) and circular dichroism
(CD). The chiro-optical effect can also appear as the motion of the chiral particles illuminated by the circularly polarized light. When a
chiral nanoparticle is optically trapped using a circularly polarized laser beam, the circular polarization (CP) dependent gradient force is
expected to be induced on the particle. We investigated the CP-dependent gradient force for the three-dimensionally chiral
nanoparticles. The experimental result showed that the gradient force depended on the handedness of CP (left- or right-handed) of the
trapping light as well as on the handedness of the particle chirality. The extended aspect of the chiral optical force obtained here can
give us novel methodologies for the researches of chirality sensing, manipulation, separation, enantio-selective biological reaction.
Optical trapping of nanoparticles is realized by optical gradient force originated from the intensity gradient of light with a focused beam. It is expected that the gradient force depending on the circular polarization (CP) acts on particles with chiral structures. Here, we investigate the CP-dependent gradient force on the chiral gold nanoparticles. We found that the amplitude (dispersion of the position of the Brownian motion) depends on the handedness of the incident light in both cases of D- and L-form particles. Based on the results on the gradient force for the chiral particles, it is expected that chiral nanomaterials can be handled by the circularly polarized light.
We demonstrate here that control of local optical field near a single non-chiral gold nano-rectangle irradiated with linearly polarized light is possible from linearly polarized to nearly pure left- or right-handed circular polarization, by adjusting the angle of the incident polarization relative to the rectangle.
Chiral nanostructures exhibiting circular dichroism (CD) activities absorb different amounts of left- (LCP) and righthanded circularly polarized (RCP) light. Here, we report the observation of dissymmetry between two-photon-induced LCP and RCP photoluminescence (TPIPL) from two-dimensional (2D) chiral plasmonic nanostructures. Under linearly polarized ultrashort pulse irradiation with a low input power of 3 mW, the excited multipolar responses of the 2D chiral nanostructure yield circularly polarized TPIPL. The handedness of the circularly polarized TPIPL was dependent on the handedness of the chiral nanostructure. The chiral nature of TPIPL may find potential applications in sensing of chiral molecules and materials.
KEYWORDS: Polarization, Near field, Gold, Plasmons, Nanostructuring, Near field scanning optical microscopy, Near field optics, Nanostructures, Nanomaterials, Plasmonics, Optical microscopy, Polarimetry
We experimentally demonstrate that non-chiral plasmonic nanostructured materials interacting with linearly polarized
(non-chiral) light generate elliptically polarized (chiral) optical near-fields in local nano spaces around the materials.
We report in this paper the near-field microscopic studies on localized plasmon resonances in gold nanoparticles and
their assemblies (nanorods, triangular nanoplates, and assembled nanospheres). We have utilized near-field
measurements of linear transmission/scattering, as well as nonlinear two-photon excitation, to enable spectroscopic
imaging of local electric field or local density of electromagnetic states. We show that the wavefunction of the plasmon
excitation in the nanoparticle is visualized by the near-field methods. For single nanorod, many plasmon resonances
were observed in the near-field transmission spectrum. At each resonant peak wavelength, the near-field image of the
nanorod gave a characteristic spatially oscillating feature along the long axis of the nanorod. The feature is attributable
to the square modulus of the resonant plasmon-mode wavefunction. In the assembled nanoparticles, strong electric-field
enhancement localized in the interstitial sites ("hot spot"), which was theoretically predicted previously, was clearly
imaged by the near-field two-photon excitation method. Major contribution of the hot spots to surface enhanced Raman
scattering is also shown for the samples weakly doped with Raman-active dye molecules, by the near-field excited
Raman spectra and images.
KEYWORDS: Gold, Near field, Surface plasmons, Near field scanning optical microscopy, Nanoparticles, Plasmons, Near field optics, Electromagnetism, Ultrafast imaging, Nanorods
We investigated near-field optical properties and images of single gold nanorods by using a near-field optical
microscope. Observed transmission spectra show distinct transverse and longitudinal surface plasmon resonances.
Transmission images observed near the surface plasmon resonances agree qualitatively with calculated maps of optical
local density-of-states, and are assignable to plasmon wavefunctions. Ultrafast temporal responses in the single gold
nanoparticles were observed by combining a near-field microscope with time-resolved techniques. Observed transient
transmission images of the single nanorods show characteristic optical features, and are in good agreement with a
calculated map of variation of local density of states arising from the elevation of electronic temperature in the nanorod
induced by photoexcitation.
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