Chirality enhancement using topology-designed 3D nanophotonic antennas

We explore chiroptical phenomena in 3D chiral nano-gap antennas using topology optimization. The characteristic helical geometries of the topology-designed antennas exhibit giant chiral dissymmetry (g=-1.70) considering the gap intensity, circular-to-linear polarization conversion, and circularly polarized light emission from a linear dipole coupled with the antenna. We observed that the spin angular momentum of light, flowing into the nanogap with opposite signs, locally amplifies optical chirality. These findings carry profound implications for the nanoscale control of complex light-matter interactions with structured light

Multiphoton-excited DUV photolithography for 3D nanofabrication

Light-matter interactions in the deep ultraviolet (DUV) wavelength region exhibits a variety of optical effects such as luminescence, photoisomerization, and polymerization in many materials. Despite the rich photochemistry and high spatial resolution due to the short wavelength, the notorious lack of DUV-compatible optical components and devices precludes use of DUV light in microscopy and lithography as a routine laboratory tool. Here, we present the use of two-photon excitation with visible laser light to realizes photo-polymerization of molecules with an excitation energy equivalent to DUV light. Using standard optics for visible light, methacrylate oligomers were polymerized with 400 nm femtosecond pulses without any addition of photo-initiators and sensitizers. By scanning the laser focus in 3D, a series of fine 3D structures were created with the smallest resolved line-space features of 80 nm. We found DUV polymerizations induced by two-photon absorption is surprisingly efficient and requires laser intensity only on the order of 100 kW/cm^2. With the variety of successful demonstrations including organic- and inorganic-material-made-structures presented, our direct nano-3D-printing method would be a valuable tool for nanofabrication in 3D

Quantitative Evaluation of Surface-Enhanced Raman Scattering Nanoparticles for Intracellular pH Sensing at a Single Particle Level

Intracellular pH is one of the key factors for understanding various biological processes in biological cells. Plasmonic gold and silver nanoparticles (NPs) have been extensively studied for surface-enhanced Raman scattering (SERS) applications for pH sensing as a local pH probe in a living cell. However, the SERS performance of NPs depends on material, size, and shape, which can be controlled by chemical synthesis. Here, we synthesized 18 types of gold and silver NPs with different morphologies such as sphere, rod, flower, star, core/shell, hollow, octahedra, core/satellites, and chainlike aggregates, and quantitatively compared their SERS performance for pH sensing. The SERS intensity from the most commonly utilized SERS probe molecule (para-mercaptobenzoic acid, p-MBA) for pH sensing was measured at the single nanoparticle level under the same measurement parameters such as low laser power (0.5 mW/μm2), short integration time (100 ms) at wavelengths of 405, 488, 532, 584, 676, and 785 nm. In our measurement, the Ag chain, Ag core/satellites, Ag@Au core/satellites, and Au core/satellites nanoassemblies showed efficient pH sensing at the single particle level. By using p-MBA-conjugated Au@Ag core/satellites, we performed time-lapse pH measurements during apoptosis of HeLa cells. These experimental results confirmed that the pH measurement using p-MBA-conjugated Au@Ag core/satellites can be applied for long-term measurements of intracellular pH during cellular events

Indium for Deep-Ultraviolet Surface-Enhanced Resonance Raman Scattering

The dielectric constant of indium in the deep-ultraviolet (DUV) region satisfies the conditions for localized surface plasmon resonance with low absorption loss. We report that indium acts as an agent of efficient surface-enhanced resonance Raman scattering (SERRS) in the DUV. Indium-coated SERRS substrates were prepared by depositing indium on fused silica glass substrates with control of the deposition thickness to tailor the plasmon resonance in the DUV. With excitation at 266 nm, SERRS was observed from thin adenine films deposited on the indium-coated substrates, and the signal intensity was up to 11 times higher than that of a bare fused silica glass substrate. FDTD calculations showed that an enhanced electromagnetic field can be locally generated on the indium-coated substrates. Considering the volume of the enhanced field region in the excitation spot, we estimated the average enhancement factor to be 10² or higher. Our results indicate that indium is a promising and easy-to-use metal for efficiently exciting DUV-SERRS of samples containing a small number of molecules