Two-photon excitation provides a means of activating chemical or physical processes with high spatial resolution in three dimensions and has made possible the development of three-dimensional fluorescence imaging, optical data storage, and lithographic microfabrication. These applications take advantage of the fact that the two-photon absorption probability depends quadratically on intensity, so under tight-focusing conditions, the absorption is confined at the focus to a volume of order λ3 (where λ is the laser wavelength). Any subsequent process, such as fluorescence or a photoinduced chemical reaction, is also localized in this small volume. Although three-dimensional data storage and microfabrication have been illustrated using two-photon-initiated polymerization of resins incorporating conventional ultraviolet-absorbing initiators, such photopolymer systems exhibit low photosensitivity as the initiators have small two-photon absorption cross-sections (δ). Consequently, this approach requires high laser power, and its widespread use remains impractical. Here we report on a class of π;-conjugated compounds that exhibit large δ (as high as 1, 250 × 10−50 cm4 s per photon) and enhanced two-photon sensitivity relative to ultraviolet initiators. Two-photon excitable resins based on these new initiators have been developed and used to demonstrate a scheme for three-dimensional data storage which permits fluorescent and refractive read-out, and the fabrication of three-dimensional micro-optical and micromechanical structures, including photonic-bandgap-type structures.

Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication

Über die Adsorption in Lösungen

Laser-induced periodic surface structures (LIPSS, ripples) are a universal phenomenon and can be generated on almost any material upon irradiation with linearly polarized radiation. With the availability of ultrashort laser pulses, LIPSS have gained an increasing attraction during the past decade, since these structures can be generated in a simple single-step process, which allows a surface nanostructuring for tailoring optical, mechanical, and chemical surface properties. In this study, the current state in the field of LIPSS is reviewed. Their formation mechanisms are analyzed in ultrafast time-resolved scattering, diffraction, and polarization constrained double-pulse experiments. These experiments allow us to address the question whether the LIPSS are seeded via ultrafast energy deposition mechanisms acting during the absorption of optical radiation or via self-organization after the irradiation process. Relevant control parameters of LIPSS are identified, and technological applications featuring surface functionalization in the fields of optics, fluidics, medicine, and tribology are discussed.

Laser-Induced Periodic Surface Structures— A Scientific Evergreen

2D layered materials (2DLMs) are a subject of intense research for a wide variety of applications (e.g., electronics, photonics, and optoelectronics) due to their unique physical properties. Most recently, increasing research efforts on 2DLMs are projected toward the nonlinear optical properties of 2DLMs, which are not only fascinating from the fundamental science point of view but also intriguing for various potential applications. Here, the current state of the art in the field of nonlinear optics based on 2DLMs and their hybrid structures (e.g., mixed-dimensional heterostructures, plasmonic structures, and silicon/fiber integrated structures) is reviewed. Several potential perspectives and possible future research directions of these promising nanomaterials for nonlinear optics are also presented.

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Nonlinear Optics with 2D Layered Materials.

Silicon nanoparticles are of interest for their optical properties, for example, in light scattering. Here, Zywietz et al. achieve the laser printing of silicon nanoparticles on a substrate at predefined positions, and with control over their crystalline phase.

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Laser printing of silicon nanoparticles with resonant optical electric and magnetic responses

Gold (Au) nanoparticles, particularly nanorods, are actively employed as imaging probes because of their special nonblinking and nonbleaching absorption, scattering, and emitting properties that arise from the excitation of surface plasmons. Herein, we report a novel sensing method that detects feature orientation at the nanoscale via the defocused imaging of individual Au nanorods (AuNRs) with an ordinary wide-field optical microscope. By simultaneously recording defocused images and two-photon luminescence intensities for a large number of individual AuNRs, we correlate their defocused images with their three-dimensional spatial orientations. The spatial orientation of many individual AuNRs can be monitored in situ and in real-time within a single frame, enabling its use as a technique for high-throughput sensing. The probe size can be as small as several nanometers, which is highly desirable for minimization of any potential interference from the probe itself. Furthermore, the sensing property is insensitive to the excitation polarization and the distribution of the probe aspect ratio, which allows AuNRs of any length within a proper regime to be used as orientation sensors without changing the laser frequency and polarization. These unique features make the orientation probes proposed here outstanding candidates for optical imaging and sensing in materials science and biological applications.

Three-dimensional Orientation Sensors by Defocused Imaging of Gold Nanorods through an Ordinary Wide-Field Microscope

Effects of catalyst characters on the photocatalytic activity and process of NiO nanoparticles in the degradation of methylene blue

Periodic surface structures with periods as small as about one-tenth of the irradiating femtosecond (fs) laser light wavelength were created on the surface of a titanium (Ti) foil by exploiting laser-induced oxidation and third harmonic generation (THG). They were achieved by using 100-fs laser pulses with a repetition rate of 1 kHz and a wavelength ranging from 1.4 to 2.2 μm. It was revealed that an extremely thin TixOy layer was formed on the surface of the Ti foil after irradiating fs laser light with a fluence smaller than the ablation threshold of Ti, leading to a significant enhancement in THG which may exceed the ablation threshold of TixOy. As compared with Ti, the maximum efficacy factor for TixOy appears at a larger normalized wavevector in the direction perpendicular to the polarization of the fs laser light. As a result, the THG-dominated laser ablation of TixOy induces 100-nm periodic structures parallel to the polarization of the fs laser light. The depth of the periodic structures was found to be ~10 nm by atomic force microscopy and the formation of the thin TixOy layer was verified by energy dispersive X-ray spectroscopy.

Formation of 100-nm periodic structures on a titanium surface by exploiting the oxidation and third harmonic generation induced by femtosecond laser pulses

Data storage with ultrahigh density, ultralow energy, high security, and long lifetime is highly desirable in the 21st century and optical data storage is considered as the most promising way to meet the challenge of storing big data. Plasmonic coupling in regularly arranged metallic nanoparticles has demonstrated its superior properties in various applications due to the generation of hot spots. Here, the discovery of the polarization and spectrum sensitivity of random hot spots generated in a volume gold nanorod assembly is reported. It is demonstrated that the two-photon-induced absorption and two-photon-induced luminescence of the gold nanorods adjacent to such hot spots are enhanced significantly because of plasmonic coupling. The polarization, wavelength, and spatial multiplexing of the hot spots can be realized by using an ultralow energy of only a few picojoule per pulse, which is two orders of magnitude lower than the value in the state-of-the-art technology that utilizes isolated gold nanorods. The ultralow recording energy reduces the cross-talk between different recording channels and makes it possible to realize rewriting function, improving significantly both the quality and capacity of optical data storage. It is anticipated that the demonstrated technology can facilitate the development of multidimensional optical data storage for a greener future.

Encoding Random Hot Spots of a Volume Gold Nanorod Assembly for Ultralow Energy Memory.

The linear and nonlinear optical properties of thin MoS2 layers exfoliated on an Au/SiO2 substrate were investigated both numerically and experimentally. It was found that the MoS2 layers with different thicknesses exhibited different colors on the gold film. The reflection spectra of the MoS2 layers with different thicknesses were calculated by using the finite-difference time-domain technique and the corresponding chromaticity coordinates were derived. The electric field enhancement factors at both the fundamental light and the second harmonic were calculated and the enhancement factors for second harmonic generation (SHG) were estimated for the MoS2 layers with different thicknesses. Different from the MoS2 layers on a SiO2/Si substrate where the maximum SHG was observed in the single-layer MoS2, the maximum SHG was achieved in the 17 nm-thick MoS2 layer on the Au/SiO2 substrate. As compared with the MoS2 layers on the SiO2/Si substrate, a significant enhancement in SHG was found for the MoS2 layers on the Au/SiO2 substrate due to the strong localization of the electric field. More interestingly, it was demonstrated experimentally that optical data storage can be realized by modifying the SHG intensity of a MoS2 layer through thinning its thickness.

Shaolong Tie

Papers

Three-dimensional Orientation Sensors by Defocused Imaging of Gold Nanorods through an Ordinary Wide-Field Microscope

Effects of catalyst characters on the photocatalytic activity and process of NiO nanoparticles in the degradation of methylene blue

Formation of 100-nm periodic structures on a titanium surface by exploiting the oxidation and third harmonic generation induced by femtosecond laser pulses

Encoding Random Hot Spots of a Volume Gold Nanorod Assembly for Ultralow Energy Memory.

Enhanced second harmonic generation of MoS2 layers on a thin gold film.