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.

As one of the most important semiconductors, silicon has been used to fabricate electronic devices, waveguides, detectors, solar cells, etc. However, the indirect bandgap and low quantum efficiency (10−7) hinder the use of silicon for making good emitters. For integrated photonic circuits, silicon-based emitters with sizes in the range of 100−300 nm are highly desirable. Here, we show the use of the electric and magnetic resonances in silicon nanoparticles to enhance the quantum efficiency and demonstrate the white-light emission from silicon nanoparticles with feature sizes of ~200 nm. The magnetic and electric dipole resonances are employed to dramatically increase the relaxation time of hot carriers, while the magnetic and electric quadrupole resonances are utilized to reduce the radiative recombination lifetime of hot carriers. This strategy leads to an enhancement in the quantum efficiency of silicon nanoparticles by nearly five orders of magnitude as compared with bulk silicon, taking the three-photon-induced absorption into account.

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The high spatial frequency periodic structures induced on metal surface by femtosecond laser pulses was investigated experimentally and numerically. It is suggested that the redistribution of the electric field on metal surface caused by the initially formed low spatial frequency periodic structures plays a crucial role in the creation of high spatial frequency periodic structures. The field intensity which is initially localized in the grooves becomes concentrated on the ridges in between the grooves when the depth of the grooves exceeds a critical value, leading to the ablation of the ridges in between the grooves and the formation of high spatial frequency periodic structures. The proposed formation process is supported by both the numerical simulations based on the finite-difference time-domain technique and the experimental results obtained on some metals such as stainless steel and nickel.

We investigate systematically the competition between the second harmonic generation (SHG) and two-photon-induced luminescence (TPL) that are simultaneously present in Au nanoparticles excited by using a femtosecond (fs) laser. For a large-sized (length ~ 800 nm, diameter ~ 200 nm) Au nanorod, the SHG appears to be much stronger than the TPL. However, the situation is completely reversed when the Au nanorod is fragmented into many Au nanoparticles by the fs laser. In sharp contrast, only the TPL is observed in small-sized (length ~ 40 nm, diameter ~ 10 nm) Au nanorods. When a number of the small-sized Au nanorods are optically trapped and fused into a large-sized Au cluster by focused fs laser light, the strong TPL is reduced while the weak SHG increases significantly. In both cases, the morphology change is characterized by scanning electron microscope. In addition, the modification of the scattering and absorption cross sections due to the morphology change is calculated by using the discrete dipole approximation method. It is revealed that SHG is dominant in the case when the scattering is much larger than the absorption. When the absorption becomes comparable to or larger than the scattering, the TPL increases dramatically and will eventually become dominant. Since the relative strengths of scattering and absorption depend strongly on the size of the Au nanoparticles, the competition between SHG and TPL is found to be size dependent.

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.

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.

We propose a numerical method to evaluate the two-photon-induced luminescence (TPL) of single gold nanorods (GNRs). The validity of this method is confirmed by the cos4 α dependence of the TPL of single GNRs on the polarization angle α, which is in good agreement with experimental observations. As comparing with their linear optical properties such as scattering and absorption, the TPL of a single GNR is found to be more sensitive to the change of the surrounding environment. This property is exploited to detect nanoparticles (NPs) approaching the GNR from a far place. By monitoring the evolution of the TPL on the distance between the GNR and a NP, it is possible to extract various information on the NP, including the moving direction, position, size, and material type. For GNRs whose extinction is dominated by absorption, the response and sensitivity are found to depend strongly on their sizes. The detection of the nonlinear optical responses of GNRs may find potential applications in the fields of nanophotonics and biophotonics.