Shaolong Tie

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

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.

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

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.

Polarization beam splitters, converters and analyzers based on a metasurface composed of regularly arranged silicon nanospheres with controllable coupling strength

A metasurface composed of regularly arranged silicon (Si) nanospheres (NSs) with coupling was investigated both theoretically and numerically based on the Mie theory, the simple Lorentz line shape model and the finite-difference time-domain technique. By deliberately controlling the coupling strength between Si NSs through the design of the lattice constants of a rectangular lattice, polarization beam splitters, converters and analyzers with good performance can be successfully constructed. A square lattice as well as a large incidence angle was employed to build the polarization beam splitters and converters. At an incidence angle of 80°, the polarization beam splitters can completely reflect the s-polarized light and transmit the p-polarized light in a wavelength region of 510-620 nm. For a circularly polarized light incident on the polarization converters, one can get s-polarized light in the reflection direction and p-polarized light in the transmission direction. For the polarization beam analyzers, a rectangular lattice with deliberately chosen lattice constants was employed and the transmissivity of a linearly polarized light can be continuously adjusted from 0 to ~0.90 by simply rotating the metasurface. We revealed that the broadening of either the electric dipole resonance or the magnetic dipole resonance or both of them, which is induced by the asymmetric coupling of Si NSs, is responsible for the modification in the transmissivity spectrum of the metasurface. Our findings provide a guideline for designing photonic devices based on the metasurfaces composed of Si NSs with controllable coupling strength.

Controllable color display induced by excitation-intensity-dependent competition between second and third harmonic generation in ZnO nanorods

We investigated the second and third harmonic generation (SHG and THG) in ZnO nanorods (NRs) by using a femtosecond laser (optical parametric amplifier with tunable wavelengths) with a long excitation wavelength of 1350 nm and a low repetition rate of 1 kHz. The damage threshold for ZnO NRs in this case was sufficiently large, enabling us to observe the competition between SHG and THG. The transition from red to blue emission and the mixing of red and blue light with different ratios were successfully demonstrated by simply varying excitation intensity, implying the potential applications of ZnO NRs in all-optical display.

Competition between second harmonic generation and two-photon-induced luminescence in single, double and multiple ZnO nanorods

The nonlinear optical properties of single, double and multiple ZnO nanorods (NRs) were investigated by using a focused femtosecond (fs) laser beam. The excitation wavelength of the fs laser was intentionally chosen to be 754 nm at which the energy of two photons is slightly larger than that of the exciton ground state but smaller than the bandgap energy of ZnO. Second harmonic generation (SHG) or/and two-photon-induced luminescence (TPL) were observed and their dependences on excitation density were examined. For single ZnO NRs, only SHG was observed even at the highest excitation density we used in the experiments. The situation was changed when the joint point of two ZnO NRs perpendicular to each other was excited. In this case, TPL could be detected at low excitation densities and it increased rapidly with increasing excitation density. At the highest excitation density of ~15 MW/cm(2), the intensity of the TPL became comparable to that of the SHG. For an ensemble of ZnO NRs packed closely, a rapid increase of TPL with a slope of more than 7.0 and a gradual saturation of SHG with a slope of ~0.34 were found at high excitation densities. Consequently, the nonlinear response spectrum was eventually dominated by the TPL at high excitation densities and the SHG appeared to be very weak. We interpret this phenomenon by considering both the difference in electric field distribution and the effect of heat accumulation. It is suggested that the electric field enhancement in double and multiple NRs plays a crucial role in determining the nonlinear response of the NRs. In addition, the reduction in the bandgap energy induced by the heat accumulation effect also leads to the significant change in nonlinear response. This explanation is supported by the calculation of the electric field distribution using the discrete dipole approximation method and the simulation of temperature rise in different ZnO NRs based on the finite element method.

Numerical study of nanoparticle sensors based on the detection of the two-photon-induced luminescence of gold nanorod antennas

We investigate numerically the modification of the nonlinear optical properties of a nanoantenna in the trapping of nanoparticles (NPs) by using both the discrete dipole approximation method and the finite-difference time-domain technique. The nanoantenna, which is formed by two gold nanorods (GNRs) aligned end to end and separated by a small gap, can emit strong two-photon-induced luminescence (TPL) under the excitation of a femtosecond laser light which is resonant with its longitudinal surface plasmon resonance. In addition, the excited antenna can stably trap small NPs which in turn induce modifications in the emitted TPL. These two features make it a promising candidate for building highly sensitive detectors for NPs of different materials and sizes. It is demonstrated that sensors built with antennas possess higher sensitivities than those built with single GNRs and nanorod-based antennas are more sensitive than nanoprism-based antennas. In addition, it is found that the trapping probability for a second NP is significantly reduced for the antenna with a trapped NP, implying that trapping of NPs may occur sequentially. A relationship between the TPL of the system (antenna + NP) and the optical potential energy of the NP is established, enabling the extraction of the information on the optical potential energy and optical force by recording the TPL of the system. It is shown that the sequential trapping and releasing of NPs flowing in a microfluid channel can be realized by designing two different antennas arranged closely.

Hot-electron intraband luminescence from GaAs nanospheres mediated by magnetic dipole resonances

Significantly enhanced electric field in plasmonic hot spots can dramatically increase the linear and nonlinear absorption of light, leading to a high-temperature electron gas which radiates, through mainly intraband transition, a broadband luminescence quite similar to blackbody radiation. Here, we demonstrate that such hot-electron intraband luminescence (HEIL) can also be achieved by exploiting the significantly enhanced electric field at the magnetic dipole resonances of gallium arsenide (GaAs) nanospheres (NSs). We show that monocrystalline GaAs NSs with distinct electric and magnetic dipole (ED and MD) resonances can be obtained by using femtosecond laser ablation and annealing. Significantly enhanced second harmonic generation and broadband HEIL are observed when the MD resonances of such GaAs NSs are resonantly excited. The lifetime of the HEIL is found to be as short as ∼82 ps, indicating a significant enhancement in radiative intraband transition rate. We reveal that the slope extracted from the dependence of the HEIL intensity on the irradiance is linearly proportional to the energy of the emitted photon. The existence of distinct ED and MD resonances in combination with a direct bandgap makes GaAs NSs an attractive candidate for constructing novel all-dielectric metamaterials and active photonic devices.

Encoding random hot spots of a volume gold nanorod assembly for ultralow energy memory

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.

Three-photon-induced blue emission with narrow bandwidth from hot flower-like ZnO nanorods.

ZnO nanorods (NRs) self-organized into flowers were synthesized at different temperatures ranging from 100°C to 180°C by using the hydrothermal method. The existence of Zn interstitials (Zn(i)) was confirmed by X-ray photoelectron spectroscopy and a larger amount of Zn(i) was found in the ZnO NRs prepared at higher temperatures. A redshift of the emission peak of more than 15 nm was observed for the ZnO NRs under single photon excitation. The nonlinear optical properties of the flower-like ZnO NRs were characterized by using focused femtosecond laser light and strong three-photon-induced luminescence was observed at an excitation wavelength of ~750 nm. More interestingly, a large redshift of the emission peak was observed with increasing excitation intensity, resulting in efficient blue emission with a narrow bandwidth of ~30 nm. It was confirmed that the large redshift originates from the heating of the ZnO NRs to a temperature of more than 800°C and the closely packed ZnO NRs in the flowers play a crucial role in heat accumulation. The stable and efficient three-photon-induced blue emission from such ZnO NRs may find potential applications in the fields of optical display, high-temperature sensors and light therapy of tumors.

Upconversion luminescence from aluminoborate glasses doped with Tb 3+ , Eu 3+ and Dy 3+ under the excitation of 2.6-μm femtosecond laser pulses

We investigated the upconversion luminescence of three aluminoborate glasses doped with Tb(3+), Eu(3+), and Dy(3+) under the excitation of 2.6-μm femtosecond (fs) laser pulses. Efficient upconversion luminescence appearing in the visible light spectral region was observed in all three glasses and the emission spectra are quite similar to those obtained under single photon excitation. From the dependence of the luminescence intensity on the excitation intensity in the low excitation intensity regime, it was revealed that a four-photon process is involved in the generation of the upconversion luminescence in the Tb(3+)- and Eu(3+)-doped glasses while a mixed two- and three-photon process is involved in the Dy(3+)-doped glass. In the high excitation intensity regime, a reduction of the slope to about 1.0 was observed for all glasses. A physical mechanism based on the super saturation of the intermediate states of the rare-earth ions was employed to interpret the upconversion luminescence under the excitation of long-wavelength fs laser pulses. Significantly broadened luminescence spectra were observed in thick glasses under high excitation intensities and it can be attributed to the self-focusing of the laser beam in the thick glasses.