Temperature-dependent photoluminescence properties of single defects in AlGaN micropillars.

Single-photon emitters (SPEs) are attractive as integrated platforms for quantum applications in technologically mature wide-bandgap semiconductors since their stable operation at room temperature or even at high temperatures. In this study, we systematically studied the temperature dependence of the SPE in AlGaN micropillar by experiment. The photoluminescence (PL) spectrum, PL intensity, radiative lifetime and second-order autocorrelation function measurements are investigated over the temperature range from 303 to 373 K. The point defects of AlGaN show strong zero phonon line in the wavelength range of 800-900 nm and highly antibunched photon emission even up to 373 K. Our study reveals a possible mechanism for linewidth broadening in AlGaN SPE at high temperatures. This indicates a possible key for on-chip integration applications based on this material operating at high temperatures.

Deciphering the photophysical properties of near-infrared quantum emitters in AlGaN films by transition dynamics.

Point defects in wide bandgap III-nitride semiconductors have been recently reported to be one kind of the most promising near-infrared (NIR) quantum emitters operating at room temperature (RT). But the identification of the point defect species and the energy level structures as well as the transition dynamics remain unclear. Here, the photophysical properties of single-photon emission from point defects in AlGaN films are investigated in detail. According to the first-principles calculations, a three-level model was established to explain the transition dynamics of the quantum emitters. An anti-site nitrogen vacancy complex (VNNGa) was demonstrated to be the most likely origin of the measured emitter since the calculated zero-phonon line (ZPL) and the lifetime of VNNGa in the AlGaN film coincide well with the experimental results. Our results provide new insights into the optical properties and energy level structures of quantum emission from point defects in AlGaN films at RT and establish the foundation for future AlGaN-based on-chip quantum technologies.

Plasmon Enhanced Second Harmonic Generation from ZnO Nanofilms on Vertical Au Nanorod Arrays.

Vertically aligned gold nanorod arrays have attracted much attention for their fascinating optical properties. Different from longitudinal surface plasmon wavelength (LSPW) and edge-to-edge spacing of gold nanorods, the role of gold nanorod diameter in plasmonic enhancement ability of vertical gold nanorod arrays has rarely been explored. In this work, we selected gold nanorods with similar LSPW but two different diameters (22 and 41 nm), the optical properties of which are dominated by absorption and scattering cross sections, respectively. The vertically aligned arrays of these gold nanorods formed by evaporation self-assembly are coupled with nonlinear ZnO nanocrystal films spin-coated on their surfaces. It was found that the gold nanorod array with a larger diameter can enhance the second harmonic generation (SHG) of ZnO nanofilm by a factor of 27.0, while it is about 7.3 for the smaller gold nanorod array. Theoretical simulations indicate that such stronger enhancement of the larger vertical gold nanorod array compared with the smaller one is due to its stronger scattering ability and greater extent of near-field enhancement at SHG fundamental wavelength. Our work shows that the diameter of gold nanorods is also an important factor to be considered in realizing strong plasmon enhancement of vertically aligned gold nanorod arrays.

Polarization control of plasmon-induced transparency in metamaterials with reversibly convertible bright and dark modes.

We numerically demonstrate a Z-shaped metal-based metamaterial to realize an active polarization-controlled plasmon-induced transparency (PIT). The metamaterial unit cell contains two horizontal Au bars and a vertical Au bar. Simply by varying the incident light polarization, a tunable PIT can be achieved due to the reversible conversion of bright and dark modes between the horizontal and vertical Au bars. Moreover, a switchable PIT window modulation can be accomplished via changing the geometrical parameters, and the theoretical fittings according to the coupled Lorentz oscillator model display consistency with the simulated results. Our proposed metamaterials provide a promising strategy for fabricating compact PIT devices such as optical switching, sensing, and selective filters.

Scalable Direct Writing of Lanthanide-Doped KMnF3 Perovskite Nanowires into Aligned Arrays with Polarized Up-Conversion Emission.

The use of one-dimensional nano- and microstructured semiconductor and lanthanide materials is attractive for polarized-light-emission studies. Up-conversion emission from single-nanorod or anisotropic nanoparticles with a degree of polarization has also been discussed. However, microscale arrays of nanoparticles, especially well-aligned one-dimensional nanostructures as well as their up-conversion polarization characterization, have not been investigated yet. Herein, we present a novel and facile paradigm for preparing highly aligned arrays of lanthanide-doped KMnF3 (KMnF3:Ln) perovskite nanowires, which are good candidates for polarized up-conversion emission studies. These perovskite nanowires, with a width of 10 nm and length of a few micrometers, are formed through the oriented attachment of KMnF3:Ln nanocubes along the [001] direction. By the employment of KMnF3:Ln nanowire gel as nanoink, a direct-writing method is developed to obtain diverse types of aligned patterns from the nanoscale to the wafer scale. Up-conversion emissions from the highly aligned nanowire arrays are polarized along the array direction with a polarization degree up to 60%. Taking advantage of microscopic nanowire arrays, these polarized up-conversion emissions should offer potential applications in light or information transportation.

Tuning Plasmonic Enhancement of Single Nanocrystal Upconversion Luminescence by Varying Gold Nanorod Diameter.

Plasmonic enhancement induced by metallic nanostructures is an effective strategy to improve the upconversion efficiency of lanthanide-doped nanocrystals. It is demonstrated that plasmonic enhancement of the upconversion luminescence (UCL) of single NaYF4 :Yb3+ /Er3+ /Mn2+ nanocrystal can be tuned by tailoring scattering and absorption cross sections of gold nanorods, which is synthesized wet chemically. The assembly of the single gold nanorod and single upconversion nanocrystal is achieved by the atomic force microscope probe manipulation. By selecting two kinds of gold nanorods with similar longitudinal surface plasmon resonance wavelength but different diameters (27.3 and 46.7 nm), which extinction spectra are separately dominant by the absorption and scattering, the maximum UCL enhancement by a factor of 110 is achieved with the 46.7 nm-diameter gold nanorod, while it is 19 for the nanorod with the diameter of 27.3 nm. Such strong enhancement with the larger gold nanorod is due to stronger scattering ability and greater extent of the near-field enhancement. The enhanced UCL shows a strong dependence on the excitation polarization relative to the nanorod long axis. Time-resolved measurements and finite-difference time-domain simulations unveil that both excitation and emission processes of UCL are accelerated by the nanorod plasmonic effect.