Tuning the Photoluminescence Anisotropy of Semiconductor Nanocrystals.

Semiconductor nanocrystals are promising optoelectronic materials. Understanding their anisotropic photoluminescence is fundamental for developing quantum-dot-based devices such as light-emitting diodes, solar cells, and polarized single-photon sources. In this study, we experimentally and theoretically investigate the photoluminescence anisotropy of CdSe semiconductor nanocrystals with various shapes, including plates, rods, and spheres, with either wurtzite or zincblende structures. We use defocused wide-field microscopy to visualize the emission dipole orientation and find that spheres, rods, and plates exhibit the optical properties of 2D, 1D, and 2D emission dipoles, respectively. We rationalize the seemingly counterintuitive observation that despite having similar aspect ratios (width/length), rods and long nanoplatelets exhibit different defocused emission patterns by considering valence band structures calculated using multiband effective mass theory and the dielectric effect. The principles are extended to provide general relationships that can be used to tune the emission dipole orientation for different materials, crystalline structures, and shapes.

Modulation of Cathodoluminescence by Surface Plasmons in Silver Nanowires.

The waveguide modes in chemically-grown silver nanowires on silicon nitride substrates are observed using spectrally- and spatially-resolved cathodoluminescence (CL) excited by high-energy electrons in a scanning electron microscope. The presence of a long-range, travelling surface plasmon mode modulates the coupling efficiency of the incident electron energy into the nanowires, which is observed as oscillations in the measured CL with the point of excitation by the focused electron beam. The experimental data are modeled using the theory of surface plasmon polariton modes in cylindrical metal waveguides, enabling the complex mode wavenumbers and excitation strength of the long-range surface plasmon mode to be extracted. The experiments yield insight into the energy transfer mechanisms between fast electrons and coherent oscillations in surface charge density in metal nanowires and the relative amplitudes of the radiative processes excited in the wire by the electron.

Memory in quantum dot blinking.

The photoluminescence intermittency (blinking) of quantum dots is interesting because it is an easily measured quantum process whose transition statistics cannot be explained by Fermi's golden rule. Commonly, the transition statistics are power-law distributed, implying that quantum dots possess at least trivial memories. By investigating the temporal correlations in the blinking data, we demonstrate with high statistical confidence that there is nontrivial memory between the on and off brightness duration data of blinking quantum dots. We define nontrivial memory to be statistical complexity greater than one. We show that this memory cannot be discovered using the transition distribution. We show by simulation that this memory does not arise from standard data manipulations. Finally, we conclude that at least three physical mechanisms can explain the measured nontrivial memory: (1) storage of state information in the chemical structure of a quantum dot; (2) the existence of more than two intensity levels in a quantum dot; and (3) the overlap in the intensity distributions of the quantum dot states, which arises from fundamental photon statistics.

Macroporous perovskite nanocrystal composites for ultrasensitive copper ion detection.

Accumulation of heavy metal ions, including copper ions (Cu2+), presents a serious threat to human health and to the environment. A substantial amount of research has focused on detecting such species in aqueous solutions. However, progress towards ultrasensitive and easy-to-use sensors for non-aqueous solutions is still limited. Here, we focus on the detection of copper species in hexane, realising ultra-sensitive detection through a fluorescence-based approach. To achieve this, a novel macroporous composite material has been developed featuring luminescent CsPbBr3 nanocrystals (NCs) chemically adhered to a polymerized high internal phase emulsion (polyHIPE) substrate through surface thiol groups. Due to this thiol functionality, sub-monolayer NC formation is realised, which also renders outstanding stability of the composite in the ambient environment. Copper detection is achieved through a direct solution based immersion of the CsPbBr3-(SH)polyHIPE composite, which results in concentration-dependent quenching of the NC photoluminescence. This newly developed sensor has a limit of detection (LOD) for copper as low as 1 × 10-16 M, and a wide operating window spanning 10-2 to 10-16 M. Moreover, the composite exhibits excellent selectivity among different transition metals.

Quasiperiodic light.

Quasiperiodicity is a form of spatial order that has been observed in quasicrystalline matter but not light. We construct a quasicrystalline surface out of a light emitting diode. Using a nanoscale waveguide as a microscope (NSOM), we directly image the light field at the surface of the diode. Here we show, using reciprocal space representations of the images, that the light field is quasiperiodic. We explain the structure of the light field with wave superposition. Periodic ordering is limited to at most six-fold symmetry. The light field exhibits 12-fold quasisymmetry, showing order while disproving periodicity. This demonstrates that a new class, consisting of projections from hyperspace, exists in the taxonomy of light ordering.

Two Mechanisms Determine Quantum Dot Blinking.

Many potential applications of quantum dots (QDs) can only be realized once the luminescence from single nanocrystals (NCs) is understood. These applications include the development of quantum logic devices, single-photon sources, long-life LEDs, and single-molecule biolabels. At the single-nanocrystal level, random fluctuations in the QD photoluminescence occur, a phenomenon termed blinking. There are two competing models to explain this blinking: Auger recombination and surface trap induced recombination. Here we use lifetime scaling on core-shell chalcogenide NCs to demonstrate that both types of blinking occur in the same QDs. We prove that Auger-blinking can yield single-exponential on/off times in contrast to earlier work. The surface passivation strategy determines which blinking mechanism dominates. This study summarizes earlier studies on blinking mechanisms and provides some clues that stable single QDs can be engineered for optoelectronic applications.

Tuning Single Quantum Dot Emission with a Micromirror.

The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.

[The electroluminescence spectra of InGan/GaN blue LEDs during aging time].

The luminescence spectra of InGaN/GaN multiple quantum wells light-emitting diodes under low level injection current (<4 mA) during aging process was investigated for the first time. Comparing the electroluminescence (EL) spectra of LEDs before and after aging time it was found that the peak wavelength and the full width at half maximum (FWHM) decreased with stress time and the changes of EL spectrum had two different stages-drastic decrease at the early stress stage and slow decrease later showing the same trend with the output optical power of LEDs, which indicates that the effective polarization electric field of LEDs becomes weak during the aging process and the change has a clear correlation with the increase of the defects in the multiple quantum wells of LEDs. Electrical measurement revealed that junction capacitance (C(j)) under the same junction voltage (V(j) = 1.8 V) and the junction voltage (V(j)) with the same injection current 1 mA calculated by ac small-signal IV method increased along with aging time, which explicates that the carrier density under the same low injection increases as the aging time increases. Analyses indicate that the polarization field in the quantum well is more seriously screened by the increased carriers captured by defects activated during stress time, the weaker effective polarization electric field makes the tilt of the energy band smaller, the energy radiated through the band edge and the density of energy states of the band edge increase which leads to the behaviors of peak wavelength and the FWHM of InGaN/GaN multiple quantum wells LEDs under low level injection current.

Valence subband coupling effect on polarization of spontaneous emissions from Al-rich AlGaN/AlN quantum wells.

The optical polarization properties of Al-rich AlGaN/AlN quantum wells (QWs) were investigated using the theoretical model based on the k·p method. Numerical results show that there is valence subband coupling which can influence the peak emission wavelength and emission intensity for TE and TM polarization components from Al-rich AlGaN/AlN QWs. Especially the valence subband coupling could be strong enough when CH1 is close to HH1 and LH1 subbands to modulate the critical Al content switching dominant emissions from TE to TM polarization. It is believed that the valence subband coupling may give important influence on polarization properties of spontaneous emissions and should be considered in designing high efficiency AlGaN-based ultraviolet (UV) LEDs.

Enhancement of surface emission in deep ultraviolet AlGaN-based light emitting diodes with staggered quantum wells.

The optical polarization properties of staggered AlGaN-AlGaN/AlN quantum wells (QWs) are investigated using the theoretical model based on the k·p method. The numerical results show that the energy level order and coupling relation of the valence subband structure change in the staggered QWs and the trend is beneficial to TE polarized transition compared to that of conventional AlGaN/AlN QWs. As a result, the staggered QWs have much stronger TE-polarized emission than conventional AlGaN-based QWs, which can enhance the surface emission of deep ultraviolet (DUV) light-emitting diodes (LEDs). The polarization control by using staggered QWs can be applied in high efficiency DUV AlGaN-based LEDs.