Improved Q-factors of III-nitride-based photonic crystal nanocavities by optical loss engineering.

III-nitride-based two-dimensional photonic crystal (2D-PhC) cavities with high-quality factors (Q-factors) have a large potential application, however realized Q-factors in the visible wavelength regime have been relatively moderate. In this study, we demonstrate the design and fabrication of 2D-PhC cavities to achieve high Q-factors, especially in the visible range. From the comparison of numerical calculations and the experimental results, we discuss the dominant optical losses that limit the Q-factor of H3-type cavities formed in an Eu,O-codoped GaN film. Based on these results we designed 2D-PhC cavities which can effectively suppress these dominant losses. We fabricated 2D-heterostructures and show a high Q-factor of 10500 at a resonant wavelength of ∼660 nm, which is considerably larger than any existing GaN-based nano/micro-resonators in the visible region. This study provides design guidelines for the realization of high Q-factors in photonic crystal nanocavities based on III-nitride semiconductors.

Electronic Coupling of Highly Ordered Perovskite Nanocrystals in Supercrystals.

Assembled perovskite nanocrystals (NCs), known as supercrystals (SCs), can have many exotic optical and electronic properties different from the individual NCs due to energy transfer and electronic coupling in the dense superstructures. We investigate the optical properties and ultrafast carrier dynamics of highly ordered SCs and the dispersed NCs by absorption, photoluminescence (PL), and femtosecond transient absorption (TA) spectroscopy to determine the influence of the assembly on the excitonic properties. Next to a red shift of absorption and PL peak with respect to the individual NCs, we identify signatures of the collective band-like states in the SCs. A smaller Stokes shift, decreased biexciton binding energy, and increased carrier cooling rates support the formation of delocalized states as a result of the coupling between the individual NC states. These results open perspectives for assembled perovskite NCs for application in optoelectronic devices, with design opportunities exceeding the level of NCs and bulk materials.

Nanorod photonic crystal ring resonators.

In this study, we shed light on the properties of a photonic ring resonator made up of a closed array of circular dielectric nanorods arranged periodically in a background material. This type of resonator can reach high-quality factors (Q-factor) for specific transverse-magnetic (TM)-like modes, while maintaining a small footprint. We validate this by full 3D finite difference time domain simulations. The properties of the mode most interesting for applications are determined for various parameters of the resonator for the material parameters of GaN. This study provides design guidelines for the realization of this type of photonic nano-resonator and proposes and analyses two practical implementations.

High-Q 1D rod-based nanocavities.

We report an analysis of one-dimensional rod-based photonic crystal nanocavities. These cavities offer opportunities for dielectric materials which lack a matching low-refractive index substrate or are limited in under-etching possibilities to create slab-based PhC cavities. They offer high theoretical Q-values exceeding 106 for transverse magnetic polarized modes with modal volumes below 2.5(λ/n)3. For practical implementations, we propose embedding these structures in a low-refractive index polymer. An analysis of intentionally introduced variations in a rod diameter reveals which design directions should be followed in order to create cavities that are most robust for fabrication-induced variations.

Direct Visualization and Determination of the Multiple Exciton Generation Rate.

Multiple exciton generation (MEG) takes place in competition to other hot carrier cooling processes. While the determination of carrier cooling rates is well established, direct information on MEG dynamics has been lacking. Here, we present a methodology to obtain the MEG rate directly in the initial ultrafast transient absorption dynamics. This method is most effective to systems with slow carrier cooling rates. Perovskite quantum dots exhibit this property and are used to illustrate this approach. They show a delayed carrier concentration buildup following an excitation pulse above the MEG threshold energy, which is accompanied by a faster carrier relaxation, providing a direct evidence of the MEG process. Numerical modeling within a simple framework of two competing cooling mechanisms allows us to extract the MEG rate and carrier energy cooling rates for this material. The presented methodology could provide new insights in carrier generation physics and valuable information for MEG investigations.

Repairing Nanoparticle Surface Defects.

Solar devices based on semiconductor nanoparticles require the use of conductive ligands; however, replacing the native, insulating ligands with conductive metal chalcogenide complexes introduces structural defects within the crystalline nanostructure that act as traps for charge carriers. We utilized atomically thin semiconductor nanoplatelets as a convenient platform for studying, both microscopically and spectroscopically, the development of defects during ligand exchange with the conductive ligands Na4 SnS4 and (NH4 )4 Sn2 S6 . These defects can be repaired via mild chemical or thermal routes, through the addition of L-type ligands or wet annealing, respectively. This results in a higher-quality, conductive, colloidally stable nanomaterial that may be used as the active film in optoelectronic devices.

Power-dependent spectral shift of photoluminescence from ensembles of silicon nanocrystals.

: Nanocrystals are widely studied for their tunable optical properties, most importantly increased luminescence efficiency and emission energy. Quantum confinement effects are found for many different types of nanocrystals, and these introduce a relation between the emission wavelength and the size of nanocrystals. When ensembles of nanocrystals with a distribution of sizes are studied, this can have profound effects on their luminescence spectra. Here, we show how photoluminescence spectra of ensembles of silicon nanocrystals can shift under different excitation conditions, resulting from differences in absorption cross-section of the individual nanocrystal sizes. This effect, together with the fact that after a pulsed excitation a silicon nanocrystal can only emit a single photon, determines how the distribution of excited nanocrystals changes and leads to the spectral shift for different excitation powers. Next to this effect, the influence of different radiative rates in such ensembles is also addressed. These notions are important for the interpretation of photoluminescence data for silicon nanocrystals but can be extended to any nanoparticle system comprising size-distributed ensembles.