Enhanced light extraction efficiency of Eu-related emission from a nano-patterned GaN layer grown by MOCVD.

Eu-doped GaN is a promising material for the active layer in red light emitting diodes. Although the output power of LEDs based on GaN:Eu has been increasing by a combination of structural and growth optimizations, there is still a significant limitation resulting from a poor light extraction efficiency, typical for high refractive index materials. Here we studied nanostructuring of the top of the optical active layer by nano-cubes for enhancement of the light extraction efficiency, and its effect on the optical emission characteristics. By etching nano-cubes into the active layer, we observed an increase in directional light output power of Eu3+ ions of up to 60%, as well as a grating effect. Simultaneously, the absorption of excitation light into the optical active layer was improved, leading to a 12.8 times increase of output power per available Eu3+ ion.

Nanophotonics of higher-plant photosynthetic membranes.

The thylakoid membrane inside chloroplasts hosts the light-dependent reactions of photosynthesis. Its embedded protein complexes are responsible for light harvesting, excitation energy transfer, charge separation, and transport. In higher plants, when the illumination conditions vary, the membrane adapts its composition and nanoscale morphology, which is characterized by appressed and non-appressed regions known as grana and stroma lamellae, respectively. Here we investigate the nanophotonic regime of light propagation in chloroplasts of higher plants and identify novel mechanisms in the optical response of the thylakoid membrane. Our results indicate that the relative contributions of light scattering and absorption to the overall optical response of grana strongly depend on the concentration of the light-harvesting complexes. For the pigment concentrations typically found in chloroplasts, the two mechanisms have comparable strengths, and their relative value can be tuned by variations in the protein composition or in the granal diameter. Furthermore, we find that collective modes in ensembles of grana significantly increase light absorption at selected wavelengths, even in the presence of moderate biological disorder. Small variations in the granal separation or a large disorder can dismantle this collective response. We propose that chloroplasts use this mechanism as a strategy against dangerously high illumination conditions, triggering a transition to low-absorbing states. We conclude that the morphological separation of the thylakoid membrane in higher plants supports strong nanophotonic effects, which may be used by chloroplasts to regulate light absorption. This adaptive self-organization capability is of interest as a model for novel bioinspired optical materials for artificial photosynthesis, imaging, and sensing.

Strong infrared photoluminescence in highly porous layers of large faceted Si crystalline nanoparticles.

Almost all physical processes in solids are influenced by phonons, but their effect is frequently overlooked. In this paper, we investigate the photoluminescence of large silicon nanoparticles (approximately 100 nm size, synthesized by chemical vapor deposition) in the visible to the infrared detection range. We find that upon increasing laser irradiance, an enormous photoluminescence emission band appears in the infrared. Its intensity exhibits a superlinear power dependence, increasing over four orders of magnitude in the investigated pump power range. Particles of different sizes as well as different shapes in porous layers are investigated. The results are discussed taking into account the efficient generation of phonons under high-power pumping, and the reduced capability, porosity dependent, of the silicon nanoparticles to exchange energy with each other and with the substrate. Our findings are relevant for heat management strategies in silicon.

Efficient optical extraction of hot-carrier energy.

Light-induced generation of free charge carriers in semiconductors constitutes the physical basis of photodetection and photovoltaics. To maximize its efficiency, the energy of the photons must be entirely used for this purpose. This is highly challenging owing to the ultrafast thermalization of 'hot' carriers, which are created by absorption of high-energy photons. Thermalization leads to heat generation, and hence efficiency loss. To circumvent this, dedicated schemes such as photovoltaic hot-carrier cells are being explored. Here we consider optical extraction of the excess energy of hot carriers by emission of infrared photons, using erbium ions in combination with silicon nanocrystals. We determine the external quantum yield of the infrared photon generation by the erbium ions, and demonstrate that cooling of the hot carriers induces a steep, step-like, increase in erbium-related external quantum yield by up to a factor of 15 towards higher excitation energies. Finally, we comment on the potential of our findings for future photovoltaics in the form of an optical ultraviolet-to-infrared spectral converter.

Optical excitation and external photoluminescence quantum efficiency of Eu³âº in GaN.

We investigate photoluminescence of Eu-related emission in a GaN host consisting of thin layers grown by organometallic vapor-phase epitaxy. By comparing it with a reference sample of Eu-doped Y2O3, we find that the fraction of Eu(3+) ions that can emit light upon optical excitation is of the order of 1%. We also measure the quantum yield of the Eu-related photoluminescence and find this to reach (~10%) and (~3%) under continuous wave and pulsed excitation, respectively.

Silicon quantum dots: surface matters.

Silicon quantum dots (SiQDs) hold great promise for many future technologies. Silicon is already at the core of photovoltaics and microelectronics, and SiQDs are capable of efficient light emission and amplification. This is crucial for the development of the next technological frontiers-silicon photonics and optoelectronics. Unlike any other quantum dots (QDs), SiQDs are made of non-toxic and abundant material, offering one of the spectrally broadest emission tunabilities accessible with semiconductor QDs and allowing for tailored radiative rates over many orders of magnitude. This extraordinary flexibility of optical properties is achieved via a combination of the spatial confinement of carriers and the strong influence of surface chemistry. The complex physics of this material, which is still being unraveled, leads to new effects, opening up new opportunities for applications. In this review we summarize the latest progress in this fascinating research field, with special attention given to surface-induced effects, such as the emergence of direct bandgap transitions, and collective effects in densely packed QDs, such as space separated quantum cutting.

Step-like enhancement of luminescence quantum yield of silicon nanocrystals.

Carrier multiplication by generation of two or more electron-hole pairs following the absorption of a single photon may lead to improved photovoltaic efficiencies and has been observed in nanocrystals made from a variety of semiconductors, including silicon. However, with few exceptions, these reports have been based on indirect ultrafast techniques. Here, we present evidence of carrier multiplication in closely spaced silicon nanocrystals contained in a silicon dioxide matrix by measuring enhanced photoluminescence quantum yield. As the photon energy increases, the quantum yield is expected to remain constant, or to decrease as a result of new trapping and recombination channels being activated. Instead, we observe a step-like increase in quantum yield for larger photon energies that is characteristic of carrier multiplication. Modelling suggests that carrier multiplication is occurring with high efficiency and close to the energy conservation limit.

Red spectral shift and enhanced quantum efficiency in phonon-free photoluminescence from silicon nanocrystals.

Crystalline silicon is the most important semiconductor material in the electronics industry. However, silicon has poor optical properties because of its indirect bandgap, which prevents the efficient emission and absorption of light. The energy structure of silicon can be manipulated through quantum confinement effects, and the excitonic emission from silicon nanocrystals increases in intensity and shifts to shorter wavelengths (a blueshift) as the size of the nanocrystals is reduced. Here we report experimental evidence for a short-lived visible band in the photoluminescence spectrum of silicon nanocrystals that increases in intensity and shifts to longer wavelengths (a redshift) with smaller nanocrystal sizes. This higher intensity indicates an increased quantum efficiency, which for 2.5-nm-diameter nanocrystals is enhanced by three orders of magnitude compared to bulk silicon. We assign this band to the radiative recombination of non-equilibrium electron-hole pairs in a process that does not involve phonons.

Donor-state-enabling Er-related luminescence in silicon: direct identification and resonant excitation.

We conclusively establish a direct link between formation of an Er-related donor gap state and the 1.5 microm emission of Er in Si. The experiment is performed on Si/Si:Er nanolayers where a single type of Er optical center dominates. We show that the Er emission can be resonantly induced by direct pumping into the bound exciton state of the identified donor. Using two-color spectroscopy with a free-electron laser we determine the ionization energy of the donor-state-enabling Er excitation as E(D) approximately 218 meV. We demonstrate quenching of the Er-related emission upon ionization of the donor.

Nanosecond dynamics of the near-infrared photoluminescence of Er-doped SiO2 sensitized with Si nanocrystals.

We report on an observation of a fast 1.5 microm photoluminescence band from Er3+ ions embedded in an SiO2 matrix doped with Si nanocrystals, which appears and decays within the first microsecond after the laser excitation pulse. We argue that the fast excitation and quenching are facilitated by Auger processes related to transitions of confined electrons or holes between the space-quantized levels of Si nanocrystals dispersed in SiO2. We show that a great part--about 50%--of all Er dopants is involved in these fast processes and contributes to the submicrosecond emission.

Isotope dependence of the lifetime of the vibration of oxygen in silicon.

By simply changing the isotopes of the Si atoms that neighbor an oxygen Oi atom in crystalline silicon, the measured decay rate tau of the asymmetric-stretch vibration (nu3=1136 cm-1) of oxygen (Oi) in silicon changes by a factor of approximately 2.5. These data establish that nu3 decays by creating one nu1 symmetric-stretch, local-vibrational mode of the Si-Oi-Si structure. If the residual energy (nu3-nu1) is less than the maximum frequency num of the host lattice, as for 28Si-16O-28Si in natural silicon, then it is emitted as one lattice mode, and tau depends on the density of one-phonon states at nu3-nu1. If (nu3-nu1)>num, as for 16O in single-isotope 30Si silicon, two lattice modes are created in addition to nu1, increasing tau. Prediction of tau for a particular defect clearly requires a detailed knowledge of that defect.

Microscopic structure of Er-related optically active centers in crystalline silicon.

A successful observation and analysis of the Zeeman effect on the lambda approximately 1.54 microm photoluminescence band in Er-doped crystalline MBE-grown silicon are presented. The symmetry of the dominant optically active centers is conclusively established as orthorhombic I(C(2v)) with g axially approximately 18.39 and g radially approximately 0. In this way the long standing puzzle as regards the paramagnetism of optically active Er-related centers in silicon is settled. Preferential generation of a single type of an optically active Er-related center confirmed in this study is essential for photonic applications of Si:Er.

Optically induced deexcitation of rare-Earth ions in a semiconductor matrix.

We report on verification of the proposed energy transfer mechanism responsible for photoluminescence of rare earth (RE) ions in semiconductors. Using two-color spectroscopy in the visible and the midinfrared regions (with a free-electron laser) we demonstrate reversal of the most important step in the excitation process. In that way, formation of the intermediate state bridging atomic states of the RE ion core and extended orbitals of a semiconducting host is explicitly confirmed and its characteristic energy spectroscopically determined. The study is performed for InP:Yb. It is argued, however, that the conclusions are valid for all semiconductor:RE systems, including the notorious Si:Er.