Klaus Lips

Improving the light-harvesting of amorphous silicon solar cells with photochemical upconversion

Single-threshold solar cells are fundamentally limited by their ability to harvest only those photons above a certain energy. Harvesting below-threshold photons and re-radiating this energy at a shorter wavelength would thus boost the efficiency of such devices. We report an increase in light harvesting efficiency of a hydrogenated amorphous silicon (a-Si:H) thin-film solar cell due to a rear upconvertor based on sensitized triplet–triplet-annihilation in organic molecules. Low energy light in the range 600–750 nm is converted to 550–600 nm light due to the incoherent photochemical process. A peak efficiency enhancement of (1.0 ± 0.2)% at 720 nm is measured under irradiation equivalent to (48 ± 3) suns (AM1.5). We discuss the pathways to be explored in adapting photochemical UC for application in various single threshold devices.

On an Easy Way To Prepare Metal–Nitrogen Doped Carbon with Exclusive Presence of MeN4-type Sites Active for the ORR

Today, most metal and nitrogen doped carbon catalysts for ORR reveal a heterogeneous composition. This can be reasoned by a nonoptimized precursor composition and various steps in the preparation process to get the required active material. The significant presence of inorganic metal species interferes with the assignment of descriptors related to the ORR activity and stability. In this work we present a simple and feasible way to reduce the contribution of inorganic metal species in some cases even down to zero. Such catalysts reveal the desired homogeneous composition of MeN4 (Me = metal) sites in the carbon that is accompanied by a significant enhancement in ORR activity. Among the work of other international groups, our iron-based catalyst comprises the highest density of FeN4 sites ever reported without interference of inorganic metal sites.

Dye-Sensitized Solar Cell with Integrated Triplet-Triplet Annihilation Upconversion System.

Photon upconversion (UC) by triplet-triplet annihilation (TTA-UC) is employed in order to enhance the response of solar cells to sub-bandgap light. Here, we present the first report of an integrated photovoltaic device, combining a dye-sensitized solar cell (DSC) and TTA-UC system. The integrated device displays enhanced current under sub-bandgap illumination, resulting in a figure of merit (FoM) under low concentration (3 suns), which is competitive with the best values recorded to date for nonintegrated systems. Thus, we demonstrate both the compatibility of DSC and TTA-UC and a viable method for device integration.

Electrical detection of coherent 31 P spin quantum states

In recent years, a variety of solid-state qubits has been realized, including quantum dots1,2, superconducting tunnel junctions3,4 and point defects5,6. Owing to its potential compatibility with existing microelectronics, the proposal by Kane7,8—on the basis of phosphorus donors in silicon—has been pursued intensively9,10,11. A key issue of this concept is the readout of the 31P quantum state. Electrical measurements of magnetic resonance have been carried out on single spins12,13, but the statistical nature of these experiments based on random-telegraph-noise measurements has impeded the readout of single spin states. Here, we demonstrate the measurement of the spin state of 31P donor electrons in silicon and the observation of Rabi flops by purely electric means, that is by coherent manipulation of spin-dependent charge-carrier recombination between the 31P donor and paramagnetic localized states at the Si/SiO2 interface. The electron spin information is shown to be coupled through the hyperfine interaction to the 31P nucleus, suggesting that recombination-based readout of nuclear spins is feasible.

Direct detection of photoinduced charge transfer complexes in polymer fullerene blends

We report transient electron paramagnetic resonance (trEPR) measurements with sub-microsecond time resolution performed on a P3HT:PCBM blend at low temperature. The trEPR spectrum immediately following photoexcitation reveals signatures of spin-correlated polaron pairs. The pair partners (positive polarons in P3HT and negative polarons in PCBM) can be identified by their characteristic g-values. The fact that the polaron pair states exhibit strong non-Boltzmann population unambiguously shows that the constituents of each pair are geminate, i.e. originate from one exciton. We demonstrate that coupled polaron pairs are present even several microseconds after charge transfer and suggest that they embody the intermediate charge transfer complexes which form at the donor/acceptor interface and mediate the conversion from excitons into free charge carriers.

Photochemical Upconversion Enhanced Solar Cells: Effect of a Back Reflector

Photochemical upconversion is applied to a hydrogenated amorphous silicon solar cell in the presence of a back-scattering layer. A custom-synthesized porphyrin was utilized as the sensitizer species, with rubrene as the emitter. Under a bias of 24 suns, a peak external quantum efficiency (EQE) enhancement of ~2 % was observed at a wavelength of 720 nm. Without the scattering layer, the EQE enhancement was half this value, indicating that the effect of the back-scatterer is to double the efficacy of the upconverting device. The results represent an upconversion figure of merit of 3.5 × 10–4 mA cm–2 sun–2, which is the highest reported to date.

Defects and recombination in microcrystalline silicon

The paper addresses the defect structure of microcrystalline silicon, mc-Si:H. Electron spin resonance (ESR) techniques are employed to study the nature and energy distribution of paramagnetic states in a large variety of undoped and doped mc-Si:H samples prepared by various methods under different deposition conditions. A qualitative model for the density of states distribution in the energy gap is developed which is dominated by two kinds of dangling bonds and bandtail states at both band edges. In phosphorus-doped samples, ESR reveals a metal–insulator transition at a phosphorus concentration of 4 � 10 18 cm � 3 . Light-induced ESR and electrically detected magnetic resonance show that at low temperatures recombination is dominated by tunneling transitions from the bandtail states into neutral dangling bonds. Apparently, at higher temperatures, direct capture from conducting states prevails. The results are discussed considering the heterogeneous structure of this material. r 2002 Elsevier Science B.V. All rights reserved.

Junction formation and current transport mechanisms in hybrid n-Si/PEDOT:PSS solar cells

We investigated hybrid inorganic-organic solar cells combining monocrystalline n-type silicon (n-Si) and a highly conductive polymer poly(3,4-ethylenedioxythiophene)-poly(styrene sulfonate) (PEDOT:PSS). The build-in potential, photo- and dark saturation current at this hybrid interface are monitored for varying n-Si doping concentrations. We corroborate that a high build-in potential forms at the hybrid junction leading to strong inversion of the n-Si surface. By extracting work function and valence band edge of the polymer from ultraviolet photoelectron spectroscopy, a band diagram of the hybrid n-Si/PEDOT:PSS heterojunction is presented. The current-voltage characteristics were analyzed using Schottky and abrupt pn-junction models. The magnitude as well as the dependence of dark saturation current on n-Si doping concentration proves that the transport is governed by diffusion of minority charge carriers in the n-Si and not by thermionic emission of majorities over a Schottky barrier. This leads to a comprehensive explanation of the high observed open-circuit voltages of up to 634 mV connected to high conversion efficiency of almost 14%, even for simple planar device structures without antireflection coating or optimized contacts. The presented work clearly shows that PEDOT:PSS forms a hybrid heterojunction with n-Si behaving similar to a conventional pn-junction and not, like commonly assumed, a Schottky junction.

Room temperature electrical detection of spin coherence in C60.

An experimental demonstration of electrical detection of coherent spin motion of weakly coupled, localized electron spins in thin fullerene C60 films at room temperature is presented. Pulsed electrically detected magnetic resonance experiments on vertical photocurrents through Al/C(60)/ZnO samples showed that an electron spin Rabi oscillation is reflected by transient current changes. The nature of possible microscopic mechanisms responsible for this spin to charge conversion as well as its implications for the readout of endohedral fullerene (N@C(60)) spin qubits are discussed.

Transport and recombination in amorphous p‐i‐n‐type solar cells studied by electrically detected magnetic resonance

A detailed study of electrically detected magnetic resonance in p‐i‐n‐type solar cells made from amorphous silicon is reported. It is found that the spectra depend sensitively on the applied voltage, and the intensity and photon energy of the light. The results support the present understanding of the mechanism of the device. It is shown that in general, the transport in the dark, and the charge collection under illumination, are controlled by recombination in the bulk of the i layer. Only when a high forward bias is applied and under illumination does recombination at the p‐i interface play an important role. Degradation by both current and illumination results predominantly in an enhancement of the recombination rate in the i layer.