Andres Osvet

Overcoming the Interface Losses in Planar Heterojunction Perovskite-Based Solar Cells.

UNLABELLED A scalable, hysteresis-free and planar architecture perovskite solar cell is presented, employing a flame spray synthesized low-temperature processed NiO (LT-NiO) as hole-transporting layer yielding efficiencies close to 18%. Importantly, it is found that LT-NiO boosts the limits of open-circuit voltages toward an impressive non-radiative voltage loss of 0.226 V only, whereas PEDOT PSS suffers from significant large non-radiative recombination losses.

Black TiO2 nanotubes formed by high energy proton implantation show noble-metal-co-catalyst free photocatalytic H2-evolution

We apply high-energy proton ion-implantation to modify TiO2 nanotubes selectively at their tops. In the proton-implanted region, we observe the creation of intrinsic cocatalytic centers for photocatalytic H2-evolution. We find proton implantation to induce specific defects and a characteristic modification of the electronic properties not only in nanotubes but also on anatase single crystal (001) surfaces. Nevertheless, for TiO2 nanotubes a strong synergetic effect between implanted region (catalyst) and implant-free tube segment (absorber) can be obtained.

Hydrogenated Anatase: Strong Photocatalytic Dihydrogen Evolution without the Use of a Co-Catalyst†

The high-pressure hydrogenation of commercially available anatase or anatase/rutile TiO2 powder can create a photocatalyst for H2 evolution that is highly effective and stable without the need for any additional co-catalyst. This activation effect cannot be observed for rutile; however, for anatase/rutile mixtures, a strong synergistic effect can be found (similar to results commonly observed for noble-metal-decorated TiO2). EPR and PL measurements indicated the intrinsic co-catalytic activation of anatase TiO2 to be due to specific defect centers formed during hydrogenation. These active centers can be observed specifically for high-pressure hydrogenation; other common reduction treatments do not result in this effect.

Brightly Luminescent and Color-Tunable Formamidinium Lead Halide Perovskite FAPbX3 (X = Cl, Br, I) Colloidal Nanocrystals

In the past few years, hybrid organic-inorganic and all-inorganic metal halide perovskite nanocrystals have become one of the most interesting materials for optoelectronic applications. Here, we report a facile and rapid room temperature synthesis of 15-25 nm formamidinium CH(NH2)2PbX3 (X = Cl, Br, I, or mixed Cl/Br and Br/I) colloidal nanocrystals by ligand-assisted reprecipitation (LARP). The cubic and platelet-like nanocrystals with their emission in the range of 415-740 nm, full width at half-maximum (fwhm) of 20-44 nm, and radiative lifetimes of 5-166 ns enable band gap tuning by halide composition as well as by their thickness tailoring; they have a high photoluminescence quantum yield (up to 85%), colloidal and thermodynamic stability. Combined with surface modification that prevents degradation by water, this nanocrystalline material is an ideal candidate for optoelectronic devices and applications. In addition, optoelectronic measurements verify that the photodetector based on FAPbI3 nanocrystals paves the way for perovskite quantum dot photovoltaics.

Extending the environmental lifetime of unpackaged perovskite solar cells through interfacial design

Solution-processed oxo-functionalized graphene (oxo-G1) is employed to substitute hydrophilic PEDOT:PSS as an anode interfacial layer for perovskite solar cells. The resulting devices exhibit a reasonably high power conversion efficiency (PCE) of 15.2% in the planar inverted architecture with oxo-G1 as a hole transporting material (HTM), and most importantly, deploy the full open-circuit voltage (Voc) of up to 1.1 V. Moreover, oxo-G1 effectively slows down the ingress of water vapor into the device stack resulting in significantly enhanced environmental stability of unpackaged cells under illumination with 80% of the initial PCE being reached after 500 h. Without encapsulation, ∼60% of the initial PCE is retained after ∼1000 h of light soaking under 0.5 sun and ambient conditions maintaining the temperature beneath 30 °C. Moreover, the unsealed perovskite device retains 92% of its initial PCE after about 1900 h under ambient conditions and in the dark. Our results underpin that controlling water diffusion into perovskite cells through advanced interface engineering is a crucial step towards prolonged environmental stability.

Effective ligand passivation of Cu₂O nanoparticles through solid-state treatment with mercaptopropionic acid.

In colloidal nanoparticle (NPs) devices, trap state densities at their surface exert a profound impact on the rate of charge carrier recombination and, consequently, on the deterioration of the device performance. Here, we report on the successful application of a ligand exchange strategy to effectively passivate the surface of cuprite (Cu2O) NPs. Cu2O NPs were prepared by means of a novel synthetic route based on flame spray pyrolysis. FTIR, XRD, XPS, and HRTEM measurements corroborate the formation of cubic cuprite Cu2O nanocrystals, excluding the possible presence of undesired CuO or Cu phases. Most importantly, steady-state emission and transient absorption assays document that surface passivation results in substantial changes in the intensity of emissive excitonic states--centered at copper and oxygen vacancies--and in the lifetime of excitons near the band edge. To shed light onto ultrafast processes in Cu2O nanocrystals additional pump probe experiments on the femtosecond and nanosecond time scales were carried out. Two discernible species were observed: on one hand, an ultrafast component (~ps) that relates to the excitons; on the other hand, a long-lived component (~μs) that originates from the defects/trap states.

Photoinduced degradation of methylammonium lead triiodide perovskite semiconductors

Photoinduced degradation is a critical obstacle for the real application of novel semiconductors for photovoltaic applications. In this paper, the photoinduced degradation of CH3NH3PbI3 in a vacuum and air (relative humidity 40%) is analyzed by ex situ and advanced in situ technologies. Without light illumination, CH3NH3PbI3 films slowly degrade under vacuum and air within 24 hours. However, we find that CH3NH3PbI3 converts to metallic lead (Pb0) when exposed to vacuum and light illumination. Further, a series of lead salts (e.g. PbO, Pb(OH)2 and PbCO3) are formed when CH3NH3PbI3 is degraded under environmental conditions, i.e. under the combination of light, oxygen and moisture. Photoinduced degradation is found to be determined by the environmental atmosphere as CH3NH3PbI3 films remain very stable under nitrogen conditions. The results from vacuum conditions underpin that the high volatility of the organic component (CH3NH3I) is in conflict with reaching excellent intrinsic stability due to its role in creating ion vacancies. The degradation in air suggests that both oxygen and water contribute to the fast photodecomposition of CH3NH3PbI3 into lead salts rather than water alone. Given these basic yet fundamental understandings, the design of hydrophobic capping layers becomes one prerequisite towards long-term stable perovskite-based devices.

Qualitative Analysis of Bulk-Heterojunction Solar Cells without Device Fabrication: An Elegant and Contactless Method

The enormous synthetic efforts on novel solar cell materials require a reliable and fast technique for the rapid screening of novel donor/acceptor combinations in order to quickly and reliably estimate their optimized parameters. Here, we report the applicability of such a versatile and fast evaluation technique for bulk heterojunction (BHJ) organic photovoltaics (OPV) by utilizing a steady-state photoluminescence (PL) method confirmed by electroluminescence (EL) measurements. A strong relation has been observed between the residual singlet emission and the charge transfer state emission in the blend. Using this relation, a figure of merit (FOM) is defined from photoluminescence and also electroluminescence measurements for qualitative analysis and shown to precisely anticipate the optimized blend parameters of bulk heterojunction films. Photoluminescence allows contactless evaluation of the photoactive layer and can be used to predict the optimized conditions for the best polymer-fullerene combination. Most interestingly, the contactless, PL-based FOM method has the potential to be integrated as a fast and reliable inline tool for quality control and material optimization.

Electroluminescence imaging of organic photovoltaic modules

We report on electroluminescence (EL) imaging of organic photovoltaic cells and modules with poly(3-hexylthiophene)/[6,6]-phenyl C61 butyric acid methyl ester as semiconductor layer. The dominant EL emission is found in a spectral regime between 1200 and 1400 nm and is identified as the radiative decay of the charge transfer complex formed between the polymer and the fullerene. Electroluminescence emission from the pristine compounds is either much weaker or completely absent. Overall, electroluminescence imaging is shown to give valuable information on the defects but also on the performance of organic solar modules.

Ligand-assisted thickness tailoring of highly luminescent colloidal CH3NH3PbX3 (X = Br and I) perovskite nanoplatelets

Quantum size-confined CH3NH3PbX3 (X = Br and I) perovskite nanoplatelets with remarkably high photoluminescence quantum yield (up to 90%) were synthesized by ligand-assisted re-precipitation. Thickness-tunability was realized by varying the oleylamine and oleic acid ligand ratio. This method allows tailoring the nanoplatelet thickness by adjusting the number of unit cell monolayers. Broadly tunable emission wavelengths (450-730 nm) are achieved via the pronounced quantum size effect without anion-halide mixing.