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- Sub-Bandgap Sensitization of Perovskite Semiconductors via Colloidal Quantum Dots IncorporationPublication . Ribeiro, Guilherme; Ferreira, G.; Menda, U.D.; Alexandre, Miguel; Brites, Maria João; Barreiros, M. Alexandra; Jana, S.; Águas, Hugo; Martins, Rodrigo; Fernandes, P.A.; Salomé, P.M.P.; Mendes, M.J.ABSTRACT: By taking advantage of the outstanding intrinsic optoelectronic properties of perovskite-based photovoltaic materials, together with the strong near-infrared (NIR) absorption and electronic confinement in PbS quantum dots (QDs), sub-bandgap photocurrent generation is possible, opening the way for solar cell efficiencies surpassing the classical limits. The present study shows an effective methodology for the inclusion of high densities of colloidal PbS QDs in a MAPbI3 (methylammonium lead iodide) perovskite matrix as a means to enhance the spectral window of photon absorption of the perovskite host film and allow photocurrent production below its bandgap. The QDs were introduced in the perovskite matrix in different sizes and concentrations to study the formation of quantum-confined levels within the host bandgap and the potential formation of a delocalized intermediate mini-band (IB). Pronounced sub-bandgap (in NIR) absorption was optically confirmed with the introduction of QDs in the perovskite. The consequent photocurrent generation was demonstrated via photoconductivity measurements, which indicated IB establishment in the films. Despite verifying the reduced crystallinity of the MAPbI3 matrix with a higher concentration and size of the embedded QDs, the nanostructured films showed pronounced enhancement (above 10-fold) in NIR absorption and consequent photocurrent generation at photon energies below the perovskite bandgap.
- Scale up of microwave annealed FA0.83Cs0.17PbI1.8Br1.2 perovskite towards an industrial scale [Comunicação oral]Publication . Mascarenhas, João; Barreiros, M. Alexandra; Brites, Maria JoãoABSTRACT: Perovskite solar cells (PSCs) efficiency has rapidly increased from the initial 2009's 3.8 to recent 22.7%. This high efficiency has attracted serious attention of the researchers and industry worldwide also due to their low material cost, and simple soluction-based fabrication process.
- Charge transport and recombination of dye sensitized 1D nanostructured-TiO2 films prepared by reactive sputteringPublication . Sequeira, S.; Lobato, K.; Torres, Erica; Brites, Maria João; Barreiros, M. Alexandra; Mascarenhas, JoãoDye sensitized solar cells (DSCs) are governed by light absorption, charge injection, electron transport and recombination and electrolyte diffusion. One way to improve the efficiency of these devices is by the design of highly ordered nanostructured semiconductor materials.The advantages can be two-fold: Firstly charge transport within the metal-oxide can be enhanced and hence thicker films can be employed and secondly, the complete permeation with a solid-state hole-transport medium of the sensitized metal-oxide can be facilitated. Nanostructured materials should promote vectorial electron diffusion and have as few recombination sights as possible so as to further enhance electron lifetimes and electron collection efficiencies. These materials should also have a high surface area so as to allow for efficient dye-loading and hence light absorption. Highly ordered TiO2 nanostructured films were prepared by reactive sputtering and their charge transport characteristics evaluated in DSCs. These were compared to DSCs employing mesoporous TiO2 films prepared by doctor blade technique using commercial paste. Charge transport characteristics were evaluated by impedance spectroscopy (IS), incident photon to current conversion efficiencies (IPCE) and current-voltage (iV) curves under simulated AM1.5G irradiation. Film morphology and structural properties were evaluated by scanning electron microscopy (SEM) and X-ray diffraction (XRD), respectively.
- Synthesis and photophysical properties of tetraphenylethylene derivatives as luminescent downshifting materials for organic photovoltaic applicationsPublication . Barros, Helio; Esteves, M. Alexandra; Brites, Maria JoãoABSTRACT: Luminescent Down-Shifting (LDS) is an optical approach applied in several photovoltaic (PV) technologies in which high energy solar radiation is converted to a wavelength region where the response of the photovoltaic devices is better. The use of LDS layers on organic photovoltaics (OPV) could serve two purposes: to prevent cell degradation by filtering the incident ultraviolet (UV) radiation and to improve the spectral response of PV cells at short-wavelength. This work reports, the design and synthesis of a series of tetraphenylethylene (TPE) derivatives based on TPE-A or A-pi-TPE-pi-A molecular structure featuring various electron-acceptor (A) groups. The photo-physical properties of the new LDS compounds were systematically studied in 1,4-dioxane solution and film (Zeonex) by UV-visible absorption and fluorescence spectroscopy, and electrochemical properties studied by cyclic voltammetry. Thermal stability of the new LDS compounds was evaluated by Thermogravimetric analysis (TGA). Theoretical computational studies provided evidence of existence of intramolecular charge-transfer (ICT) between frontier orbitals of donor and acceptor moieties. The good photophysical and thermal properties of the synthesized TPE derivatives, associated with high molar absorption coefficients in UV spectrum and emission maximum in the range of 476-531 nm, make them promising candidates for LDS layers in OPV application.
- Dye assessment in nanostructured TiO2 sensitized films by microprobe techniques [Poster]Publication . Barreiros, M. Alexandra; Mascarenhas, João; Corregidor, V.; Alves, L. C.; Guimarães, Fernanda; Torres, Erica; Brites, Maria JoãoDye sensitized solar cells (DSCs) have received considerable attention once this technology offers economic and environmental advantages over conventional photovoltaic (PV) devices. The PV performance of a DSC relies on the characteristics of its photoanode, which typically consists of a nanocrystalline porous TiO2 film, enabled with a large adsorptive surface area. Dye molecules that capture photons from light during device operation are attached to the film nanoparticles. The effective loading of the dye in the TiO2 electrode is of utmost importance for controlling and optimizing solar cell parameters. Relatively few methods are known today for quantitative evaluation of the total dye adsorbed on the film. In this work, a new approach combining microprobe techniques namely, Ion Beam Analytical (IBA) techniques using a micro-ion beam (Rutherford Backscattering Spectrometry (RBS) and Particle Induced X-ray Emission (PIXE)) and Electron Probe Micro-Analysis (EPMA) was carried out to assess dye distribution and depth profile in TiO2 films and the dye load based on Ru/Ti mass ratio. Different 1D nanostructured TiO2 films were prepared, morphologically characterised by SEM, sensitized and analysed by the referred techniques. Dye load evaluation in different TiO2 films by three different techniques (PIXE, RBS and EPMA/ wavelength dispersive spectrometry (WDS)) provided similar results of Ru/Ti mass fraction ratio. Moreover, it was possible to assess dye surface distribution and its depth profile, by means of Ru signal, and to visualise the dye distribution in sample cross-section through X-ray mapping by EPMA/ energy dispersive spectrometry (EDS). PIXE maps of Ru and Ti indicated an homogeneous surface distribution. The assessment of ruthenium depth profile by RBS showed that some films have homogeneous Ru depth distribution while others present different Ru concentration in the top layer (2 ìm thickness). These results are consistent with the EPMA/EDS maps obtained. EPMA (WDS and EDS) together with IBA techniques proved to be powerful tools for functional materials characterisation and provided very promising results in the study of nanostructured TiO2 sensitized films.
- Metal-Oxide-Semiconductor devices for interface studies for perovskite technology [Resumo]Publication . Cunha, J.M.V.; Barreiros, M. Alexandra; Teixeira, J.P.; Curado, M.A.; Lopes, T.S.; Oliveira, K.; Oliveira, A.J.N.; Barbosa, J.R.S.; Vilanova, António; Brites, Maria João; Mascarenhas, João; Flandre, Denis; Silva, Ana G.; Fernandes, P.A.; Salomé, P.M.P.
- Perovskite Metal-Oxide-Semiconductor Structures for Interface CharacterizationPublication . Cunha, J.M.V.; Barreiros, M. Alexandra; Curado, M.A.; Lopes, T.S.; Oliveira, K.; Oliveira, A.J.N.; Barbosa, J.R.S.; Vilanova, António; Brites, Maria João; Mascarenhas, João; Flandre, Denis; Silva, Ana G.; Fernandes, P.A.; Salomé, P.M.P.ABSTRACT: Perovskite solar cells (PSCs) are one of the most promising photovoltaic technologies. Amongst several challenges, developing and optimizing efficient electron transport layers that can be up-scaled still remains a massive task. Admittance measurements on metal-oxide-semiconductor (MOS) devices allow to better understand the optoelectronic properties of the interface between perovskite and the charge carrier transport layer. This work discloses a new pathway for a fundamental characterization of the oxide/semiconductor interface in PSCs. Inverted MOS structures, that is, glass/fluorine-doped tin oxide/tin oxide (SnO2)/perovskite are fabricated and characterized allowing to perform a comparative study on the optoelectronic characteristics of the interface between the perovskite and sputtered SnO2. Admittance measurements allow to assess the interface fixed oxide charges (Q(f)) and interface traps density (D-it), which are extremely relevant parameters that define interface properties of extraction layers. It is concluded that a 30 nm thick SnO2 layer without annealing presents an additional recombination mechanism compared to the other studied layers, and a 20 nm thick SnO2 layer without annealing presents the highest positive Q(f) values. Thus, an effective method is shown for the characterization of the charge carrier transport layer/perovskite interface using the analysis performed on perovskite-based inverted MOS devices.
- Microscopy techniques for dye distribution in DSCs nanocrystalline TiO2 filmsPublication . Barreiros, M. Alexandra; Sequeira, S.; Alves, L. C.; Corregidor, V.; Guimarães, Fernanda; Mascarenhas, João; Brites, Maria João
- Dye-sensitized 1D anatase TiO2 nanorods for tunable efficient photodetection in the visible rangePublication . Parreira, P.; Torres, Erica; Nunes, Clarisse; Carvalho, C. Nunes de; Lavareda, G.; Amaral, A.; Brites, Maria JoãoTiO2 films with enhanced photosensitivity were deposited on alkali free glass substrates without intentional substrate heating by pulsed DC magnetron reactive sputtering with an average thickness of about 2 μm. Three dyes, commercial N719 and two new organic dyes were impregnated in order to control the optical spectral selectivity of such films. The type of dye used proved to dramatically influence the device's response to radiation pulses. The practical breakthrough is the use of different dyes according to the region of the electromagnetic spectrum one wants to detect. Devices with photocurrent 6 orders of magnitude higher than the dark current (from ∼2 × 10−12 to 2 × 10−6 A for a 100 V bias) were fabricated with a spectral response within the visible range of the electromagnetic spectrum. In addition, this approach is likely to allow for the fabrication of hybrid photodetectors on cheap heat sensible flexible polymeric substrates.
- Scale up of microwave annealed FA0.83Cs0.17PbI1.8Br1.2 perovskite towards an industrial scalePublication . Mascarenhas, João; Barreiros, M. Alexandra; Brites, Maria JoãoABSTRACT: Perovskite solar cells (PSCs) efficiency has rapidly increased from the initial 3.8 to recent 24.2%. This high efficiency has attracted serious worldwide researchers and industry attention due to their low material cost, and simple solution-based fabrication process. However, fundamental studies on PSCs are usually produced through lab-scale actions and carried out on small-area devices (≤1 cm2). Here we present the advances of up-scaling using microwave (MW) annealing of perovskite films on large area specimens (~16 cm2), looking forward the industrial-scale. Morphological, structural and optical characterization were performed to confirm the effectiveness of the scaled up MW annealing.
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