Wide-bandgap metal halide perovskite solar cells have become an alluring next-generation solar panel technology because of their simple manufacturing and rising efficiencies by up to 25.7%. When the single junction devices face the ultimate S-Q limit, the incorporation of wide-bandgap perovskite materials with low-bandgap absorbers to form multi-junction cells offers a promising route to surpass the theoretical efficiency. Monolithic perovskite-organic tandem cells are appealing among other compositions owing to the combination of the sub-cells advantages: low-cost, flexibility, and solution processing. In this work, we focused on optimizing the hole transporting materials (HTMs) separately for the two components in tandem devices. In the 1.76 eV perovskite subcell, three commonly seen HTMs are selected (2PACz, NiOx and PTAA) to investigate the influence on device performance. An MgF2 interlayer at perovskite/C60 is deposited as passivation to enhance the voltage and overall performance. It is found that 2PACz is most suitable for triple cation FA0.7MA0.15Cs0.15Pb(I0.6Br0.4)3, giving good crystallinity, energy match and absorption with a champion PCE of 16.12%. Then, we performed a similar optimization for ternary PM6: BTP-eC9: PC70BM with MoOx, MoOx/2PACz, and PEDOT: PSS as HTMs, where MoOx/2PACz present the best statistics. Finally, two terminal tandem devices were fabricated based on the two optimized subcells, and a promising efficiency of 23.6% and a Voc of 2.09V were reached free of hysteresis. More passivation methods or perovskite bandgap engineering are expected to further improve the performance and break the record.

No description available.

The tandem solar cell concept is a promising approach to improve the efficiency of photovoltaic devices. However, characterization of tandem solar cell devices is challenging since correct efficiency determination demands special experimental infrastructure as well as suitable characterization procedures. Even though the appropriate IEC and ASTM measurement standards define all that very precisely, they cannot be applied without special care to organic photovoltaics (OPV) because they were originally developed for inorganic devices. As a consequence, nowadays almost all tandem organic solar cell publications are not using correct characterization procedures, often resulting in questionable efficiency values. The aim of this work is developing a measurement procedure for tandem organic solar cells assuring their correct characterization. Therefore, at first the existing standards and measurement procedures for tandem solar cells are reviewed and challenges when applying these standards to organic solar cells are identified. As main challenges the relatively low fill factors and distinct nonlinearities of organic solar cells are identified. As preliminary experiments, single junction organic solar cells are investigated to analyze the influence of measurement parameters like bias irradiance, bias voltage, and chopper frequency on the external quantum efficiency (EQE) of organic solar cells. This results in parameter sets assuring minimized artifacts for the subsequent EQE determination of the subcells of tandem organic solar cells. The main part of this thesis presents the detailed characterization of a tandem OPV example device. First, EQE is measured and validated by two independent institutes. The EQE results are used to calculate the illumination conditions to reach AM1.5g conditions for both subcells with a multi-source sun simulator. The resulting efficiency value under standard reporting conditions (SRC) is found to be 5% lower than the efficiency measured with a single-source sun simulator. A full spectrometric characterization shows that differing fill factors of the subcells are the reason for this behavior. To overcome the main reason for the complicated measurement procedure of tandem solar cells, the inaccessibility of the individual subcells, three different approaches for the jV-characteristics determination of the subcells are presented. The so-called Bias Voltage Approach is based on EQE-measurements under varying bias voltage and needs no additional electrical contacts. Therefore, it can be applied to existing devices. The Voltage Contact Approach as well as the Current Contact Approach require in changed stack designs. Therefore, they cannot be applied to existing devices but give more accurate results. Finally, a procedure for characterizing tandem organic solar cells is formulated. This procedures aims at giving practical advice how to characterize tandem organic solar cells to achieve results conforming to the measurement standards and being as accurate and reproducible as possible. Hence, this thesis attempts to establish standards for a correct measurement of tandem organic solar cells of which other emerging solar cell technologies can profit as well.

The tandem solar cell concept is a promising approach to improve the efficiency of photovoltaic devices. However, characterization of tandem solar cell devices is challenging since correct efficiency determination demands special experimental infrastructure as well as suitable characterization procedures. Even though the appropriate IEC and ASTM measurement standards define all that very precisely, they cannot be applied without special care to organic photovoltaics (OPV) because they were originally developed for inorganic devices. As a consequence, nowadays almost all tandem organic solar cell publications are not using correct characterization procedures, often resulting in questionable efficiency values. The aim of this work is developing a measurement procedure for tandem organic solar cells assuring their correct characterization. Therefore, at first the existing standards and measurement procedures for tandem solar cells are reviewed and challenges when applying these standards to organic solar cells are identified. As main challenges the relatively low fill factors and distinct nonlinearities of organic solar cells are identified. As preliminary experiments, single junction organic solar cells are investigated to analyze the influence of measurement parameters like bias irradiance, bias voltage, and chopper frequency on the external quantum efficiency (EQE) of organic solar cells. This results in parameter sets assuring minimized artifacts for the subsequent EQE determination of the subcells of tandem organic solar cells. The main part of this thesis presents the detailed characterization of a tandem OPV example device. First, EQE is measured and validated by two independent institutes. The EQE results are used to calculate the illumination conditions to reach AM1.5g conditions for both subcells with a multi-source sun simulator. The resulting efficiency value under standard reporting conditions (SRC) is found to be 5% lower than the efficiency measured with a single-source sun simulator. A full spectrometric characterization shows that differing fill factors of the subcells are the reason for this behavior. To overcome the main reason for the complicated measurement procedure of tandem solar cells, the inaccessibility of the individual subcells, three different approaches for the jV-characteristics determination of the subcells are presented. The so-called Bias Voltage Approach is based on EQE-measurements under varying bias voltage and needs no additional electrical contacts. Therefore, it can be applied to existing devices. The Voltage Contact Approach as well as the Current Contact Approach require in changed stack designs. Therefore, they cannot be applied to existing devices but give more accurate results. Finally, a procedure for characterizing tandem organic solar cells is formulated. This procedures aims at giving practical advice how to characterize tandem organic solar cells to achieve results conforming to the measurement standards and being as accurate and reproducible as possible. Hence, this thesis attempts to establish standards for a correct measurement of tandem organic solar cells of which other emerging solar cell technologies can profit as well.

The need to accurately measure multi-junction (MJ) tandem solar cells' subcell current-voltage characteristics is increasing due to the vital information they provide about the efficiency, stability, and longevity of the cells. These measurements are rather difficult compared to their counterpart single-layer solar cell measurements. The purpose of this project is to construct an instrument that is able to successfully bias multiple subcells in a tandem solar cell. This would allow accurate measurements of the J-V behaviours of individual subcells within the stack and by extent, allow analysis to optimise future tandem cell technology. The instrument made is a controllable multi-chromatic light-emitting diode array, consisting of six wavelength-different LEDs ranging between ultraviolet and infrared light, which the intensity of is controlled bya slider control Graphical User Interface (GUI). This instrument will bemounted on a laboratory station at the institution of solar cell technology, Ångström laboratory. Although not perfect, the instrumentcan provide sufficient background light for biasing subcells of an MJ solar cell for a wide selection of cell band gaps

This thesis investigates novel hole extraction interfaces and series interconnects for applications in organic photovoltaics, specifically in single junction solid-state dye-sensitized solar cells (DSSCs) and tandem DSSC/polymer bulk heterojunction solar cells. Improvements in hole extraction and device performance by using materials compatible with scalable deposition methods are presented, including tungsten- and molybdenum-disulphide (WS₂ and MoS₂), and p-type doped spiro-OMeTAD (2,2',7,7'-tetrakis-(N,N-di-p-methoxyphenylamine)9,9'-spirobifluorene) nanoparticle dispersions. WS₂ and MoS₂ hole extraction layers increase averaged short circuit currents by 20% and 16% respectively, and power conversion efficiencies by 19% and 14% respectively when compared with control devices. Similarly, doped spiro-OMeTAD nano-particle layers improved short circuit current densities by 32% and efficiencies by 9%. Tandem device interconnects using these novel hole extraction formats have been fabricated, but although devices did exhibit rectification, overall performance was poor. Possible reasons for their limited success have been analysed. Dye-sensitized solar mini-modules are also reported. In order to assure the scalability of DSSC technology, these larger area devices were constructed using doctor blade coating to deposit the hole transporter material. As well as achieving a respectable maximum power conversion efficiency of 2.6%, it has also been shown that the extent to which hole transporter infiltrates the mesoporous photoanode of these devices may be tuned by altering substrate temperature during deposition. It was found that an optimal coating temperature of 70 degrees C produced the best efficiency, with a corresponding pore-filling fraction of 41%.

Photovoltaic technologies use light from the sun to create electricity, using a wide range of materials and mechanisms. The generation of clean, renewable energy using this technology must become price competitive with conventional power generation if it is to succeed on a large scale. The field of photovoltaics can be split into many sub-groups, however the overall aim of each is to reduce the cost per watt of the produced electricity. One such solar cell which has potential to reduce the cost significantly is the dye sensitised solar cell (DSC), which utilises cheap materials and processing methods. The reduction in cost of the generated electricity is largely dependent on two parameters. Firstly, the efficiency that the solar cell can convert light into electricity and secondly, the cost to deposit the solar cell. This thesis aims to address both factors, specifically looking at altering the transparent conducting oxide (TCO) and substrate in the solar cell. One method to improve the overall conversion efficiency of the device is to implement the DSC as the top cell in a tandem structure, with a bottom infra-red absorbing solar cell. The top solar cell in such a structure must not needlessly absorb photons which the bottom solar cell can utilise, which can be the case in solar cells utilising standard transparent contacts such as fluorine-doped tin oxide. In this work, transparent conducting oxides with high mobility such as titanium-doped indium oxide (ITiO) have been used to successfully increase the amount of photons through a DSC, available for a bottom infra-red sensitive solar cell such as Cu(In,Ga)Se2 (CIGS). Although electrically and optically of very high quality, the production of DSCs on this material is difficult due to the heat and chemical instability of the film, as well as the poor adhesion of TiO2 on the ITiO surface. Deposition of a interfacial SnO2 layer and a post-deposition annealing treatment in vacuum aided the deposition process, and transparent DSCs of 7.4% have been fabricated. The deposition of a high quality TCO utilising cheap materials is another method to improve the cost/watt ratio. Aluminium-doped zinc oxide (AZO) is a TCO which offers very high optical and electronic quality, whilst avoiding the high cost of indium based TCOs. The chemical and thermal instability of AZO films though present a problem due to the processing steps used in DSC fabrication. Such films etch very easily in slightly acidic environments, and are susceptible to a loss of conductivity upon annealing in air, so some steps have to be taken to fabricate intact devices. In this work, thick layers of SnO2 have been used to reduce the amount of etching on the surface of the film, whilst careful control of the deposition parameters can produce AZO films of high stability. High efficiency devices close to 9% have been fabricated using these stacked layers. Finally, transferring solar cells from rigid to flexible substrates offers cost advantages, since the price of the glass substrate is a significant part of the final cost of the cell. Also, the savings associated with roll to roll deposition of solar cells is large since the production doesn't rely on a batch process, using heavy glass substrates, but a fast, continuous process. This work has explored using the high temperature stable polymer, polyimide, commonly used in CIGS and CdTe solar cells. AZO thin films have been deposited on 7.5um thick polyimide foils, and DSCs of efficiency over 4% have been fabricated on the substrates, using standard processing methods.

No description available.

L'objectif de cette thèse est de réaliser l'intégration monolithique de nanofils (NFs) à base de l’alliage Al0.2Ga0.8As sur des substrats de Si par épitaxie par jets moléculaires via la méthode vapeur-liquide-solide (VLS) auto-assistée et de développer une cellule solaire tandem (TSC) à base de ces NFs.Pour atteindre cet objectif, nous avons tout d'abord étudié la croissance de NFs GaAs, étape clé pour le développement des NFs p-GaAs/p.i.n-Al0.2Ga 0.8As coeur/coquille, qui devraient constituer la cellule supérieure de la TSC. Nous avons montré, en particulier, l'influence de l'angle d'incidence du flux de Ga sur la cinétique de croissance des NFs GaAs. Un modèle théorique et des simulations numériques ont été réalisées pour expliquer ces résultats expérimentaux.Nous avons ensuite utilisé le savoir-faire acquis pour faire croître des NFs p-GaAs/p.i.n-Al0,2Ga0,8As coeur/coquille sur des substrats de Si prêts pour l'emploi. Les caractérisations EBIC réalisées sur ces NFs ont montré qu'ils sont des candidats potentiels pour la réalisation d’une cellule photovoltaïque. Nous avons ensuite fait croître ces NFs sur des substrats de Si patternés afin d'obtenir des réseaux réguliers de ces NFs. Nous avons développé un protocole, basé sur un pré-traitement thermique, qui permet d'obtenir des rendements élevés de NFs verticaux (80-90 %) sur une surface patternée de 0,9 x 0,9 mm2.Enfin, nous avons consacré une partie de notre travail à définir le procédé de fabrication optimal pour la TSC, en concentrant notre attention sur le développement de la jonction tunnel de la TSC, l'encapsulation des NFs et le contact électrique supérieur du réseau de NFs. / The objective of this thesis is to achieve monolithical integration of Al0.2Ga0.8As-based nanowires (NWs) on Si substrates by molecular beam epitaxy via the self-assisted vapour-liquid-solid (VLS) method and develop a NWs-based tandem solar cell (TSC).In order to fulfil this purpose, we firstly focused our attention on the growth of GaAs NWs this being a key-step for the development of p-GaAs/p.i.n-Al0.2Ga0.8As core/shell NWs, which are expected to constitute the top cell of the TSC. We have shown, in particular, the influence of the incidence angle of the Ga flux on the GaAs NW growth kinetic. A theoretical model and numerical simulations were performed to explain these experimental results.Subsequently, we employed the skills acquired to grow p-GaAs/p.i.n-Al0.2Ga0.8As core/shell NWs on epi-ready Si substrates. EBIC characterizations performed on these NWs have shown that they are potential building blocks for a photovoltaic cell. We then committed to growing them on patterned Si substrates so as to obtain regular arrays of NWs. We have developed a protocol, based on a thermal pre-treatment, which allows obtaining high vertical yields of such NWs (80-90 %) on patterned Si substrates (on a surface of 0.9 x 0.9 mm2).Finally, we dedicated part of our work to define the optimal fabrication process for the TSC, focusing our attention to the development of the TSC tunnel junction, the NW encapsulation and the top contacting of the NWs.

Depuis une vingtaine d’année les nanofils des semiconducteurs suscitent un intérêt majeur pour des applications diverses grâce à leurs propriétés optoélectroniques particulières. Dans le domaine du photovoltaïque ils présentent aussi un atout majeur. La combinaison du fort coefficient d’absorption des semiconducteurs III-V et le faible coût des substrats de silicium permettraient la réalisation des cellules photovoltaïques à faible coût et à haut rendement. C’est dans ce contexte que s’est déroulé cette thèse qui visait le développement des dispositifs à base des nanofils III-V pour le photovoltaïque. Dans une première partie, les techniques de nanofabrication pour la réalisation des dispositifs à base d’ensemble de nanofils pour les cellules photovoltaïques sont présentées. Ensuite, la fabrication et la caractérisation de dispositifs à base d’ensembles de nanofils de GaN pour les applications photovoltaïque sont permis d’ouvrir la voie au développement des cellules solaires tandems d’InGaN⁄Si. Dans la suite des travaux on a étudié la croissance des nanofils de GaAs du type cœur-coquille sur Si ainsi que les étapes technologiques pour la fabrication des dispositifs à base d’ensemble de nanofils dans l’optique de préparer le terrain pour la réalisation d’une cellule tandem III-V sur Si. Enfin la croissance et la caractérisation électro-optique des nanofils contenant des jonctions axiales de GaAsP crus par la méthode VLS-EJM a permis de déterminer le type de dopage et l’optimisation de la structure en vue d’obtenir un effet photovoltaïque. / Over the past twenty years, semiconductor nanowires have attracted major interest for various applications thanks to their particular optoelectronic properties. The combination of the high absorption coefficient of the III-V semiconductors and the low cost of the silicon substrates would allow the realization of photovoltaic cells at low cost and high efficiency. It is in this context that this thesis was developed which focused on the development of devices based on III-V nanowires for photovoltaics. In a first part, the nanofabrication techniques for the realization of devices based on set of nanowires for photovoltaic cells are presented. Next, the fabrication and characterization of devices based on GaN nanowire arrays for photovoltaic applications is paving the way for the development of InGaN / Si tandem solar cells. In the following, we studied the growth of core-shell GaAs nanowires on Si as well as the technological steps for the fabrication of nanowire-based devices in order to prepare the ground for the realization of a tandem III-V cell on Si. Finally, the growth and electro-optical characterization of the nanowires containing axial junctions of raw GaAsP by the VLS-EJM method made it possible to determine the type of doping and the optimization of the structure in order to obtain a photovoltaic effect.