With the rapid increase in energy demand and the rise of CO2 levels due to traditional energy production from fossil fuels, it is critical to the transition to a sustainable and renewable energy sources. Recently, photovoltaic technology has been raised as a promising alternative to fossil fuel energy production. Solar cells, predominately crystalline silicon technology, are currently 3.6% of electricity production. To maintain this progress, coupling the perovskite and silicon in tandem devices has enormous potential to increase the efficiency of solar energy production, where perovskite solar cells emerged as a promising technology. Textured silicon solar cells are a well-established technology; keeping the advantage of this technology, it is crucial to employ the perovskite to be a compatible top cell for silicon-based tandems. Here, we optimize the silicon bottom cell by understanding the influence of temperature, time, and etchant concentration on the optical properties and performance of the device. Then, we investigate the impact of the textured silicon on the optoelectronic properties of perovskite. Using hyperspectral imaging, we demonstrate that different texturing substrates influence the PL of perovskite, which is associated with the thickness of the perovskite. Lastly, we explored the delamination of the devices due to the weak adhesion between C60/SnO2 after the deposition of IZO and MgF2, which was found to be caused by the deposition conditions. The high temperature and power density caused a weak adhesion between C60/SnO2. Overall, these findings will help to alter the design of Perovskite/Silicon tandem devices to accelerate the commercialization of tandem technology.

With the global energy demand projected to grow rapidly, it is imperative to divest from traditional greenhouse gas-based power production toward renewable energy sources such as solar. In recent years, solar photovoltaics (PV) hold a large share among renewables sources. Currently, the market is dominated by crystalline silicon solar cells due to their low levelized cost of energy (LCOE) values. However, to sustain this progress, the power conversion efficiency of PV devices must be further improved since tiny costs cut from the other expenses is difficult. On the other hand, the margin for the PCE improvement in c-Si technology is also quite limited since the technology is approaching its practical limits. At this stage, coupling c-Si devices with another efficient solar cell in tandem configuration is a promising way to overcome this challenge. Perovskite solar cells (PSCs) represent a breakthrough solar technology to enable this target due to their proven high efficiency and potential cost-effectiveness. Whereas perovskite/silicon tandem solar cells are promising, their operational stabilities are still a significant concern for market entry. Here, the degradation mechanism of n-i-p perovskite/Si tandem solar cells was investigated. Thermal stability tests have shown severe degradation in such tandem devices. On the other hand, tandem devices were relatively stable when placed in a humidity cabinet with 25% relative humidity (RH). Conversely, temperature degraded devices showed cracks all over the perovskite surface and rupture in the top electrode after 1000 hrs at 85 oC. Additionally, silver iodide formation was depicted in XRD and XPS analysis. To enhance the stability, methods to reduce the hysteresis were studied. First, potassium chloride (KCl) was applied as a passivation agent to the electron transport layer (ETL) to reduce surface defects. Second, 2D passivation was applied to reduce trap density and enhance the crystallinity of the perovskite film. Finally, organic molecules were placed between the hole transport layer (HTL) and metal-oxide interface as interlayers to prevent diffusion of metal oxide to the HTL and accumulation of the dopant at the metal-oxide interface. After passivation and interface layers, stability enhanced but further improvement is still required.

High efficiency solar cells can be attained by the development of two junctions one stacked on top of each other into tandem structures. So that, if a photon is not able to excite an electron-hole pair in the top cell can create a pair in the bottom cell, which has a smaller bandgap. For a two junction tandem device structure, the bandgap of the top cell should be 1.6-1.8eV and for the bottom cell should be 1eV to attain efficiencies in the range of 25%. Cadmium Zinc Telluride which has a tunable bandgap of 1.45- 2.2eV is a candidate for the top cell of the tandem structure. Cadmium Zinc Telluride (Cd1-xZnxTe) films were deposited by co-sputtering of CdTe and ZnTe. Deposition of Cd1-xZnxTe was studied in Ar and Ar/N2 ambient. Characterization of the films was done using transmission response, X-ray diffraction (XRD), Atomic Force Microscopy (AFM), Secondary Electron Microscopy (SEM), current-voltage (I-V) and spectral response measurements. CZT deposited on CdS/SnO2 substrates showed improved performance compared to other heterojunction partners. Doped graphite and copper were utilized as back contacts for CZT devices. Post deposition annealing treatments with ZnCl2 on CZT films were done and their effect on the devices was also studied. The best combination of Voc and Jsc were 530mV and 3.66mA/cm² respectively.

Title from PDF of title page. / Document formatted into pages; contains 70 pages. / Thesis (M.S.E.E.)--University of South Florida, 2003. / Includes bibliographical references. / Text (Electronic thesis) in PDF format. / ABSTRACT: Currently thin film solar cells have efficiencies in the range of 16-18%. Higher efficiencies of 20% or more can be achieved by two junction solar cells in which two p-n junctions are connected in series one on top of the other in a tandem structure. The ideal bandgaps for optimum efficiency in a tandem structure are about 1eV for the top cell and 1.7 eV for the bottom cell. Copper Indium Gallium di-Selenide (CIGS) with a bandgap of 1 eV is a suitable candidate for the bottom cell and Cadmium Zinc Telluride (CZT) with a tunable bandgap of 1.44-2.26 eV is a suitable candidate for the top cell. This work involves characterization of cadmium zinc telluride films and solar cells prepared by close spaced sublimation. CZT is deposited by co-sublimation of CdTe and ZnTe. The process has been investigated on various wide bandgap semiconductor materials including cadmium sulphide, cadmium oxide and zinc selenide. / ABSTRACT: Different post deposition heat treatments were carried out to determine their effect on film and device properties. Characterization of the CZT devices was done using XRD, EDS, SIMS, J-V and spectral response measurements. CZT (Eg 1.7 eV) /CdS exhibited best performance when compared to the other window layers investigated. The best device exhibited Voc=640mV, FF=40% and Jsc=4.5 mA/cm2. The theoretical performance of CZT based solar cells were investigated using SCAPS. The effect of bulk and interface defects on the device parameters were studied. / System requirements: World Wide Web browser and PDF reader. / Mode of access: World Wide Web.

abstract: The emergence of perovskite and practical efficiency limit to silicon solar cells has opened door for perovskite and silicon based tandems with the possibility to achieve >30% efficiency. However, there are material and optical challenges that have to be overcome for the success of these tandems. In this work the aim is to understand and improve the light management issues in silicon and perovskite based tandems through comprehensive optical modeling and simulation of current state of the art tandems and by characterizing the optical properties of new top and bottom cell materials. Moreover, to propose practical solutions to mitigate some of the optical losses. Highest efficiency single-junction silicon and bottom silicon sub-cell in silicon based tandems employ monocrystalline silicon wafer textured with random pyramids. Therefore, the light trapping performance of random pyramids in silicon solar cells is established. An accurate three-dimensional height map of random pyramids is captured and ray-traced to record the angular distribution of light inside the wafer which shows random pyramids trap light as well as Lambertian scatterer. Second, the problem of front-surface reflectance common to all modules, planar solar cells and to silicon and perovskite based tandems is dealt. A nano-imprint lithography procedure is developed to fabricate polydimethylsiloxane (PDMS) scattering layer carrying random pyramids that effectively reduces the reflectance. Results show it increased the efficiency of planar semi-transparent perovskite solar cell by 10.6% relative. Next a detailed assessment of light-management in practical two-terminal perovskite/silicon and perovskite/perovskite tandems is performed to quantify reflectance, parasitic and light-trapping losses. For this first a methodology based on spectroscopic ellipsometry is developed to characterize new absorber materials employed in tandems. Characterized materials include wide-bandgap (CH3NH3I3, CsyFA1-yPb(BrxI1-x)3) and low-bandgap (Cs0.05FA0.5MA0.45(Pb0.5Sn0.5)I3) perovskites and wide-bandgap CdTe alloys (CdZnSeTe). Using this information rigorous optical modeling of two-terminal perovskite/silicon and perovskite/perovskite tandems with varying light management schemes is performed. Thus providing a guideline for further development. / Dissertation/Thesis / Doctoral Dissertation Electrical Engineering 2019

Currently thin film solar cells have efficiencies in the range of 16-18%. Higher efficiencies of 20% or more can be achieved by two junction solar cells in which two p-n junctions are connected in series one on top of the other in a tandem structure. The ideal bandgaps for optimum efficiency in a tandem structure are about 1eV for the top cell and 1.7 eV for the bottom cell. Copper Indium Gallium di-Selenide (CIGS) with a bandgap of 1 eV is a suitable candidate for the bottom cell and Cadmium Zinc Telluride (CZT) with a tunable bandgap of 1.44-2.26 eV is a suitable candidate for the top cell. This work involves characterization of cadmium zinc telluride films and solar cells prepared by close spaced sublimation. CZT is deposited by co-sublimation of CdTe and ZnTe. The process has been investigated on various wide bandgap semiconductor materials including cadmium sulphide, cadmium oxide and zinc selenide. Different post deposition heat treatments were carried out to determine their effect on film and device properties. Characterization of the CZT devices was done using XRD, EDS, SIMS, J-V and spectral response measurements. CZT (Eg~1.7 eV) /CdS exhibited best performance when compared to the other window layers investigated. The best device exhibited Voc=640mV, FF=40% and Jsc=4.5 mA/cm2. The theoretical performance of CZT based solar cells were investigated using SCAPS. The effect of bulk and interface defects on the device parameters were studied.

La limite théorique d’efficacité d’une cellule solaire simple jonction est de ~29 %. Afin de dépasser cette limite, une des moyens les plus prometteurs est de combiner le silicium avec des matériaux III-V. Alors que la plupart des solutions proposées dans la littérature proposent de faire croître directement le matériau III-V sur substrat silicium, ce travail présente une approche innovante de fabriquer ces cellules solaires tandem. Nous proposons une approche inverse métamorphique, où le silicium cristallin ou SiGe est cru directement sur le matériau III-V par PECVD. La faible température de dépôt (< 200 °C) diminue les problèmes de différence de dilatation thermique, et le fait de croître le matériau IV sur le matériau III-V élimine les problèmes de polarité.La réalisation de la cellule tandem finale en SiGe/AlGaAs passe par le développement et l’optimisation de plusieurs briques technologiques. Tout d’abord, nous développons l’épitaxie à 175 °C de Si(Ge) sur des substrats de Si (100) dans un réacteur de RF-PECVD industriel. La réalisation de cellules solaires à hétérojonction à partir de ce matériau Si(Ge) crû par PECVD montre que ses performances électriques s’avèrent prometteuses. Nous obtenons pour un absorbeur de 1.5 µm des Voc qui atteignent 0.57 V. L’incorporation de Ge permet d’augmenter le JSC de 15.4 % jusqu’à 16.6 A/cm2 pour Si0.72Ge0.28.En parallèle, la croissance de cellules solaires AlGaAs a été développée, ainsi que sa fabrication technologique. Nous obtenons une efficacité de 17.6 % pour une cellule simple en Al0.22Ga0.78As. Nous développons aussi des jonctions tunnel, parties essentielles d’une cellule tandem dans une configuration à deux terminaux. Nous développons notamment le dopage n du GaAs en utilisant le précurseur DIPTe, et obtenons des jonctions tunnel ayant des courants pic atteignant jusqu’à 3000 A/cm2, rejoignant ainsi les résultats de l’état de l’art.Ensuite, nous étudions l’hétéro-épitaxie de Si sur GaAs par PECVD. Le c-Si montre d’excellentes propriétés structurales. Les premiers stades de croissance sont étudiés par diffraction des rayons X avec rayonnement synchrotron. Nous trouvons un comportement inattendu : le Si est relâché dès les premiers nanomètres, mais sa maille est tétragonale. Alors que le GaAs a un paramètre de maille plus grand que le Si, le paramètre hors du plan (a⏊) du Si est plus élevé que son paramètre dans le plan (a//). Nous trouvons une forte corrélation entre cette tétragonalité et la présence d’hydrogène dans la couche de silicium. D’autre part, nous montrons que le plasma d’hydrogène présent lors du dépôt PECVD affecte les propriétés du GaAs : son dopage diminue d’environ un ordre de grandeur lorsque le GaAs est exposé au plasma H2, dû à la formation de complexes entre le H et le dopant (C, Te ou Si). Le dopage initial peut être retrouvé après un recuit à 350 °C.Enfin, nous étudions la dernière étape de fabrication de la cellule tandem : le collage. Nous avons pu reporter une cellule simple inversée en AlGaAs sur un substrat hôte (en Si), retirer le substrat GaAs et effectuer les étapes de microfabrication sur un substrat 2 pouces. Des couches épaisses de Si (>1 µm) ont été crues avec succès sur une cellule AlGaAs inversée suivie d’une jonction tunnel. Le collage de cette cellule tandem, et la processus de fabrication technologique du dispositif final sont ensuite étudiés, afin de pouvoir caractériser électriquement la première cellule solaire tandem fabriquée par croissance inverse métamorphique de Si sur III-V. / Combining Silicon with III-V materials represents a promising pathway to overcome the ≈29% efficiency limit of a single c-Si solar cell. While the standard approach is to grow III-V materials on Si, this work deals with an innovative way of fabricating tandem solar cells. We use an inverted metamorphic approach in which crystalline silicon or SiGe is directly grown on III-V materials by PECVD. The low temperature of this process (<200 °C) reduces the usual thermal expansion problems, and growing the group IV material on the III-V prevents polarity issues.The realization of the final tandem solar cell made of SiGe/AlGaAs requires the development and optimization of various building blocks. First, we develop the epitaxy at 175°C of Si(Ge) on (100) Si substrates in an industrial standard RF-PECVD reactor. We prove the promising electrical performances of such grown Si(Ge) by realizing PIN heterojunction solar cells with 1.5µm epitaxial absorber leading to a Voc up to 0.57 V. We show that the incorporation of Ge in the layer increases the Jsc from 15.4 up to 16.6 A/cm2 (SiGe28%).Meanwhile, we develop the growth of AlGaAs solar cells by MOVPE and its process flow. We reach an efficiency of 17.6 % for a single Al0.22GaAs solar cell. We then develop the tunnel junction (TJ), essential part of a tandem solar cell with 2-terminal integration. We develop the growth of n-doped GaAs with DIPTe precursor to fabricate TJs with peak tunneling currents up to 3000 A/cm2, reaching state-of-the art TJs.Then, the hetero-epitaxy of Si on GaAs by PECVD is studied. c-Si exhibits excellent structural properties, and the first stages of the growth are investigated by X-ray diffraction with synchrotron beam. We find an unexpected behavior: the grown Si is fully relaxed, but tetragonal. While the GaAs lattice parameter is higher than silicon one, we find a higher out-of-plane Si parameter (a⏊) than in-plane (a//), contradicting the common rules of hetero-epitaxy. We find a strong correlation between this tetragonal behavior and the presence of hydrogen in the Si layer. We furthermore show that hydrogen also plays a strong role in GaAs: the doping level of GaAs is decreased by one order of magnitude when exposed to a H2 plasma, due to the formation of complexes between H and the dopants (C, Te, Si). This behavior can be recovered after annealing at 350°C.Finally, the last step of device fabrication is studied: the bonding. We successfully bonded an inverted AlGaAs cell, removed it from its substrate, and processed a full 2” wafer. We succeeded in growing our first tandem solar cells by growing thick layers (>1 µm) of Si on an inverted AlGaAs solar cells followed by a TJ. The bonding and process of this final device is then performed, leading, as a next step, to the electrical measurement of the very first tandem solar cell grown by inverted metamorphic growth of Si on III-V.

Solar photovoltaics (PV) is expected to be a critical contributor to mitigating the effects of climate change by helping to satisfy net zero emissions. Since crystalline silicon-based solar cells are close to their practical efficiency limit, further reducing the balance of system (BoS) costs is only possible by increasing the cell efficiencies. The most promising candidate is perovskite/silicon (Si) tandem solar cell technology, which allows efficient solar spectrum harvesting. This relatively new technology attracts attention due to its potential to dominate the PV market; however, it also brings challenges that must be overcome, like stability and scalability concerns. This thesis project focuses on optimizing and characterizing recombination junctions (RJs) for monolithic perovskite/Si tandem solar cells aimed at improved performance and stability. Tandem solar cell PV parameter measurements, encapsulated stability measurements, and thin film characterizations are performed for RJ developments. The optimizations are performed for tandem solar cells with solution-processing and hybrid methods. Self-assembled monolayer (SAM) molecules and transparent conductive oxide (TCO) recombination layer (RL) combinations are optimized to obtain tandems with hybrid technique. In addition, the influence of the thickness of TCO RL on the tandem devices’ performance is also investigated, particularly solution-processed tandems. The improvements are observed by thinning down the thickness of TCOs regardless of the material type. 3 Characterizations revealed that ultra-thin ( 5 nm) amorphous indium zinc oxide (IZO) RL allows more workfunction shift, homogeneous surface potential distribution with SAM deposition, and better carrier recombination suppression at the perovskite/hole transport layer (HTL) interface. Ultra-thin RL idea is combined with some optical improvements in the device architecture, and stable high-efficient perovskite/Si tandem solar cells with 32.5% power conversion efficiency (PCE) and 80% fill factor (FF) values are realized. In addition, the preliminary examples of tandem devices with a larger active area (4 cm2 ) are presented. Finally, the remaining challenges and alternative concepts are also discussed.

No description available.

Recent studies suggest that the performance of dye-sensitised solar cells (DSC) has appeared to have reached a limit, therefore solar cells based on semiconductor materials, such as extremely thin absorber (ETA) solar cells and tandem solar cells are currently the subject of intense research in the framework of low-cost photovoltaic devices as sources of harvesting sunlight to generate electricity. Generally, semiconductor solar cells have been divided into two different types, namely anodic and cathodic type solar cells. Extensive research and development work has been focused on anodic semiconductor sensitised solar cells to date. In contrast, the cathodic semiconductor sensitised solar cells have received no attention which is very surprising. Developing the cathodic semiconductor sensitised solar cell concept is very important in the development of tandem solar cells as well as other new solar cell configurations. The main reason for the lack of research in this area was due to the rarity of p-type semiconductor materials, which made it difficult to find suitable materials to match the energy band edges for cathodic semiconductor sensitised solar cells (CSSC) as well as solid-state cathodic semiconductor solar cells (SS-CSSC). The primary aim of this thesis was to construct cathodic semiconductor sensitised solar cells as well as their solid-state analogues (SS-CSSC). The work conducted within this doctoral study presents state-of-art materials and thin film processing/preparation methods, their characterisation and developing CSSCs and SS-CSSCs employing such films in cascade configurations. No reports have been published in the literature on SS-CSSC to date. The first stage of this thesis is focused on optimising the morphology and the texture (porosity) of the CuI and NiO semiconductor photocathode, by the introduction of new deposition methods namely, pulsed-electrodeposition (PED) and Aerosol-Assisted Deposition (AAD) and Aerosol-Assisted Chemical Vapour Deposition (AACVD). The electrodes prepared by employing the methods mentioned above and controlling the deposition parameters systematically, we have achieved significant improvement in the film morphology and the texture of the deposited films. The resulting electrodes showed excellent improvement in the photoelectrochemical performance which made it suitable for application in construction of both CSSC and SS-CSSC. The photoelectrochemical performance of the electrodes can be seen clearly through the photocurrent density data. For the case of bare CuI, the PEC performance of electrode prepared by the AAD and PED compared against that of continuous-electrodeposition (ED) electrodes. The photocurrent density achieved for the electrodes prepared by AAD and PED was reported around 175 and 75 µAcm-2 respectively which are way higher than the ED case. At the second stage of this study, the work focused on fabrication and characterisation of the CSSCs. Cathodic sensitised PEC solar cells (CuI/Cu2S/(Eu2+/Eu3+) and NiO/Cu2S/(I3-/I-)) were fabricated by deposition of p-Cu2S on the texture controlled CuI and NiO photocathodes. The morphological properties of the photocathode, in particular layer thickness, particle size and film porosity, play an important role in the PEC performance of CSSCs. Optimisation of these parameters led to increased adsorption of the Cu2S light harvester on the photocathode s surface. As a result, the charge injection from Cu2S to the wide band gap photocathode material (CuI and NiO) was significantly improved. Due to this, the CSSC performance showed significant improvement as semiconductor sensitised cathodic solar cells (CSSC). The IPCE and photocurrent density of the CSSC achieved in this study was around (19 and 7 %) and (1 and 0.5 mAcm-2) for the CuI/Cu2S and NiO/Cu2S electrodes respectively. Finally, the SS-CSSC has been fabricated by employing n-Fe2O3 electron transport layer. The construction of SS-CSSC for the first time using the n-Fe2O3 electron transport layer (CuI/Cu2S/Fe2O3 and NiO/Cu2S/Fe2O3) allowed us to study the materials, optical and photoelectrochemical properties of this device. Under AM 1.5 illumination, the SS-CSSC shows a photocurrent density of 6 and 9 µAcm-2 for CuI/Cu2S/Fe2O3 and NiO/Cu2S/Fe2O3 solar cells, respectively. The results of this work indicated low performance for both SS-CSSC compared to CSSC results, due to the lack of adsorption between the absorber and Fe2O3 electrode. However, this study proved the concept of SS-CSSC based on semiconductor material, which is valuable for the future work of cathodic semiconductor sensitised solar cells as well as solid-state tandem solar cells.