Design Approaches for Enhancing Photovoltaic Performance of Silicon Solar Cells Sensitized by Proximal Nanocrystalline Quantum Dots
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Energy transfer (ET) based sensitization of silicon (Si) using proximal nanocrystal quantum dots (NQDs) has been studied extensively in recent years as a means to develop thin and flexible Si based solar cells. The driving force for this research activity is a reduction in materials cost. To date, the main method for determining the role of ET in sensitizing Si has been optical spectroscopic studies. The quantitative contribution from two modes of ET (namely, nonradiative and radiative) has been reported using time-resolved photoluminescence (TRPL) spectroscopy coupled with extensive theoretical modelling. Thus, optical techniques have established the potential for utilizing ET based sensitization of Si as a feasible way to develop novel NQD-Si hybrid solar cells. However, the ultimate measure of the efficiency of ET-based mechanisms is the generation of electron-hole pairs by the impinging photons. It is therefore important to perform electrical measurements. However, only a couple of studies have attempted electrical quantification of ET modes. A few studies have focused on photocurrent measurements, without considering industrially relevant photovoltaic (PV) systems. Therefore, there is a need to develop a systematic approach for the electrical quantification of ET-generated charges and to help engineer new PV architectures optimized for harnessing the full advantages of ET mechanisms. Within this context, the work presented in this dissertation aims to develop an experimental testing protocol that can be applied to different PV structures for quantifying ET contributions from electrical measurements. We fabricated bulk Si solar cells (SCs) as a test structure and utilized CdSe/ZnS NQDs for ET based sensitization. The NQD-bulk Si hybrid devices showed ~30% PV enhancement after NQD deposition. We measured external quantum efficiency (EQE) of these devices to quantify ET-generated charges. Reflectance measurements were also performed to decouple contributions of intrinsic optical effects (i.e., anti-reflection) from NQD mediated ET processes. Our analysis indicates that the contribution of ET-generated charges cannot be detected by EQE measurements. Instead, changes in the optical properties (i.e., anti-reflection property) due to the NQD layer are found to be the primary source of the photocurrent enhancement. Based on this finding, we propose to minimize bulk Si absorption by using an ultrathin (~300 nm) Si PV architecture which should enable measurements of ET-generated charges. We describe an optimized process flow for fabricating such ultrathin Si devices. The devices fabricated by this method behave like photo-detectors and show enhanced sensitivity under 1 Sun AM1.5G illumination. The geometry and process flow of these devices make it possible to incorporate NQDs for sensitization. Overall, this dissertation provides a protocol for the quantification of ET-generated charges and documents an optimized process flow for the development of an ultrathin Si solar cells.