Browsing by Author "Shafiq, Natis"
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Item Design Approaches for Enhancing Photovoltaic Performance of Silicon Solar Cells Sensitized by Proximal Nanocrystalline Quantum Dots(2017-07-24) Shafiq, Natis; 0000 0000 4239 3958 (Chabal, YJ); Chabal, Yves J.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.Item Morphology and Chemical Termination of HF-Etched Si₃N₄ Surfaces(American Institute of Physics Inc.) Liu, Li-Hong; Debenedetti, William J. I.; Peixoto, Tatiana; Gokalp, Sumeyra; Shafiq, Natis; Veyan, Jean-François; Michalak, D. J.; Hourani, R.; Chabal, Yves J.Several reports on the chemical termination of silicon nitride films after HF etching, an important process in the microelectronics industry, are inconsistent claiming N-Hx, Si-H, or fluorine termination. An investigation combining infrared and x-ray photoelectron spectroscopies with atomic force and scanning electron microscopy imaging reveals that under some processing conditions, salt microcrystals are formed and stabilized on the surface, resulting from products of Si₃N₄ etching. Rinsing in deionized water immediately after HF etching for at least 30s avoids such deposition and yields a smooth surface without evidence of Si-H termination. Instead, fluorine and oxygen are found to terminate a sizeable fraction of the surface in the form of Si-F and possibly Si-OH bonds. The fluorine termination is remarkably stable in air and water vapor in ambient conditions, with clear implications on further surface chemical functionalization.Item Structural Band-Gap Tuning in g-C₃N₄(Royal Society of Chemistry) Zuluaga, S.; Liu, Li-Hong; Shafiq, Natis; Rupich, Sara M.; Veyan, Jean-François; Chabal, Yves J.; Thonhauser, T.g-C3N4 is a promising material for hydrogen production from water via photo-catalysis, if we can tune its band gap to desirable levels. Using a combined experimental and ab initio approach, we uncover an almost perfectly linear relationship between the band gap and structural aspects of g-C3N4, which we show to originate in a changing overlap of wave functions associated with the lattice constants. This changing overlap, in turn, causes the unoccupied pz states to experience a significantly larger energy shift than any other occupied state (s, px, or py), resulting in this peculiar relationship. Our results explain and demonstrate the possibility to tune the band gap by structural means, and thus the frequency at which g-C3N4 absorbs light.Item Structural Band-Gap Tuning in g-C₃N₄(The Royal Society of Chemistry) Zuluaga, S.; Liu, Li-Hong; Shafiq, Natis; Rupich, Sara M.; Veyan, Jean-François; Chabal, Yves J.; Thonhauser, T.g-C₃N₄ is a promising material for hydrogen production from water via photo-catalysis, if we can tune its band gap to desirable levels. Using a combined experimental and ab initio approach, we uncover an almost perfectly linear relationship between the band gap and structural aspects of g-C₃N₄, which we show to originate in a changing overlap of wave functions associated with the lattice constants. This changing overlap, in turn, causes the unoccupied pz states to experience a significantly larger energy shift than any other occupied state (s, p(x), or p(y)), resulting in this peculiar relationship. Our results explain and demonstrate the possibility to tune the band gap by structural means, and thus the frequency at which g-C₃N₄ absorbs light.