Person:

Mangan, Niall

This thesis is composed of two problems. The first is a systems level analysis of the carbon concentrating mechanism in cyanobacteria. The second presents a theoretical analysis of femtosecond laser melting for the purpose of hyperdoping silicon with sulfur. While these systems are very distant, they are both relevant to the development of alternative energy (production of biofuels and methods for fabricating photovoltaics respectively). Both problems are approached through analysis of the underlying diffusion equations.

e quantify the effects of growth temperature on material and deviceproperties of thermally evaporated SnSthin-films and test structures. Grain size, Hall mobility, and majority-carrier concentration monotonically increase with growth temperature. However, the charge collection as measured by the long-wavelength contribution to short-circuit current exhibits a non-monotonic behavior: the collection decreases with increased growth temperature from 150 °C to 240 °C and then recovers at 285 °C. Fits to the experimental internal quantum efficiency using an opto-electronic model indicate that the non-monotonic behavior of charge-carrier collection can be explained by a transition from drift- to diffusion-assisted components of carrier collection. The results show a promising increase in the extracted minority-carrier diffusion length at the highest growth temperature of 285 °C. These findings illustrate how coupled mechanisms can affect early stage device development, highlighting the critical role of direct materials property measurements and simulation.

An outstanding challenge in the development of novel functional materials for optoelectronic devices is identifying suitable charge-carrier contact layers. Herein, we simulate the photovoltaic device performance of various n-type contact material pairings with tin(II) sulfide (SnS), a p-type absorber. The performance of the contacting material, and resulting device efficiency, depend most strongly on two variables: conduction band offset between absorber and contact layer, and doping concentration within the contact layer. By generating a 2D contour plot of device efficiency as a function of these two variables, we create a performance-space plot for contacting layers on a given absorber material. For a simulated high-lifetime SnS absorber, this 2D performance-space illustrates two maxima, one local and one global. The local maximum occurs over a wide range of contact-layer doping concentrations (below 1016 cm−3), but only a narrow range of conduction band offsets (0 to −0.1 eV), and is highly sensitive to interface recombination. This first maximum is ideal for early-stage absorber research because it is more robust to low bulk-minority-carrier lifetime and pinholes (shunts), enabling device efficiencies approaching half the Shockley-Queisser limit, greater than 16%. The global maximum is achieved with contact-layer doping concentrations greater than 1018 cm−3, but for a wider range of band offsets (−0.1 to 0.2 eV), and is insensitive to interface recombination. This second maximum is ideal for high-quality films because it is more robust to interface recombination, enabling device efficiencies approaching the Shockley-Queisser limit, greater than 20%. Band offset measurements using X-ray photoelectron spectroscopy and carrier concentration approximated from resistivity measurements are used to characterize the zinc oxysulfide contacting layers in recent record-efficiency SnS devices. Simulations representative of these present-day devices suggest that record efficiency SnS devices are optimized for the second local maximum, due to low absorber lifetime and relatively well passivated interfaces. By employing contact layers with higher carrier concentrations and lower electron affinities, a higher efficiency ceiling can be enabled.