The functionality of a novel 3-dimensional betavoltaic battery design will be investigated to improve conversion efficiency over existing planar devices. A beta-emitting isotope of nickel, Ni-63, is embedded in the volume of empty space between self-assisted p-i-n junction gallium phosphide nanowires to improve the beta capture efficiency. Parameters such as nanowire pitch, diameter, and height will influence the efficiency and were investigated thoroughly. Material selection was performed based on the following considerations. Gallium phosphide is chosen to achieve a high open circuit voltage under beta exposure. Ni-63 has an optimal beta energy spectrum for a nanowire device and a half-life of 101 years for long term application. The majority of the work focused on the development of the fabrication process, particularly the radioactive source deposition. The method used for embedding the source was a citrate-based sol-gel which was spun onto the sample. This method was modified for this nanowire application and specific challenges to the process are outlined. Furthermore, the obstacles of working with radioactive materials will be discussed. The first nanowire-based betavoltaic device is reported to produce beta-generated current and achieved a beta conversion efficiency of 0.03%. Investigation of the junction was performed to provide future improvements to the efficiency. Additionally, simulated IV curves for a non-active sample exhibited a possible conversion efficiency of 1.92%. / Thesis / Master of Applied Science (MASc)

In order to increase the efficiency of betavoltaic devices, an architecture utilizing nanowires has been developed. In this architecture, a radioisotope is deposited between a nanowire array in order to increase the fraction of beta particles captured by the semiconductor converter and minimize the energy lost to self-shielding. Previous work has prototyped such a design; however, performance was limited to an efficiency of 0.5%. This thesis outlines the design and optimization of the nanowire-based betavoltaic generator. Both the nanowire array geometry and the nanowire p-i-n diode design are optimized for maximum radiation capture and conversion efficiency, respectively. First, a model was developed in the GEANT4 Monte Carlo toolkit in order to investigate the radiation capture of various array geometries. Radioisotope sources of elemental 3H, 63Ni, and 147Pm, as well as compounds of each were examined with gallium phosphide nanowires. Overall, it was found that nanowires should be grown as long as possible to accommodate the most source material while the ratio of the diameter to array pitch can be optimized for maximum power capture. Optimized arrays presented an improvement in energy capture of approximately 6 and 15 times for 63Ni and 3H devices, respectively, while 147Pm devices indicated no improvement. Optimized array geometry was extended to both silicon and gallium arsenide and the radiation capture simulations were coupled to drift-diffusion calculations in COMSOL Multiphysics for axial junction nanowires. Following the junction optimization, devices were predicted to be between 4 and 10% efficient with power outputs ranging from 2 to 6 μW cm^-2. Despite the large improvement compared to experimental results, surface recombination was found to limit the performance of long gallium phosphide nanowires. Therefore, core-shell junctions were then investigated and found to improve upon all axial designs. Overall, it has been determined that the nanowire device design is advantageous over planar betavoltaics due to the mitigation of self-shielding effects. Devices utilizing 10 μm long gallium phosphide core-shell nanowires with a 3H source are predicted to achieve the top performance of 12% effciency and a power density of 7 μW cm^-2. In addition, gallium phosphide and gallium arsenide devices with 63Ni are able to achieve an energy density in excess of 1 Wh cm^-2 due to the long half-life. / Thesis / Master of Applied Science (MASc) / Widely used batteries, such as lithium-polymer cells, are bulky and suffer from short discharge times or temperature sensitivity. Betavoltaics - also known as "nuclear batteries" - offer an opportunity to surpass these issues. Beta particles, or energetic electrons, are the result of certain nuclear decay reactions. Betavoltaic batteries create electricity from these particles, can remain active for hundreds of years, and are insensitive to environmental conditions. In addition, these particles are easy to shield, rendering them safe for users. This work focuses on a new type of betavoltaic which uses nanowires to capture more beta particles and ultimately improve performance. These devices have been designed through a simulation-based approach that has maximized the total power output as well as effciency by fine-tuning different parameters. The designs described in this work exhibit huge improvements over conventional devices and will allow nanowire-based betavoltaics to compete with the top performing devices developed to date.

<div>In this work new methodologies for measuring and monitoring nuclear decay parameters is explored. A determination of the tritium half-life by measuring the current of a betavoltaic device is presented. The benefits of this approach in exploring the possibility of time dependence of nuclear decay parameters is discussed.</div>