The relative abundances of Sn, Te, Xe, Ba, and Ce in the cosmic radiation

Elements with even atomic number (Z) in the interval 50 ≤ Z ≤ 58 have been resolved in the cosmic radiation using the Heavy Nuclei Experiment on the HEAO-3 satellite. Their relative abundances have been compared with the results expected from pure r-process material, pure s-process material, and solar system material, both with and without a modification due to possible first ionization potential effects. Such effects may be the result of the preferential acceleration, and hence enhancement in the cosmic rays, or those elements having low first ionization potentials. We find that our measurements are inconsistent with pure r-process material at the greater than 98% confidence level whether or not the first ionization potential adjustments are made.

In addition, we have compared our results with mixtures having varying ratios of pure r-process material to pure s-process material. We find that, if no first ionization potential effects are included,

(r/s)CRS/(r/s)SS = 0.20^+0.18_-0.14

where CRS refers to the cosmic ray source and SS refers to the solar system, consistent with having an almost pure s-process source. If the first ionization potential adjustments are applied

(r/s)CRS/(r/s)SS = 1.5^+1.1_-0.7

consistent with a solar system mixture.

Earth-abundant materials for solar hydrogen generation

A critical challenge for the 21st century is shifting from the predominant use of fossil fuels to renewables for energy. Among many options, sunlight is the only single renewable resource with sufficient abundance to replace most or all of our current fossil energy use. However, existing photovoltaic and solar thermal technologies cannot be scaled infinitely due to the temporal and geographic intermittency of sunlight. Therefore efficient and inexpensive methods for storage of solar energy in a dense medium are needed in order to greatly increase utilization of the sun as a primary resource. For this purpose we have proposed an artificial photosynthetic system consisting of semiconductors, electrocatalysts, and polymer membranes to carry out photoelectrochemical water splitting as a method for solar fuel generation.

This dissertation describes efforts over the last five years to develop critical semiconductor and catalyst components for efficient and scalable photoelectrochemical hydrogen evolution, one of the half reactions for water splitting. We identified and developed Ni–Mo alloy and Ni₂P nanoparticles as promising earth-abundant electrocatalysts for hydrogen evolution. We thoroughly characterized Ni–Mo alloys alongside Ni and Pt catalysts deposited onto planar and structured Si light absorbers for solar hydrogen generation. We sought to address several key challenges that emerged in the use of non-noble catalysts for solar fuels generation, resulting in the synthesis and characterization of Ni–Mo nanopowder for use in a new photocathode device architecture. To address the mismatch in stability between non-noble metal alloys and Si absorbers, we also synthesized and characterized p-type WSe₂ as a candidate light absorber alternative to Si that is stable under acidic and alkaline conditions.

Photonic and Device Design Principles for Ultrahigh-Efficiency (>50%), Spectrum-Splitting Photovoltaics

The sun has the potential to power the Earth's total energy needs, but electricity from solar power still constitutes an extremely small fraction of our power generation because of its high cost relative to traditional energy sources. Therefore, the cost of solar must be reduced to realize a more sustainable future. This can be achieved by significantly increasing the efficiency of modules that convert solar radiation to electricity. In this thesis, we consider several strategies to improve the device and photonic design of solar modules to achieve record, ultrahigh (> 50%) solar module efficiencies. First, we investigate the potential of a new passivation treatment, trioctylphosphine sulfide, to increase the performance of small GaAs solar cells for cheaper and more durable modules. We show that small cells (mm2), which currently have a significant efficiency decrease (~ 5%) compared to larger cells (cm2) because small cells have a higher fraction of recombination-active surface from the sidewalls, can achieve significantly higher efficiencies with effective passivation of the sidewalls. We experimentally validate the passivation qualities of treatment by trioctylphosphine sulfide (TOP:S) through four independent studies and show that this facile treatment can enable efficient small devices. Then, we discuss our efforts toward the design and prototyping of a spectrum-splitting module that employs optical elements to divide the incident spectrum into different color bands, which allows for higher efficiencies than traditional methods. We present a design, the polyhedral specular reflector, that has the potential for > 50% module efficiencies even with realistic losses from combined optics, cell, and electrical models. Prototyping efforts of one of these designs using glass concentrators yields an optical module whose combined spectrum-splitting and concentration should correspond to a record module efficiency of 42%. Finally, we consider how the manipulation of radiatively emitted photons from subcells in multijunction architectures can be used to achieve even higher efficiencies than previously thought, inspiring both optimization of incident and radiatively emitted photons for future high efficiency designs. In this thesis work, we explore novel device and photonic designs that represent a significant departure from current solar cell manufacturing techniques and ultimately show the potential for much higher solar cell efficiencies.