Investigation of Group V doping and passivating oxides to reduce the voltage deficit in CdTe solar cells
Thin film cadmium telluride is one of the most successful photovoltaic technologies on the market today. Second only to silicon in yearly output and accounting for 40% of U.S. utility-scale photovoltaic installation, CdTe is known for its ease of manufacture, ideal bandgap, and low levelized cost of energy. Despite its commercial success, CdTe underperforms compared to its theoretical potential. The current world record CdTe device is only 21.0% compared to a theoretical maximum of 33.1%. This significant discrepancy in efficiencies can mostly be attributed to the poor open-circuit voltage of CdTe devices. Compared to silicon technologies, CdTe has a large voltage deficiency, exceeding 250 mV. While copper doping has traditionally been used for CdTe devices, it has proven to be incapable of sufficiently doping CdTe. Copper typically dopes CdTe in the 1014 to 1015 holes/cm3 range where most models predict that 1016–1017 is needed. Additionally, interstitial copper is a fast diffuser in CdTe, and can lead to numerous stability issues. As an alternative to copper, this work explores arsenic as a dopant for CdTe. Using a novel arsenic doping technique, hole concentrations greater than 1015 cm-3, microsecond lifetimes, and increased radiative efficiency are achieved. These are important prerequisites to achieving higher voltages. Achieving high doping levels alone is not sufficient to achieve higher device performance. A well-passivated and carrier selective contact is needed to ensure that electron-hole pairs do not recombine and are extracted as useable energy. Aluminum oxide has been shown to passivate CdTe surfaces. This work illustrates the explorations of using Al2O¬3 as a passivation layer, pairing it with highly doped amorphous silicon as a hole contact, resulting in excess-carrier lifetimes up to 8 µs, the highest reported to date for polycrystalline Cd(Se)Te. Although the inclusion of arsenic doping and an aluminum oxide back contact are each explored separately, the combination of both methods result in massive improvements to the carrier lifetime, interface passivation and radiative efficiency. Through this combination, microsecond lifetime and External Radiative Efficiency of over 4% are achieved. The excellent ERE values measured here are indicative of large quasi-Fermi level splitting, leading to an implied voltage with multiple device structures of nearly 1 V and an implied voltage of 25%. Finally, while CdSeTe serves as a more promising photovoltaic absorber candidate compared to CdTe, certain difficulties remain which must be addressed. Careful selection of processing conditions is shown to create a dense and large-grained film while eliminating wurtzite-phase crystal growth, which has been shown to degrade device performance. Surprisingly, as-deposited CdSeTe is shown to be n-type or nearly intrinsic rather than the previously supposed p-type. This necessitates additional steps to account for very poor hole conductivity, which can produce zero-current devices if not addressed. Challenges notwithstanding, CdSeTe absorbers are shown to be a key component in devices capable of a photovoltaic conversion efficiency of greater than 25%.
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