Heterojunctions of carbon nanotubes interfaced with silicon and doped with AuCl3 can achieve attractive power conversion efficiencies when operated in the photovoltaic regime; however, the cost and long-term stability of such devices must be improved before they could become commercially viable. Here, we investigate the role of chemical treatment of the carbon nanotube/silicon interface with either SOCl2 or HNO3, prior to AuCl3 doping, on the stability of the photovoltaic devices. We find that while both treatments initially lead to similar device performance, devices treated with HNO3 are significantly more stable. Using X-ray photoemission spectroscopy, we demonstrate that pretreatment with the powerful organic oxidant SOCl2 generates a variety of low-oxidation-state silicon species at the nanotube-silicon interface that are not generated by exposure to HNO3. These species and their evolution over time are implicated in the reduced device stability, highlighting the importance of silicon oxidation states in determining the stability of carbon nanotube-silicon photovoltaic devices.
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