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A combination of high-resolution microscopy and photoelectrochemical techniques is used to characterise the photovoltage generated by a TiO2 nanotube-capped SiO2 nano-engineered conical-tip (NTC-CNT) coupled to colloidal quantum dots (QDs). The QD-NTC-CNT is coupled to the gold substrate by means of poly(3-mercaptopropionic acid) (MPA). The NTC-CNT offers optimal charging conditions due to its conical shape, while also allowing one to exploit the unique photovoltaic response of the MPA-capped SiO2 NTC-CNT. We show that the conical shape of the nanotube opens up the possibility of tuning the position of the conical tip with respect to the surface, thus allowing the QD-NTC-CNT to be brought to the minimum of the conical tip potential. A maximum of two QDs per potential well of the NTC-CNT is found by optimising the deposition of the QDs. This is evidenced by a shift in the position of the on-off current transition of the QD-NTC-CNT in the presence of a photoelectron source. Using a single sub-nanometre-diameter (∼1-2 nm) CdSe/CdS core/shell QD coupled to the NTC-CNT, we observe a large photovoltage of ∼850 mV when the Fermi level of the QD-NTC-CNT is aligned with the conical tip minimum. This large photovoltage is attributed to the highly tunable charge separation due to the confined space of the
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