on PERC technologies and get even closer to the theoretical single-junction efficiency limit, electrical losses in the contacted regions must be reduced. [3][4][5] Passivating contacts can help alleviate such losses by simultaneously suppressing the current of non-collected carriers to the contact, and by reducing recombination sites at the interface. Introducing a passivating interlayer between the metal/silicon interface provides a route to reducing the recombination current density, J 0 , [6,7] thereby increasing device voltage. [3] Passivating contacts have achieved some success to date, with the strongest candidates being polysilicon on top of thin silicon oxide layers (e.g., tunnel oxide passivating contacts (TOPCon) or poly silicon on oxide (POLO)) and amorphous silicon (a-Si) heterojunctions. [3,7,8] TOPCon is an efficient electron-selective contact but has a high thermal budget with temperatures around 900 °C needed to reduce the contact resistivity to acceptable levels. [9] An efficient hole-selective layer that can match or exceed the performance of the current electron-selective materials would be of considerable interest. The use of SiO 2 -based hole-selective contacts has so far failed to reach equivalent levels. [10,11] The most promising hole-selective contacting materials are p-type a-Si and siliconrich SiC, but conventional high-temperature Ag screen printing methods are not necessarily compatible with such contacts. [10] Surface passivating thin films are crucial for limiting the electrical losses during charge carrier collection in silicon photovoltaic devices. Certain dielectric coatings of more than 10 nm provide excellent surface passivation, and ultra-thin (<2 nm) dielectric layers can serve as interlayers in passivating contacts. Here, ultra-thin passivating films of SiO 2 , Al 2 O 3 , and HfO 2 are created via plasma-enhanced atomic layer deposition and annealing. It is found that thin negatively charged HfO 2 layers exhibit excellent passivation properties-exceeding those of SiO 2 and Al 2 O 3 -with 0.9 nm HfO 2 annealed at 450 °C providing a surface recombination velocity of 18.6 cm s −1 . The passivation quality is dependent on annealing temperature and layer thickness, and optimum passivation is achieved with HfO 2 layers annealed at 450 °C measured to be 2.2-3.3 nm thick which give surface recombination velocities ≤2.5 cm s −1 and J 0 values of ≈14 fA cm −2 . The superior passivation quality of HfO 2 nanolayers makes them a promising candidate for future passivating contacts in high-efficiency silicon solar cells.