Prof Henry Snaith FRS

Abstract:

Cation-exchange has been used to synthesize PbS/CdS core/shell colloidal quantum dots from PbS starting cores. These were then incorporated as the active material in solar cell test devices using a solution-based, air-ambient, layer-by-layer spin coating process. We show that core/shell colloidal quantum dots can replace their unshelled counterparts with a similar band gap as the active layer in a solar cell device, leading to an improvement in open circuit voltage from 0.42 to 0.66 V. This improvement is attributed to a reduction in recombination as a result of the passivating shell. However, this increase comes at the expense of short circuit current by creating a barrier for transport. To overcome this, we first optimize the shell thickness by varying the conditions for cation-exchange to form the thinnest shell layer possible that provides sufficient surface passivation. Next, ligand exchange with a combination of halide and bifunctional organic molecules is used in conjunction with the core/shell strategy. Power conversion efficiencies of 5.6 ± 0.4% have been achieved with a simple heterojunction device architecture.

Abstract:

© 2014 WILEY-VCH Verlag GmbH & Co. KGaA. Reversible photo-induced performance deterioration is observed in mesoporous TiO2-containing devices in an inert environment. This phenomenon is correlated with the activation of deep trap sites due to astoichiometry of the metal oxide. Interestingly, in air, these defects can be passivated by oxygen adsorption. These results show that the doping of TiO2with aluminium has a striking impact upon the density of sub-gap states and enhances the conductivity by orders of magnitude. Dye-sensitized and perovskite solar cells employing Al-doped TiO2have increased device efficiencies and significantly enhanced operational device stability in inert atmospheres. This performance and stability enhancement is attributed to the substitutional incorporation of Al in the anatase lattice, "permanently" passivating electronic trap sites in the bulk and at the surface of the TiO2.

Abstract:

The solid-state dye-sensitized solar cell (DSSC) was introduced to overcome inherent manufacturing and instability issues of the electrolyte-based DSSC and progress has been made to deliver high photovoltaic efficiencies at low cost. However, despite 15 years research and development, there still remains no clear demonstration of long-term stability. Here, solid-state DSSCs are subjected to the severe aging conditions of continuous illumination at an elevated temperature. A fast deterioration in performance is observed for devices encapsulated in the absence of oxygen. The photovoltaic performance recovers when re-exposed to air. This reversible behavior is attributed to three related processes: i) the creation of light and oxygen sensitive electronic shunting paths between TiO and the top metal electrode, ii) increased recombination at the TiO/organic interface, and iii) the creation of deep electron traps that reduce the photocurrent. The device deterioration is remedied by the formation of an insulating alumino-silicate shell around the TiO nanocrystals, which reduces interfacial recombination, and the introduction of an insulating mesoporous SiO buffer layer between the top electrode and TiO, which acts as a permanent insulating barrier between the TiO and the metal electrode, preventing shunting. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.