Thermal and Environmental Stability of Semi-Transparent Perovskite Solar Cells for Tandems Enabled by a Solution-Processed Nanoparticle Buffer Layer and Sputtered ITO Electrode.

A sputtered oxide layer enabled by a solution-processed oxide nanoparticle buffer layer to protect underlying layers is used to make semi-transparent perovskite solar cells. Single-junction semi-transparent cells are 12.3% efficient, and mechanically stacked tandems on silicon solar cells are 18.0% efficient. The semi-transparent perovskite solar cell has a T 80 lifetime of 124 h when operated at the maximum power point at 100 °C without additional sealing in ambient atmosphere under visible illumination.

Enhancing the hole-conductivity of spiro-OMeTAD without oxygen or lithium salts by using spiro(TFSI)2 in perovskite and dye-sensitized solar cells.

2,2',7,7'-Tetrakis(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (spiro-OMeTAD), the prevalent organic hole transport material used in solid-state dye-sensitized solar cells and perovskite-absorber solar cells, relies on an uncontrolled oxidative process to reach appreciable conductivity. This work presents the use of a dicationic salt of spiro-OMeTAD, named spiro(TFSI)2, as a facile means of controllably increasing the conductivity of spiro-OMeTAD up to 10(-3) S cm(-1) without relying on oxidation in air. Spiro(TFSI)2 enables the first demonstration of solid-state dye-sensitized solar cells fabricated and operated with the complete exclusion of oxygen after deposition of the sensitizer with higher and more reproducible device performance. Perovskite-absorber solar cells fabricated with spiro(TFSI)2 show improved operating stability in an inert atmosphere. Gaining control of the conductivity of the HTM in both dye-sensitized and perovskite-absorber solar cells in an inert atmosphere using spiro(TFSI)2 is an important step toward the commercialization of these technologies.

Melt-infiltration of spiro-OMeTAD and thermal instability of solid-state dye-sensitized solar cells.

A method for achieving complete pore-filling in solid-state dye-sensitized solar cells termed melt-infiltration is presented: after the customary solution-processed deposition of spiro-OMeTAD, the device is heated above the glass transition temperature of spiro-OMeTAD to soften the material and allow capillary action to pull additional spiro-OMeTAD from the overlayer reservoir into the pores. The pore-filling fraction increases from 60-65% to 90-100% as a result of melt-infiltration. The organic D-π-A dye used in this study is found to withstand the thermal treatment without performance loss, unlike ruthenium-based dyes. Through our experiments, we find that the 4-tert-butylpyridine (tBP) additive, commonly used in dye-sensitized solar cells, evaporates from the device during heat treatment at temperatures as low as 85 °C. This significantly impacts device performance, potentially excluding its use in commercial applications, and demonstrates the need for a more thermally stable tBP alternative. Melt-infiltration is expected to be a viable method for achieving complete pore-filling in systems where volatile additives are not required for operation.

The importance of dye chemistry and TiCl4 surface treatment in the behavior of Al2O3 recombination barrier layers deposited by atomic layer deposition in solid-state dye-sensitized solar cells.

Atomic layer deposition (ALD) was used to fabricate Al(2)O(3) recombination barriers in solid-state dye-sensitized solar cells (ss-DSSCs) employing an organic hole transport material (HTM) for the first time. Al(2)O(3) recombination barriers of varying thickness were incorporated into efficient ss-DSSCs utilizing the Z907 dye adsorbed onto a 2 µm-thick nanoporous TiO(2) active layer and the HTM spiro-OMeTAD. The impact of Al(2)O(3) barriers was also studied in devices employing different dyes, with increased active layer thicknesses, and with substrates that did not undergo the TiCl(4) surface treatment. In all instances, electron lifetimes (as determined by transient photovoltage measurements) increased and dark current was suppressed after Al(2)O(3) deposition. However, only when the TiCl(4) treatment was eliminated did device efficiency increase; in all other instances efficiency decreased due to a drop in short-circuit current. These results are attributed in the former case to the similar effects of Al(2)O(3) ALD and the TiCl(4) surface treatment whereas the insulating properties of Al(2)O(3) hinder charge injection and lead to current loss in TiCl(4)-treated devices. The impact of Al(2)O(3) barrier layers was unaffected by doubling the active layer thickness or using an alternative ruthenium dye, but a metal-free donor-π-acceptor dye exhibited a much smaller decrease in current due to its higher excited state energy. We develop a model employing prior research on Al(2)O(3) growth and dye kinetics that successfully predicts the reduction in device current as a function of ALD cycles and is extendable to different dye-barrier systems.