Improving the Morphology Stability of Spiro-OMeTAD Films for Enhanced Thermal Stability of Perovskite Solar Cells.

To guarantee a long lifetime of perovskite-based photovoltaics, the selected materials need to survive relatively high-temperature stress during the solar cell operation. Highly efficient n-i-p perovskite solar cells (PSCs) often degrade at high operational temperatures due to morphological instability of the hole transport material 2,2',7,7'-tetrakis (N,N-di-p-methoxyphenyl-amine)9,9'-spirobifluorene (Spiro-OMeTAD). We discovered that the detrimental large-domain spiro-OMeTAD crystallization is caused by the simultaneous presence of tert-butylpyridine (tBP) additive and gold (Au) as a capping layer. Based on this discovery and our understanding, we demonstrated facile strategies that successfully stabilize the amorphous phase of spiro-OMeTAD film. As a result, the thermal stability of n-i-p PSCs is largely improved. After the spiro-OMeTAD films in the PSCs were stressed for 1032 h at 85 °C in the dark in nitrogen environment, reference PSCs retained only 22% of their initial average power conversion efficiency (PCE), while the best target PSCs retained 85% relative average PCE. Our work suggests facile ways to realize efficient and thermally stable spiro-OMeTAD containing n-i-p PSCs.

Light Management Enhancement for Four-Terminal Perovskite-Silicon Tandem Solar Cells: The Impact of the Optical Properties and Thickness of the Spacer Layer between Sub-Cells.

Mechanical stacking of a thin film perovskite-based solar cell on top of crystalline Si (cSi) solar cell has recently attracted a lot of attention as it is considered a viable route to overcome the limitations of cSi single junction power conversion efficiency. Effective light management is however crucial to minimize reflection or parasitic absorption losses in either the top cell or in the light in-coupling of the transmitted light to the bottom sub-cell. The study here is focused on calculating an optimum performance of a four-terminal mechanically stacked tandem structure by varying the optical property and thickness of the spacer between top and bottom sub-cells. The impact of the nature of the spacer material, with its refractive index and absorption coefficient, as well as the thickness of that layer is used as variables in the optical simulation. The optical simulation is done by using the transfer matrix-method (TMM) on a stack of a semi-transparent perovskite solar cell (top cell) mounted on top of a cSi interdigitated back contact (IBC) solar cell (bottom cell). Two types of perovskite absorber material are considered, with very similar optical properties. The total internal and external short circuit current (Jsc) losses for the semitransparent perovskite top cell as a function of the different optical spacers (material and thickness) are calculated. While selecting the optical spacer materials, Jsc for both silicon (bottom cell) and perovskite (top cell) were considered with the aim to optimize the stack for maximum overall short circuit current. From these simulations, it was found that this optimum in our four-terminal tandem occurred at a thickness of the optical spacer of 160 nm for a material with refractive index n = 1.25. At this optimum, with a combination of selected semi-transparent perovskite top cell, the simulated maximum overall short circuit current (Jsc-combined, max) equals to 34.31 mA/cm². As a result, the four-terminal perovskite/cSi multi-junction solar cell exhibits a power conversion efficiency (PCE) of 25.26%, as the sum of the perovskite top cell PCE = 16.50% and the bottom IBC cSi cell PCE = 8.75%. This accounts for an improvement of more than 2% absolute when compared to the stand-alone IBC cSi solar cell with 23.2% efficiency.

Interfacial Modification for High-Efficiency Vapor-Phase-Deposited Perovskite Solar Cells Based on a Metal Oxide Buffer Layer.

Vacuum deposition is one of the most technologically relevant techniques for the fabrication of perovskite solar cells. The most efficient vacuum-based devices rely on doped organic contacts, compromising the long-term stability of the system. Here, we introduce an inorganic electron-transporting material to obtain power conversion efficiencies matching the best performing vacuum-deposited devices, with open-circuit potential close to the thermodynamic limit. We analyze the leakage current reduction and the interfacial recombination improvement upon use of a thin (<10 nm) interlayer of C60, as well as a more favorable band alignment after a bias/ultraviolet light activation process. This work presents an alternative for organic contacts in highly efficient vacuum-deposited perovskite solar cells.

Highly Efficient and Stable Flexible Perovskite Solar Cells with Metal Oxides Nanoparticle Charge Extraction Layers.

In this study, the fabrication of highly efficient and durable flexible inverted perovskite solar cells (PSCs) is reported. Presynthesized, solution-derived NiOx and ZnO nanoparticles films are employed at room temperature as a hole transport layer (HTL) and electron transport layer (ETL), respectively. The triple cation perovskite films are produced in a single step and for the sake of comparison, ultrasmooth and pinhole-free absorbing layers are also fabricated using MAPbI3 perovskite. The triple cation perovskite cells exhibit champion power conversion efficiencies (PCEs) of 18.6% with high stabilized power conversion efficiency of 17.7% on rigid glass/indium tin oxide (ITO) substrates (comparing with 16.6% PCE with 16.1% stabilized output efficiency for the flexible polyethylene naphthalate (PEN)/thin film barrier/ITO substrates). More interestingly, the durability of flexible PSC under simulation of operative condition is proved. Over 85% of the maximum stabilized output efficiency is retained after 1000 h aging employing a thin MAPbI3 perovskite (over 90% after 500 h with a thick triple cation perovskite). This result is comparable to a similar state of the art rigid PSC and represents a breakthrough in the stability of flexible PSC using ETLs and HTLs compatible with roll to roll production speed, thanks to their room temperature processing.

Nafion-modified MoOx as effective room-temperature hole injection layer for stable, high-performance inverted organic solar cells.

We present a hole injection layer processed from solution at room temperature for inverted organic solar cells. Bis(2,4-pentanedionato) molybdenum(VI) dioxide (MoO2(acac)2) is used as the precursor for MoOx. Small amounts of Nafion in the precursor solution allow it to form continuous films with good wetting onto the active layers. The hydrolysis of MoO2(acac)2 and the effects of adding Nafion to the precursor solution are studied by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The devices with solution-processed MoOx including Nafion exhibited comparable performance to the reference devices based on the commonly used hole injection layers such as poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) or evaporated MoO3. Inverted poly(3-hexylthiophene):[6,6]-phenyl C61-butyric acid methyl ester devices with Nafion-modified MoOx maintain 80% of their initial power conversion efficiency upon exposure to ambient air for ∼5000 h, outperforming devices with PEDOT:PSS or with evaporated MoO3.

Ultrathin ammonium heptamolybdate films as efficient room-temperature hole transport layers for organic solar cells.

Ammonium heptamolybdate (NH4)6Mo7O24·4H2O (AHM) and its peroxo derivatives are analyzed as solution-processed room temperature hole transport layer (HTL) in organic solar cells. Such AHM based HTLs are investigated in devices with three different types of active layers, i.e., solution-processed poly(3-hexylthiophene)/[6,6]-phenyl C61-butyric acid methyl ester(P3HT/PC60BM), poly[N-9'-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)]/[6,6]-phenyl C70-butyric acid methyl ester(PCDTBT/PC70BM) and evaporated small molecule chloro(subphthalocyaninato)boron(III) (SubPc)/C60. By virtue of their high work functions, AHM based HTLs outperform the commonly used poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) HTL for devices employing deep HOMO level active materials. Moreover, devices using AHM based HTLs can achieve higher short circuit current (Jsc) than the ones with evaporated molybdenum oxide(eMoO3), and thus better power conversion efficiency (PCE). In addition, P3HT/PC60BM devices with AHM based HTLs show air stability comparable to those with eMoO3, and much better than the ones with PEDOT:PSS.