Thomas Webb

Over the past decade perovskite solar cells (PSCs) have quickly established themselves as a promising technology boasting both high efficiency and low processing costs. The rapid development and success of PSCs is a product of substantial research effort addressing compositional engineering, thin film fabrication, surface passivation and interfacial treatments. Recently, engineering of the device architecture has entered a renaissance with the emergence of several new bulk and graded heterojunction structures. These structures promote a lateral approach to the development of single-junction PSCs affording new opportunities in light management, defect passivation, carrier extraction and long-term stability. Following a short overview of the historic evolution of PSC architectures, we offer a detailed discussion of the promising progress of the recently reported perovskite bulk heterojunction (BHJ) and graded heterojunction (GHJ) approaches. To enable better understanding of these novel architectures, a range of approaches to characterizing the 2 architectures are presented. Finally, an outlook and perspective are provided offering insights into the future development of PSC architecture engineering.

Triple cation CsFAMA perovskite films fabricated via a one-step method have recently gained attention as an outstanding light-harvesting layer for photovoltaic devices. However, questions remain over the suitability of one-step processes for the production of large-area films, owing to difficulties in controlling the crystallinity, in particular, scaling of the frequently used anti-solvent washing step. This can be mitigated through the use of the two-step method which has recently been used to produce large-area films via techniques such as slot dye coating, spray coating or printing techniques. Nevertheless, the poor solubility of Cs containing salts in IPA solutions has posed a challenge for forming triple cation perovskite films using the two-step method. In this study, we tackle this challenge through fabricating perovskite films on a caesium carbonate (Cs2CO3) precursor layer, enabling Cs incorporation within the film. Synergistically, we find that Cs2CO3 passivates the SnO2 electron transport layer (ETL) through interactions with Sn 3d orbitals, thereby promoting a reduction in trap states. Devices prepared with Cs2CO3 treatment also exhibited an improvement in the power conversion efficiency (PCE) from 19.73% in a control device to 20.96% (AM 1.5G, 100 mW cm−2) in the champion device. The Cs2CO3 treated devices (CsFAMA) showed improved stability, with un-encapsulated devices retaining nearly 80% efficiency after 20 days in ambient air.

Targeted functionalization of 3D perovskite with a 2D passivation layer via R-NH3I treatment has emerged as an effective strategy for enhancing both the efficiency and chemical stability of ABX3 perovskite solar cells, but the underlying mechanisms behind these improvements remain unclear. Here, we assign a passivation mechanism where R-NH3I reacts with excess PbI2 in the MAPbI3 film and unsaturated PbI6 octahedra to form (R-NH3)2(MA)n-1PbnI3n+1. Crucially, we show that precise control of the 2D (R-NH3)2(MA)n-1PbnI3n+1 layer underpins performance improvements: n = 1 yields over a 2-fold improvement in hole injection to the HTL; n > 1 deteriorates hole injection. Ultrafast transient absorption spectroscopy suggests this n-dependence is rooted in the fact that fast (

Interface-mediated recombination losses between perovskite and charge transport layers are one of the main reasons that limit the device performance, in particular for the open-circuit voltage (VOC) of perovskite solar cells (PSCs). Here, functional molecular interface engineering (FMIE) is employed to retard the interfacial recombination losses. The FMIE is a facile solution-processed means that introducing functional molecules, the fluorene-based conjugated polyelectrolyte (CPE) and organic halide salt (OHS) on both contacts of the perovskite absorber layer. Through the FMIE, the champion PSCs with an inverted planar heterojunction structure show a remarkable high VOC of 1.18 V whilst maintaining a fill factor (FF) of 0.83, both of which result in improved power conversion efficiencies (PCEs) of 21.33% (with stabilized PCEs of 21.01%). In addition to achieving one of the highest PCEs in the inverted PSCs, the results also highlight the synergistic effect of these two molecules in improving device performance. Therefore, the study provides a straightforward avenue to fabricate highly efficient inverted PSCs.

Vertically aligned carbon nanotubes (VACNTs) present an exciting avenue for nanoelectronics due to their predetermined orientation and exceptional transport capabilities along the tube length, with the potential to be employed in a variety of optoelectronic applications. However, growth of VACNTs using conventional chemical vapor deposition (CVD) methods requires elevated temperatures (>720 °C) and therefore, the suitability of commonly used transparent conductive oxide (TCO) glasses, such as fluorine‐doped tin oxide (FTO) and indium‐tin oxide (ITO), as the substrates for nanotube growth are limited by their temperature‐sensitive nature. Here, the successful growth of multi‐walled VACNTs directly onto commonly used TCO glasses, FTO and ITO, using the photo‐thermal chemical vapor deposition (PTCVD) growth method is reported. The benefit of reflection, within the infrared region, of the TCO substrate and the effect of surface roughness on the growth of VACNTs is investigated. The application of VACNTs on ITO in inverted planar perovskite solar cells is investigated, which shows superior charge transfer, larger grain sizes in the perovskite film, and a champion device efficiency approaching 16%. Vertically aligned carbon nanotubes are grown directly onto temperature‐sensitive transparent conductive oxide glass; the morphology, quality and electrical properties are analyzed and used to fabricate optimized patterned carbon nanotube forest films which are used in perovskite solar cells to improve charge extraction resulting in a champion efficiency approaching 16%.

Curved X-ray detectors have the potential to revolutionise diverse sectors due to benefits such as reduced image distortion and vignetting compared to their planar counterparts. While the use of inorganic semiconductors for curved detectors are restricted by their brittle nature, organic-inorganic hybrid semiconductors which incorporated bismuth oxide nanoparticles in an organic bulk heterojunction consisting of poly(3-hexylthiophene-2,5-diyl) (P3HT) and [6,6]-phenyl C71 butyric acid methyl ester (PC70BM) are considered to be more promising in this regard. However, the influence of the P3HT molecular weight on the mechanical stability of curved, thick X-ray detectors remains less well understood. Herein, high P3HT molecular weights (>40 kDa) are identified to allow increased intermolecular bonding and chain entanglements, resulting in X-ray detectors that can be curved to a radius as low as 1.3 mm with low deviation in X-ray response under 100 repeated bending cycles while maintaining an industry-standard dark current of

Phosphorene nanoribbons (PNRs) have been widely predicted to exhibit a range of superlative functional properties; however, because they have only recently been isolated, these properties are yet to be shown to translate to improved performance in any application. PNRs show particular promise for optoelectronics, given their predicted high exciton binding energies, tunable bandgaps, and ultrahigh hole mobilities. Here, we verify the theorized enhanced hole mobility in both solar cells and space14 charge-limited-current devices, demonstrating the potential for PNR improving hole extraction in universal optoelectronic applications. Specifically, PNRs are demonstrated to act as an effective charge-selective interlayer by enhancing hole extraction from polycrystalline methylammonium lead iodide (MAPbI3) perovskite to the poly(triarylamine) semiconductor. Introducing PNRs at the hole-transport/MAPbI3 interface achieves fill factors above 0.83 and efficiencies exceeding 21% for planar p−i−n (inverted) perovskite solar cells (PSCs). Such efficiencies are typically only reported in single-crystalline MAPbI3-based inverted PSCs. Methylammonium-free PSCs also benefit from a PNR interlayer, verifying applicability to architectures incorporating mixed perovskite absorber layers. Device photoluminescence and transient absorption spectroscopy are used to demonstrate that the presence of the PNRs drives more effective carrier extraction. Isolation of the PNRs in space-charge-limited-current hole-only devices improves both hole mobility and conductivity, demonstrating applicability beyond PSCs. This work provides primary experimental evidence that the predicted superlative functional properties of PNRs indeed translate to improved optoelectronic performance.