18.73% efficient and stable inverted organic photovoltaics featuring a hybrid hole-extraction layer.

Developing efficient and stable organic photovoltaics (OPVs) is crucial for the technology's commercial success. However, combining these key attributes remains challenging. Herein, we incorporate the small molecule 2-((3,6-dibromo-9H-carbazol-9-yl)ethyl)phosphonic acid (Br-2PACz) between the bulk-heterojunction (BHJ) and a 7 nm-thin layer of MoO3 in inverted OPVs, and study its effects on the cell performance. We find that the Br-2PACz/MoO3 hole-extraction layer (HEL) boosts the cell's power conversion efficiency (PCE) from 17.36% to 18.73% (uncertified), making them the most efficient inverted OPVs to date. The factors responsible for this improvement include enhanced charge transport, reduced carrier recombination, and favourable vertical phase separation of donor and acceptor components in the BHJ. The Br-2PACz/MoO3-based OPVs exhibit higher operational stability under continuous illumination and thermal annealing (80 °C). The T80 lifetime of OPVs featuring Br-2PACz/MoO3 - taken as the time over which the cell's PCE reduces to 80% of its initial value - increases compared to MoO3-only cells from 297 to 615 h upon illumination and from 731 to 1064 h upon continuous heating. Elemental analysis of the BHJs reveals the enhanced stability to originate from the partially suppressed diffusion of Mo ions into the BHJ and the favourable distribution of the donor and acceptor components induced by the Br-2PACz.

Bismuth-based mixed-anion compounds for anode materials in rechargeable batteries.

A facile solvothermal synthesis approach for chemical composition control in ternary Bi-S-I systems is reported by simply controlling the sulfide concentration. We demonstrate the application of these bismuth-based ternary mixed-anion compounds as high capacity anode materials in rechargeable batteries. Cells utilising Bi13S18I2 achieved an initial capacity value of 807 mA h g-1, while those with BiSI/Bi13S18I2 a value of 1087 mA h g-1 in lithium-ion battery systems.

Scaled Deposition of Ti3C2Tx MXene on Complex Surfaces: Application Assessment as Rear Electrodes for Silicon Heterojunction Solar Cells.

Two-dimensional transition metal carbides (MXenes) are of great interest as electrode materials for a variety of applications, including solar cells, due to their tunable optoelectronic properties, high metallic conductivity, and attractive solution processability. However, thus far, MXene electrodes have only been exploited for lab-scale device applications. Here, to demonstrate the potential of MXene electrodes at an industry-relevant level, we implemented a scalable spray coating technique to deposit highly conductive (ca. 8000 S/cm, at a ca. 55 nm thickness) Ti3C2Tx films (Tx: surface functional groups, i.e., -OH, -O, -F) via an automated spray system. We employed these Ti3C2Tx films as rear electrodes for silicon heterojunction solar cells as a proof of concept. The spray-deposited MXene flakes have formed a conformal coating on top of the indium tin oxide (ITO)-coated random pyramidal textured silicon wafers, leading to >20% power conversion efficiency (PCE) over both medium-sized (4.2 cm2) and large (243 cm2, i.e., industry-sized 6 in. pseudosquare wafers) cell areas. Notably, the Ti3C2Tx-rear-contacted devices have retained around 99% of their initial PCE for more than 600 days of ambient air storage. Their performance is comparable with state-of-the-art solar cells contacted with sputtered silver electrodes. Our findings demonstrate the high-throughput potential of spray-coated MXene-based electrodes for solar cells in addition to a wider variety of electronic device applications.

18.4 % Organic Solar Cells Using a High Ionization Energy Self-Assembled Monolayer as Hole-Extraction Interlayer.

Self-assembled monolayers (SAMs) based on Br-2PACz ([2-(3,6-dibromo-9H-carbazol-9-yl)ethyl]phosphonic acid) 2PACz ([2-(9H-Carbazol-9-yl)ethyl]phosphonic acid) and MeO-2PACz ([2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid) molecules were investigated as hole-extracting interlayers in organic photovoltaics (OPVs). The highest occupied molecular orbital (HOMO) energies of these SAMs were measured at -6.01 and -5.30 eV for Br-2PACz and MeO-2PACz, respectively, and found to induce significant changes in the work function (WF) of indium-tin-oxide (ITO) electrodes upon chemical functionalization. OPV cells based on PM6 (poly[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione)]) : BTP-eC9 : PC71 BM ([6,6]-phenyl-C71-butyric acid methyl ester) using ITO/Br-2PACz anodes exhibited a maximum power conversion efficiency (PCE) of 18.4 %, outperforming devices with ITO/MeO-2PACz (14.5 %) and ITO/poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT : PSS) (17.5 %). The higher PCE was found to originate from the much higher WF of ITO/Br-2PACz (-5.81 eV) compared to ITO/MeO-2PACz (4.58 eV) and ITO/PEDOT : PSS (4.9 eV), resulting in lower interface resistance, improved hole transport/extraction, lower trap-assisted recombination, and longer carrier lifetimes. Importantly, the ITO/Br-2PACz electrode was chemically stable, and after removal of the SAM it could be recycled and reused to construct fresh OPVs with equally impressive performance.

Dopant-Assisted Matrix Stabilization Enables Thermoelectric Performance Enhancement in n-Type Quantum Dot Films.

Efficient thermoelectric generators require further progress in developing n-type semiconductors that combine low thermal conductivity with high electrical conductivity. By embedding colloidal quantum dots (CQDs) in a metal halide matrix (QDMH), the metal halide matrix can enhance phonon scattering, thus suppressing thermal transport; however, simultaneously achieving high electrical conductivity in such systems has previously been limited by the deleterious impact of a large density of interfaces on charge transport. Therefore, new strategies are needed to improve charge carrier transport without sacrificing matrix-enabled low thermal transport. Here, we report the use of chemical doping in the solution state to improve electron transport while maintaining low thermal transport in QDMH films. By incorporating cesium carbonate (Cs2CO3) salts as a dopant prior to matrix formation, we find that the dopant stabilizes the matrix in colloidal inks and enables efficient n-type doping in QDMH films. As a result, this strategy leads to an enhanced n-type thermoelectric behavior in solution-processed QDMH films near room temperature, with a thermal conductivity of 0.25 W m-1 K-1-significantly lower than in prior films based on organic-ligand-cross-linked CQD films (>0.6 W m-1 K-1) and spark-plasma-sintered CQD systems (>1 W m-1 K-1). This study provides a pathway to developing efficient n-type thermoelectric materials with low thermal conductivity using single-step deposition and low-temperature processing.

Rapid Photonic Processing of High-Electron-Mobility PbS Colloidal Quantum Dot Transistors.

Recent advances in solution-processable semiconducting colloidal quantum dots (CQDs) have enabled their use in a range of (opto)electronic devices. In most of these studies, device fabrication relied almost exclusively on thermal annealing to remove organic residues and enhance inter-CQD electronic coupling. Despite its widespread use, however, thermal annealing is a lengthy process, while its effectiveness to eliminate organic residues remains limited. Here, we exploit the use of xenon flash lamp sintering to post-treat solution-deposited layers of lead sulfide (PbS) CQDs and their application in n-channel thin-film transistors (TFTs). The process is simple, fast, and highly scalable and allows for efficient removal of organic residues while preserving both quantum confinement and high channel current modulation. Bottom-gate, top-contact PbS CQD TFTs incorporating SiO2 as the gate dielectric exhibit a maximum electron mobility of 0.2 cm2 V-1 s-1, a value higher than that of control transistors (≈10-2 cm2 V-1 s-1) processed via thermal annealing for 30 min at 120 °C. Replacing SiO2 with a polymeric dielectric improves the transistor's channel interface, leading to a significant increase in electron mobility to 3.7 cm2 V-1 s-1. The present work highlights the potential of flash lamp annealing as a promising method for the rapid manufacture of PbS CQD-based (opto)electronic devices and circuits.

17% Efficient Organic Solar Cells Based on Liquid Exfoliated WS2 as a Replacement for PEDOT:PSS.

The application of liquid-exfoliated 2D transition metal disulfides (TMDs) as the hole transport layers (HTLs) in nonfullerene-based organic solar cells is reported. It is shown that solution processing of few-layer WS2 or MoS2 suspensions directly onto transparent indium tin oxide (ITO) electrodes changes their work function without the need for any further treatment. HTLs comprising WS2 are found to exhibit higher uniformity on ITO than those of MoS2 and consistently yield solar cells with superior power conversion efficiency (PCE), improved fill factor (FF), enhanced short-circuit current (JSC ), and lower series resistance than devices based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) and MoS2 . Cells based on the ternary bulk-heterojunction PBDB-T-2F:Y6:PC71 BM with WS2 as the HTL exhibit the highest PCE of 17%, with an FF of 78%, open-circuit voltage of 0.84 V, and a JSC of 26 mA cm-2 . Analysis of the cells' optical and carrier recombination characteristics indicates that the enhanced performance is most likely attributed to a combination of favorable photonic structure and reduced bimolecular recombination losses in WS2 -based cells. The achieved PCE is the highest reported to date for organic solar cells comprised of 2D charge transport interlayers and highlights the potential of TMDs as inexpensive HTLs for high-efficiency organic photovoltaics.

Dependence of crystallite formation and preferential backbone orientations on the side chain pattern in PBDTTPD polymers.

Alkyl substituents appended to the π-conjugated main chain account for the solution-processability and film-forming properties of most π-conjugated polymers for organic electronic device applications, including field-effect transistors (FETs) and bulk-heterojunction (BHJ) solar cells. Beyond film-forming properties, recent work has emphasized the determining role that side-chain substituents play on polymer self-assembly and thin-film nanostructural order, and, in turn, on device performance. However, the factors that determine polymer crystallite orientation in thin-films, implying preferential backbone orientation relative to the device substrate, are a matter of some debate, and these structural changes remain difficult to anticipate. In this report, we show how systematic changes in the side-chain pattern of poly(benzo[1,2-b:4,5-b']dithiophene-alt-thieno[3,4-c]pyrrole-4,6-dione) (PBDTTPD) polymers can (i) influence the propensity of the polymer to order in the π-stacking direction, and (ii) direct the preferential orientation of the polymer crystallites in thin films (e.g., "face-on" vs "edge-on"). Oriented crystallites, specifically crystallites that are well-ordered in the π-stacking direction, are believed to be a key contributor to improved thin-film device performance in both FETs and BHJ solar cells.

Importance of the donor:fullerene intermolecular arrangement for high-efficiency organic photovoltaics.

The performance of organic photovoltaic (OPV) material systems are hypothesized to depend strongly on the intermolecular arrangements at the donor:fullerene interfaces. A review of some of the most efficient polymers utilized in polymer:fullerene PV devices, combined with an analysis of reported polymer donor materials wherein the same conjugated backbone was used with varying alkyl substituents, supports this hypothesis. Specifically, the literature shows that higher-performing donor-acceptor type polymers generally have acceptor moieties that are sterically accessible for interactions with the fullerene derivative, whereas the corresponding donor moieties tend to have branched alkyl substituents that sterically hinder interactions with the fullerene. To further explore the idea that the most beneficial polymer:fullerene arrangement involves the fullerene docking with the acceptor moiety, a family of benzo[1,2-b:4,5-b']dithiophene-thieno[3,4-c]pyrrole-4,6-dione polymers (PBDTTPD derivatives) was synthesized and tested in a variety of PV device types with vastly different aggregation states of the polymer. In agreement with our hypothesis, the PBDTTPD derivative with a more sterically accessible acceptor moiety and a more sterically hindered donor moiety shows the highest performance in bulk-heterojunction, bilayer, and low-polymer concentration PV devices where fullerene derivatives serve as the electron-accepting materials. Furthermore, external quantum efficiency measurements of the charge-transfer state and solid-state two-dimensional (2D) (13)C{(1)H} heteronuclear correlation (HETCOR) NMR analyses support that a specific polymer:fullerene arrangement is present for the highest performing PBDTTPD derivative, in which the fullerene is in closer proximity to the acceptor moiety of the polymer. This work demonstrates that the polymer:fullerene arrangement and resulting intermolecular interactions may be key factors in determining the performance of OPV material systems.

Highly transparent and UV-resistant superhydrophobic SiO(2)-coated ZnO nanorod arrays.

Highly transparent and UV-resistant superhydrophobic arrays of SiO2-coated ZnO nanorods are prepared in a sequence of low-temperature (<150 °C) steps on both glass and thin sheets of PET (2 × 2 in.(2)), and the superhydrophobic nanocomposite is shown to have minimal impact on solar cell device performance under AM1.5G illumination. Flexible plastics can serve as front cell and backing materials in the manufacture of flexible displays and solar cells.

Linear side chains in benzo[1,2-b:4,5-b']dithiophene-thieno[3,4-c]pyrrole-4,6-dione polymers direct self-assembly and solar cell performance.

While varying the size and branching of solubilizing side chains in π-conjugated polymers impacts their self-assembling properties in thin-film devices, these structural changes remain difficult to anticipate. This report emphasizes the determining role that linear side-chain substituents play in poly(benzo[1,2-b:4,5-b']dithiophene-thieno[3,4-c]pyrrole-4,6-dione) (PBDTTPD) polymers for bulk heterojunction (BHJ) solar cell applications. We show that replacing branched side chains by linear ones in the BDT motifs induces a critical change in polymer self-assembly and backbone orientation in thin films that correlates with a dramatic drop in solar cell efficiency. In contrast, we show that for polymers with branched alkyl-substituted BDT motifs, controlling the number of aliphatic carbons in the linear N-alkyl-substituted TPD motifs is a major contributor to improved material performance. With this approach, PBDTTPD polymers were found to reach power conversion efficiencies of 8.5% and open-circuit voltages of 0.97 V in BHJ devices with PC71BM, making PBDTTPD one of the best polymer donors for use in the high-band-gap cell of tandem solar cells.