http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

The first tunable nano-bending structures of [1]rotaxane containing a single-fluorophoric N,N′-diphenyl-dihydrodibenzo[a,c]phenazine (DPAC) moiety are developed as a loosened lasso structure to feature the bright white-light emission [CIE (0.27, 0.33), Φ = 21.2%] in THF solution, where bi-stable states of bending and twisted structures of DPAC unit in [1]rotaxane with cyan and orange emissions at 480 and 600 nm, respectively.

The first tunable nano-bending structures of [1]rotaxane containing a single-fluorophoric N,N′-diphenyl-dihydrodibenzo[a,c]phenazine (DPAC) moiety (i.e., [1]RA) are developed as a loosened lasso structure to feature the bright white-light emission [CIE (0.27, 0.33), Φ = 21.2%] in THF solution, where bi-stable states of bending and twisted structures of DPAC unit in [1]RA produce cyan and orange emissions at 480 and 600 nm, respectively. With acid/base controls, tunable loosened/tightened nano-loops of corresponding [1]rotaxanes (i.e., [1]RA/[1]RB) can be achieved via the shuttling of macrocycles reversibly, and thus to adjust their respective white-light/cyan emissions, where the cyan emission of [1]RB is obtained due to the largest conformational constraint of DPAC moiety in its bending form of [1]RB with a tightened lasso structure. Additionally, the non-interlocked analog M-Boc only shows the orange emission, revealing the twisted form of DPAC fluorophore in M-Boc without any conformational constraint. Moreover, the utilization of solvents (with different viscosities and polarities), temperatures, and water fractions could serve as effective tools to adjust the bi-stable vibration-induced emission (VIE) colors of [1]rotaxanes. Finally, tuning ratiometric emission colors of adaptive conformations of DPAC moieties by altering nano-bending structures in [1]rotaxanes and external stimuli can be further developed as intelligent temperature and viscosity sensor materials.

Rechargeable Zinc–iodine batteries (ZIBs) are gaining attention as energy storage devices due to their high energy density, low-cost, and inherent safety. However, poor cycling performance of these batteries always arise from the severe leakage and shuttle effect of polyiodides (I3 – and I5 –). Herein, a novel cationic pyridine-rich covalent triazine framework (CCTF-TPMB) is developed to capture and confine iodine (I2) species via strong electrostatic interaction, making it an attractive host for I2 in ZIBs. The as-fabricated ZIBs with I2 loaded CCTF-TPMB (I2@CCTF-TPMB) cathode achieve a large specific capacity of 243 mAh g–1 at 0.2 A g–1 and an exceptionally stable cyclic performance, retaining 93.9% of its capacity over 30, 000 cycles at 5 A g–1. The excellent electrochemical performance of the ZIBs can be attributed to the pyridine-rich cationic sites of CCTF-TPMB, which effectively suppress the leakage and shuttle of polyiodides, while also accelerating conversion reaction of I2 species. Combined in situ Raman and Ultraviolet-Visible analysis, along with theoretical calculations, clearly reveal the critical role played by pyridine-rich cationic sites in boosting the ZIBs performances. This work opens up a promising pathway for designing advanced I2 cathode materials toward next-generation ZIBs and beyond.

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Nonporous adaptive crystals (NACs) are crystalline nonporous materials that can undergo a structural adaptive phase transformation to accommodate specific guest via porous cavity or lattice voids. Most of the NACs are based on pillararenes because of their flexible backbone and intrinsic porous structure. Here we report a readily prepared organic hydrochloride of 4-(4-(diphenylamino)phenyl)pyridin-1-ium chloride (TPAPyH), exhibiting the solvent dimension-dependent adaptive crystallinity. Wherein it forms a nonporous α crystal in a solvent with larger dimensions, while forming two porous β and γ crystals capable of accommodating solvent molecules in solvent with small size. Furthermore, the thermal-induced single-crystal-to-single-crystal (SCSC) transition from the β to α phase can be initiated. Upon exposure to iodine vapor or immersion in aqueous solution, the nonporous α phase transforms to porous β phase by adsorbing iodine molecules. Owing to the formation of trihalide anion I2Clˉ within the crystal cavity, TPAPyH exhibits remarkable performance in iodine storage, with a high uptaking capacity of 1.27 g·g−1 and elevated iodine desorption temperature of up to 110 and 82 °C following the first and second adsorption stage. The unexpected adaptivity of TPAPyH inspired the design of NACs for selective adsorption and separation of volatile compound from organic small molecules.

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Introducing asymmetric elements and breaking the geometric symmetry of traditional metal-N4 site for boosting oxygen reduction reaction (ORR) are meaningful and challenging. Herein, the planar chlorination engineering of Fe-N4 site was firstly proposed for remarkably improving the ORR activity. The Fe-N4/CNCl catalyst with broken symmetry exhibited a half-wave potential (E1/2) of 0.917 V versus RHE, 49 mV and 72 mV higher than those of traditional Fe-N4/CN and commercial 20 wt% Pt/C catalysts. The Fe-N4/CNCl catalyst also had excellent stability for 25,000 cycles and good methanol tolerance ability. For Zn-air battery test, the Fe-N4/CNCl catalyst had the maximum power density of 228 mW/cm2 and outstanding stability during 150 h charge-discharge test, as the promising substitute of Pt-based catalysts in energy storage and conversion devices. The density functional theory calculation demonstrated the adjacent C-Cl bond effectively broke the symmetry of Fe-N4 site, downward shifted the d-band center of Fe, facilitated the reduction and release of OH*, and remarkably lower the energy barrier of rate-determining step. This work revealed the enormous potentials of planar chlorination engineering for boosting the ORR activity of traditional metal-N4 site by thoroughly breaking their geometric symmetry.

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solid-state electrolytes, 3D supporting skeleton, mechanical strength, uniform Li deposition, F-enriched SEIAll-solid-state lithium metal batteries (ASSLMBs) are considered as the most promising candidates for the next-generation high-safety batteries. To achieve high energy density in ASSLMBs, it is essential that the solid-state electrolytes (SSEs) are lightweight, thin, and possess superior electrochemical stability. In this study, we propose a feasible and scalable fabrication approach to construct 3D supporting skeleton using an electro-blown spinning technique. This skeleton not only enhances the mechanical strength, but also hinders the migration of Li-salt anions, improving the lithium-ion transference number of the SSE. This provides a homogeneous distribution of Li-ion flux and local current density, promoting uniform Li deposition. As a result, based on the mechanically robust and thin SSEs, the Li symmetric cells show outstanding Li plating/stripping reversibility. Besides, a stable interface contact between SSE and Li anode has been established with the formation of a F-enriched solid electrolyte interface (SEI) layer. The solid-state Li|sulfurized polyacrylonitrile (Li|SPAN) cell achieves a capacity retention ratio of 94.0% after 350 cycles at 0.5 C. Also, the high-voltage Li|LCO cell shows a capacity retention of 92.4% at 0.5 C after 500 cycles. This fabrication approach for SSEs is applicable for commercially large-scale production and application in high-energy-density and high-safety ASSLMBs.

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Continuous monitoring of clinically relevant biomarkers within the interstitial fluid (ISF) using microneedle (MN)-based assays, has the potential to transform healthcare. This study introduces the Wearable Aptalyzer, an integrated system fabricated by combining biocompatible hydrogel microneedle (HMN) arrays for ISF extraction with an electrochemical aptamer-based biosensor for in situ monitoring of blood analytes. The use of aptamers enables continuous monitoring of a wide range of analytes, beyond what is possible with enzymatic monitoring. The Wearable Aptalyzer is used for real-time and multiplexed monitoring of glucose and lactate in ISF. Validation experiments using live mice and rat models of Type 1 Diabetes demonstrate strong correlation between the measurements collected from the Wearable Aptalyzer in ISF and those obtained from gold-standard techniques for blood glucose and lactate, for each analyte alone and in combination. The Wearable Aptalyzer effectively addresses the limitations inherent in enzymatic detection methods as well as solid MN biosensors and addresses the need for reliable and multiplexed bioanalytical monitoring in vivo.

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Deterministic integration of phase-pure Ruddlesden-Popper (RP) perovskites has great significance for realizing functional optoelectronic devices. However, precise fabrications of artificial perovskite heterostructures with pristine interfaces and rational design over electronic structure configurations remain a challenge. Here, the controllable synthesis of large-area ultrathin single-crystalline RP perovskite nanosheets and the deterministic fabrication of arbitrary 2D vertical perovskite heterostructures are reported. The 2D heterostructures exhibit intriguing dual-peak emission phenomenon and dual-band photoresponse characteristic. Importantly, the interlayer energy transfer behaviors from wide-bandgap component (WBC) to narrow-bandgap component (NBC) modulated by comprising quantum wells are thoroughly revealed. Functional nanoscale photodetectors are further constructed based on the 2D heterostructures. Moreover, by combining the modulated dual-band photoresponse characteristic with double-beam irradiation modes, and introducing an encryption algorithm mechanism, a light communication system with high security and reliability is achieved. This work can greatly promote the developments of heterogeneous integration technologies of 2D perovskites, and could provide a competitive candidate for advanced integrated optoelectronics.

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Conductive metal-organic frameworks (c-MOFs) and ionic liquids (ILs) have emerged as auspicious combinations for high-performance supercapacitors. However, the nanoconfinement from c-MOFs and high viscosity of ILs slow down the charging process. This hindrance can, however, be resolved by adding solvent. Here, we performed constant-potential molecular simulations to scrutinize the solvent impact on charge storage and charging dynamics of MOF-IL-based supercapacitors. We find conditions for >100% enhancement in capacity and ∼6 times increase in charging speed. These improvements were confirmed by synthesizing near-ideal c-MOFs and developing multiscale models linking molecular simulations to electrochemical measurements. Fundamentally, our findings elucidate that the solvent acts as an “ionophobic agent” to induce a substantial enhancement in charge storage, and as an “ion traffic police” to eliminate convoluted counterion and co-ion motion paths and create two distinct ion transport highways to accelerate charging dynamics. This work paves the way for the optimal design of MOF supercapacitors.

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An organic solid-state laser under continuous-wave (CW) excitation is one of the most challenging areas in organic optoelectronics. Recent advances in long-pulsed organic lasers are comprehensively summarized with respect to molecular designs, optical-resonator architectures, triplet scavenging, and potential triplet-contribution strategies. Future directions and perspectives for CW operation are discussed.

A continuous-wave (CW) organic solid-state laser is highly desirable for spectroscopy, sensing, and communications, but is a significant challenge in optoelectronics. The accumulation of long-lived triplet excitons and relevant excited-state absorptions, as well as singlet–triplet annihilation, are the main obstacles to CW lasing. Here, progress in singlet- and triplet-state utilizations in organic gain media is reviewed to reveal the issues in working with triplets. Then, exciton behaviors that inhibit light oscillations during long excitation pulses are discussed. Further, recent advances in increasing organic lasing pulse widths from microseconds toward the indication of CW operation are summarized with respect to molecular designs, advanced resonator architectures, triplet scavenging, and potential triplet contribution strategies. Finally, future directions and perspectives are proposed for achieving stable CW organic lasers with significant triplet contribution.

The integration of thin-film photovoltaics with structural components represents an attractive prospect for mobile power applications. In this work, the first example of perovskite solar cells deposited directly onto rigid carbon-fiber-reinforced polymer composite substrates is demonstrated, heralding a new class of photocurrent-generating materials with both high specific strength and power.

Integrating photovoltaic devices onto the surface of carbon-fiber-reinforced polymer substrates should create materials with high mechanical strength that are also able to generate electrical power. Such devices are anticipated to find ready applications as structural, energy-harvesting systems in both the automotive and aeronautical sectors. Here, the fabrication of triple-cation perovskite n–i–p solar cells onto the surface of planarized carbon-fiber-reinforced polymer substrates is demonstrated, with devices utilizing a transparent top ITO contact. These devices also contain a “wrinkled” SiO2 interlayer placed between the device and substrate that alleviates thermally induced cracking of the bottom ITO layer. Devices are found to have a maximum stabilized power conversion efficiency of 14.5% and a specific power (power per weight) of 21.4 W g−1 (without encapsulation), making them highly suitable for mobile power applications.

A small modification of side-chain density in thiophene-based conjugated polymers affects the polaron formation via electrochemical doping. In situ monitoring of polaron formation allows identification of its dependence on molecular structures. Understanding of the polaron formation mechanism is important for molecular design rules and its impact on electrical properties.

Polarons exist when charges are injected into organic semiconductors due to their strong coupling with the lattice phonons, significantly affecting electronic charge-transport properties. Understanding the formation and (de)localization of polarons is therefore critical for further developing organic semiconductors as a future electronics platform. However, there are very few studies reported in this area. In particular, there is no direct in situ monitoring of polaron formation and identification of its dependence on molecular structure and impact on electrical properties, limiting further advancement in organic electronics. Herein, how a minor modification of side-chain density in thiophene-based conjugated polymers affects the polaron formation via electrochemical doping, changing the polymers’ electrical response to the surrounding dielectric environment for gas sensing, is demonstrated. It is found that the reduction in side-chain density results in a multistep polaron formation, leading to an initial formation of localized polarons in thiophene units without side chains. Reduced side-chain density also allows the formation of a high density of polarons with fewer polymer structural changes. More numerous but more localized polarons generate a stronger analyte response but without the selectivity between polar and non-polar solvents, which is different from the more delocalized polarons that show clear selectivity. The results provide important molecular understanding and design rules for the polaron formation and its impact on electrical properties.

High-brightness organic LED arrays are produced by direct vacuum deposition of the organic materials onto complementary metal–oxide–semiconductor (CMOS) backplanes produced in a commercial chip foundry. The composition of the foundry-provided aluminum anodes is analyzed by scanning transmission electron microscopy and their surface is pre-conditioned for optimal electrical contact by plasma treatment.

Direct deposition of organic light-emitting diodes (OLEDs) on silicon-based complementary metal–oxide–semiconductor (CMOS) chips has enabled self-emissive microdisplays with high resolution and fill-factor. Emerging applications of OLEDs in augmented and virtual reality (AR/VR) displays and in biomedical applications, e.g., as brain implants for cell-specific light delivery in optogenetics, require light intensities orders of magnitude above those found in traditional displays. Further requirements often include a microscopic device footprint, a specific shape and ultrastable passivation, e.g., to ensure biocompatibility and minimal invasiveness of OLED-based implants. In this work, up to 1024 ultrabright, microscopic OLEDs are deposited directly on needle-shaped CMOS chips. Transmission electron microscopy and energy-dispersive X-ray spectroscopy are performed on the foundry-provided aluminum contact pads of the CMOS chips to guide a systematic optimization of the contacts. Plasma treatment and implementation of silver interlayers lead to ohmic contact conditions and thus facilitate direct vacuum deposition of orange- and blue-emitting OLED stacks leading to micrometer-sized pixels on the chips. The electronics in each needle allow each pixel to switch individually. The OLED pixels generate a mean optical power density of 0.25 mW mm−2, corresponding to >40 000 cd m−2, well above the requirement for daylight AR applications and optogenetic single-unit activation in the brain.

Efficient and bright deep-red perovskite light-emitting diodes (LEDs) are achieved based on a lateral Cs4PbI6/FA x Cs1− x PbI3 (0D/3D) heterostructure, which can simultaneously reduce nonradiative recombination and enhance light extraction. This leads to deep-red perovskite LEDs with a record external quantum efficiency of 21% at a high current density of ≈200 mA cm−2.

Bright and efficient deep-red light-emitting diodes (LEDs) are important for applications in medical therapy and biological imaging due to the high penetration of deep-red photons into human tissues. Metal-halide perovskites have potential to achieve bright and efficient electroluminescence due to their favorable optoelectronic properties. However, efficient and bright perovskite-based deep-red LEDs have not been achieved yet, due to either Auger recombination in low-dimensional perovskites or trap-assisted nonradiative recombination in 3D perovskites. Here, a lateral Cs4PbI6/FA x Cs1− x PbI3 (0D/3D) heterostructure that can enable efficient deep-red perovskite LEDs at very high brightness is demonstrated. The Cs4PbI6 can facilitate the growth of low-defect FA x Cs1− x PbI3, and act as low-refractive-index grids, which can simultaneously reduce nonradiative recombination and enhance light extraction. This device reaches a peak external quantum efficiency of 21.0% at a photon flux of 1.75 × 1021 m−2 s−1, which is almost two orders of magnitude higher than that of reported high-efficiency deep-red perovskite LEDs. Theses LEDs are suitable for pulse oximeters, showing an error <2% of blood oxygen saturation compared with commercial oximeters.

Time-resolved microwave conductivity shows that the rate of photocatalytic hydrogen evolution by aqueous-soluble organic donor–acceptor nanoparticles is limited by charge concentration, and that nanoparticles have 3× more long-lived accumulated charges relative to bulk samples of the same material composition.

Time-resolved microwave conductivity is used to compare aqueous-soluble organic nanoparticle photocatalysts and bulk thin films composed of the same mixture of semiconducting polymer and non-fullerene acceptor molecule and the relationship between composition, interfacial surface area, charge-carrier dynamics, and photocatalytic activity is examined. The rate of hydrogen evolution reaction by nanoparticles composed of various donor:acceptor blend ratio compositions is quantitatively measured, and it is found that the most active blend ratio displays a hydrogen quantum yield of 0.83% per photon. Moreover, it is found that nanoparticle photocatalytic activity corresponds directly to charge generation, and that nanoparticles have 3× more long-lived accumulated charges relative to bulk samples of the same material composition. These results suggest that, under the current reaction conditions, with ≈3× solar flux, catalytic activity by the nanoparticles is limited by the concentration of electrons and holes in operando and not a finite number of active surface sites or the catalytic rate at the interface. This provides a clear design goal for the next generation of efficient photocatalytic nanoparticles.

The relationship between crystal packing motifs and optical properties of pure organic room temperature phosphorescent (ORTP) cocrystals with halogen bonding is investigated by comparing three different binary cocrystals. By designing ternary cocrystals based on the analysis, a highly efficient ORTP cocrystal with a PLQY of over 20% is achieved. To obtain insight into energy loss, the phosphorescent mechanism is discussed.

Recently, there has been intense interest in pure organic room-temperature phosphorescence (ORTP) from cocrystals composed of 1,4-diiodotetrafluorobenzene (DITFB) and a variety of polycyclic aromatic hydrocarbons (PAHs) or their derivatives. To expand the possibility of halogen bonding-based cocrystals, the relationship between the crystal packing motifs and ORTP characteristics in binary cocrystals composed of DITFB and PAHs of phenanthrene (Phen), chrysene (Chry), and pyrene (Pyr), respectively, is investigated. The σ-hole···π and π-hole···π interactions determine not only the crystal packing motifs but also photoluminescence quantum yields (PLQYs). The Phen-DITFB and Chry-DITFB binary cocrystals with σ-hole···π interactions show higher PLQY compared with the Pyr-DITFB binary cocrystal with π-hole···π interaction. Further, to clarify the effect of crystal structures on PLQY, ternary cocrystals are prepared by partially doping Pyr into Phen-DITFB. The crystal packing motif of the ternary cocrystal originates from a Phen-DITFB cocrystal with σ-hole···π interaction, and some of the Phen sites are randomly replaced with Pyr molecules. The ORTP emission is derived from Pyr. The maximum PLQY is >20% due to suppressing nonradiative decay by changing the crystal packing motif.

Fully solution-processed microcavities are demonstrated that allow realizing strong light–matter coupling with an organic semiconductor, all enabled by a versatile molecular hybrid material that permits the fabrication of dielectric mirrors with high-refractive-index contrast between constituting layers.

Planar microcavities with strong light–matter coupling, monolithically processed fully from solution, consisting of two polymer-based distributed Bragg reflectors (DBRs) comprising alternating layers of a high-refractive-index titanium oxide hydrate/poly(vinyl alcohol) hybrid material and a low-refractive-index fluorinated polymer are presented. The DBRs enclose a perylene diimide derivative (b-PDI-1) film positioned at the antinode of the optical mode. Strong light–matter coupling is achieved in these structures at the target excitation of the b-PDI-1. Indeed, the energy-dispersion relation (energy vs in-plane wavevector or output angle) in reflectance and the group delay of transmitted light in the microcavities show a clear anti-crossing—an energy gap between two distinct exciton-polariton dispersion branches. The agreement between classical electrodynamic simulations of the microcavity response and the experimental data demonstrates that the entire microcavity stack can be controllably produced as designed. Promisingly, the refractive index of the inorganic/organic hybrid layers used in the microcavity DBRs can be precisely manipulated between values of 1.50 to 2.10. Hence, microcavities with a wide spectral range of optical modes might be designed and produced with straightforward coating methodologies, enabling fine-tuning of the energy and lifetime of the microcavities‘ optical modes to harness strong light–matter coupling in a wide variety of solution processable active materials.

RAINBOW solar cells consist of two or more junctions placed next to each other and illuminated by spectrally spread sunlight. Guidelines for materials selection are given for this novel geometry through device simulations. Moreover, experimental efficiencies greater than 46% with respect to the best sub-cell are demonstrated for a monolithic two-junction device based on organic semiconducting absorbers.

While multi-junction geometries have the potential to boost the efficiency of organic solar cells, the experimental gains yet obtained are still very modest. This work proposes an alternative spectral splitting device concept in which various individual semiconducting junctions with cascading bandgaps are laid side by side, thus the name RAINBOW. Each lateral sub-cell receives a fraction of the spectrum that closely matches the main absorption band of the given semiconductor. Here, simulations are used to identify the important material and device properties of each RAINBOW sub-cell. Using the resulting design rules, three systems are selected, with narrow, medium, and wide effective bandgaps, and their potential as sub-cells in this geometry is experimentally investigated. With the aid of a custom-built setup that generates spectrally spread sunlight on demand, the simulations are experimentally validated, showing that this geometry can lead to a reduction in thermalization losses and an improvement in light harvesting, which results in a relative improvement in efficiency of 46.6% with respect to the best sub-cell. Finally, a working proof-of-concept monolithic device consisting of two sub-cells deposited from solution on the same substrate is fabricated, thus demonstrating the feasibility and the potential of the RAINBOW solar cell concept.

2D polymer heterojunctions are formed using a novel templating technique and are investigated as photocatalysts for proton reduction. Templated materials showed improved charge separation and reduced trapped charges at the donor–acceptor interface, which results in hydrogen evolution rates of 3–9 times that of either individual semiconductor and the ability to produce hydrogen in combination with the oxidation of reversible redox mediators, as well as sacrificial electron donors.

2D polymers have emerged as one of the most promising classes of organic photocatalysts for solar fuel production due to their tunability, charge-transport properties, and robustness. They are however difficult to process and so there are limited studies into the formation of heterojunction materials incorporating these components. In this work, a novel templating approach is used to combine an imine-based donor polymer and an acceptor polymer formed through Knoevenagel condensation. Heterojunction formation is shown to be highly dependent on the topological match of the donor and acceptor polymers with the most active templated material found to be between three and nine times more active for photocatalysis than its constituent components. Transient absorption spectroscopy reveals that this improvement is due to faster charge separation and more efficient charge extraction in the templated heterojunction. The templated material shows a very high hydrogen evolution rate of >20 mmol h−1 m−2 with an ascorbic acid hole scavenger but also produces hydrogen in the presence of only water and a cobalt-based redox mediator. This suggests the improved charge-separation interface and reduced trapping accessed through this approach could be suitable for Z-scheme formation.

12-nm layers of silver deposited on the commercial optical adhesive NOA63 serve as ultrasmooth, haze-free transparent electrodes for optoelectronics that exhibit high resilience to bending. The electrodes may be readily patterned by selectively etching the NOA63 substrate with an oxygen plasma prior to metal deposition, with the silver forming continuous, conducting regions above unetched NOA63 and fragmented, highly insulating regions above etched NOA63.

Template-patterned, flexible transparent electrodes (TEs) formed from an ultrathin silver film on top of a commercial optical adhesive – Norland Optical Adhesive 63 (NOA63) – are reported. NOA63 is shown to be an effective base-layer for ultrathin silver films that advantageously prevents coalescence of vapor-deposited silver atoms into large, isolated islands (Volmer-Weber growth), and so aids the formation of ultrasmooth continuous films. 12 nm silver films on top of free-standing NOA63 combine high, haze-free visible-light transparency (T ≈ 60% at 550 nm) with low sheet-resistance (Rs${\mathcal{R}}_s$ ≈ 16 Ω sq−1), and exhibit excellent resilience to bending, making them attractive candidates for flexible TEs. Etching the NOA63 base-layer with an oxygen plasma before silver deposition causes the silver to laterally segregate into isolated pillars, resulting in a much higher sheet resistance (Rs${\mathcal{R}}_{s}$ > 8 × 106 Ω sq-1) than silver grown on pristine NOA63 . Hence, by selectively etching NOA63 before metal deposition, insulating regions may be defined within an otherwise conducting silver film, resulting in a differentially conductive film that can serve as a patterned TE for flexible devices. Transmittance may be increased (to 79% at 550 nm) by depositing an antireflective layer of Al2O3 on the Ag layer at the cost of reduced flexibility.

A machine-learning-driven high-throughput workflow for solution-processed organic solar cells is presented, identifying causal relationships between process conditions and active layer morphology, and between morphology and stability. Using only inexpensive and fast optical probes, quantitative structure–property relationships are obtained that improve the understanding and control of electrical performance degradation.

Organic solar cells (OSCs) now approach power conversion efficiencies of 20%. However, in order to enter mass markets, problems in upscaling and operational lifetime have to be solved, both concerning the connection between processing conditions and active layer morphology. Morphological studies supporting the development of structure–process–property relations are time-consuming, complex, and expensive to undergo and for which statistics, needed to assess significance, are difficult to be collected. This work demonstrates that causal relationships between processing conditions, morphology, and stability can be obtained in a high-throughput method by combining low-cost automated experiments with data-driven analysis methods. An automatic spectral modeling feeds parametrized absorption data into a feature selection technique that is combined with Gaussian process regression to quantify deterministic relationships linking morphological features and processing conditions with device functionality. The effect of the active layer thickness and the morphological order is further modeled by drift–diffusion simulations and returns valuable insight into the underlying mechanisms for improving device stability by tuning the microstructure morphology with versatile approaches. Predicting microstructural features as a function of processing parameters is decisive know-how for the large-scale production of OSCs.