Single-junction organic solar cells with over 19% efficiency enabled by a refined double-fibril network morphology.

In organic photovoltaics, morphological control of donor and acceptor domains on the nanoscale is the key for enabling efficient exciton diffusion and dissociation, carrier transport and suppression of recombination losses. To realize this, here, we demonstrated a double-fibril network based on a ternary donor-acceptor morphology with multi-length scales constructed by combining ancillary conjugated polymer crystallizers and a non-fullerene acceptor filament assembly. Using this approach, we achieved an average power conversion efficiency of 19.3% (certified 19.2%). The success lies in the good match between the photoelectric parameters and the morphological characteristic lengths, which utilizes the excitons and free charges efficiently. This strategy leads to an enhanced exciton diffusion length and a reduced recombination rate, hence minimizing photon-to-electron losses in the ternary devices as compared to their binary counterparts. The double-fibril network morphology strategy minimizes losses and maximizes the power output, offering the possibility of 20% power conversion efficiencies in single-junction organic photovoltaics.

Intensity-based iterative reconstruction for helical grating interferometry breast CT with static grating configuration.

Grating interferometry breast computed tomography (GI-BCT) has the potential to provide enhanced soft tissue contrast and to improve visualization of cancerous lesions for breast imaging. However, with a conventional scanning protocol, a GI-BCT scan requires longer scanning time and higher operation complexity compared to conventional attenuation-based CT. This is mainly due to multiple grating movements at every projection angle, so-called phase stepping, which is used to retrieve attenuation, phase, and scattering (dark-field) signals. To reduce the measurement time and complexity and extend the field of view, we have adopted a helical GI-CT setup and present here the corresponding tomographic reconstruction algorithm. This method allows simultaneous reconstruction of attenuation, phase contrast, and scattering images while avoiding grating movements. Experiments on simulated phantom and real initial intensity, visibility and phase maps are provided to validate our method.

Surface enhanced Raman scattering active substrate based on hydrogel microspheres for pretreatment-free detection of glucose in biological samples.

Determining glucose in biological samples is tedious and time-consuming due to sample pretreatment. The sample is usually pretreated to remove lipids, proteins, hemocytes and other sugars that interfere with glucose detection. A surface-enhanced Raman scattering (SERS) active substrate based on hydrogel microspheres has been developed to detect glucose in biological samples. Due to the specific catalytic action of glucose oxidase (GOX), the high selectivity of detection is guaranteed. The hydrogel substrate prepared by microfluidic droplets technology protects the silver nanoparticles from the surrounding environment and improves the stability and reproducibility of the assay. In addition, the hydrogel microspheres have size-adjustable pores that selectively allow small molecules to pass through. The pores block the entry of large molecules, such as impurities, enabling glucose detection through glucose oxidase etching without sample pretreatment. This hydrogel microsphere-SERS platform is highly sensitive and enables reproducible detection of different glucose concentrations in biological samples. The use of SERS to detect glucose provides clinicians with new diagnostic methods for diabetes and a new application opportunity for SERS-based molecular detection techniques.

High-temperature low-humidity proton exchange membrane with "stream-reservoir" ionic channels for high-power-density fuel cells.

The perfluorosulfonic acid (PFSA) proton exchange membrane (PEM) is the key component for hydrogen fuel cells (FCs). We used in situ synchrotron scattering to investigate the PEM morphology evolution and found a "stream-reservoir" morphology, which enables efficient proton transport. The short-side-chain (SSC) PFSA PEM is fabricated under the guidance of morphology optimization, which delivered a proton conductivity of 193 milliSiemens per centimeter [95% relativity humidity (RH)] and 40 milliSiemens per centimeter (40% RH) at 80°C. The improved glass transition temperature, water permeability, and mechanical strength enable high-temperature low-humidity FC applications. Performance improvement by 82.3% at 110°C and 25% RH is obtained for SSC-PFSA PEM FCs compared to Nafion polymer PEM devices. The insights in chain conformation, packing mechanism, crystallization, and phase separation of PFSAs build up the structure-property relationship. In addition, SSC-PFSA PEM is ideal for high-temperature low-humidity FCs that are needed urgently for high-power-density and heavy-duty applications.

Iterative phase contrast CT reconstruction with novel tomographic operator and data-driven prior.

Breast cancer remains the most prevalent malignancy in women in many countries around the world, thus calling for better imaging technologies to improve screening and diagnosis. Grating interferometry (GI)-based phase contrast X-ray CT is a promising technique which could make the transition to clinical practice and improve breast cancer diagnosis by combining the high three-dimensional resolution of conventional CT with higher soft-tissue contrast. Unfortunately though, obtaining high-quality images is challenging. Grating fabrication defects and photon starvation lead to high noise amplitudes in the measured data. Moreover, the highly ill-conditioned differential nature of the GI-CT forward operator renders the inversion from corrupted data even more cumbersome. In this paper, we propose a novel regularized iterative reconstruction algorithm with an improved tomographic operator and a powerful data-driven regularizer to tackle this challenging inverse problem. Our algorithm combines the L-BFGS optimization scheme with a data-driven prior parameterized by a deep neural network. Importantly, we propose a novel regularization strategy to ensure that the trained network is non-expansive, which is critical for the convergence and stability analysis we provide. We empirically show that the proposed method achieves high quality images, both on simulated data as well as on real measurements.

Correlating Electronic Structure and Device Physics with Mixing Region Morphology in High-Efficiency Organic Solar Cells.

The donor/acceptor interaction in non-fullerene organic photovoltaics leads to the mixing domain that dictates the morphology and electronic structure of the blended thin film. Initiative effort is paid to understand how these domain properties affect the device performances on high-efficiency PM6:Y6 blends. Different fullerenes acceptors are used to manipulate the feature of mixing domain. It is seen that a tight packing in the mixing region is critical, which could effectively enhance the hole transfer and lead to the enlarged and narrow electron density of state (DOS). As a result, short-circuit current (JSC ) and fill factor (FF) are improved. The distribution of DOS and energy levels strongly influences open-circuit voltage (VOC ). The raised filling state of electron Fermi level is seen to be key in determining device VOC . Energy disorder is found to be a key factor to energy loss, which is highly correlated with the intermolecular distance in the mixing region. A 17.53% efficiency is obtained for optimized ternary devices, which is the highest value for similar systems. The current results indicate that a delicate optimization of the mixing domain property is an effective route to improve the VOC , JSC , and FF simultaneously, which provides new guidelines for morphology control toward high-performance organic solar cells.

The Molecular Ordering and Double-Channel Carrier Generation of Nonfullerene Photovoltaics within Multi-Length-Scale Morphology.

The success of nonfullerene acceptor (NFA) solar cells lies in their unique physical properties beyond the extended absorption and suitable energy levels. The current study investigates the morphology and photophysical behavior of PBDB-T donor blending with ITIC, 4TIC, and 6TIC acceptors. Single-crystal study shows that the π-π stacking and side-chain interaction dictate molecular assembly, which can be carried to blended films, forming a multi-length-scale morphology. Spontaneous carrier generation is seen in ITIC, 4TIC, and 6TIC neat films and their blended thin films using the PBDB-T donor, providing a new avenue of zero-energy-loss carrier formation. The molecular packing associated with specific contacts and geometry is key in influencing the photophysics, as demonstrated by the charge transfer and carrier lifetime results. The 2D layer of 6TIC facilitates the exciton-to-polaron conversion, and the largest photogenerated polaron yield is obtained. The new mechanism, together with the highly efficient blending region carrier generation, has the prospect of the fundamental advantage for NFA solar cells, from molecular assembly to thin-film morphology.

Design Rules of the Mixing Phase and Impacts on Device Performance in High-Efficiency Organic Photovoltaics.

In nonfullerene acceptor- (NFA-) based solar cells, the exciton splitting takes place at both domain interface and donor/acceptor mixture, which brings in the state of mixing phase into focus. The energetics and morphology are key parameters dictating the charge generation, diffusion, and recombination. It is revealed that tailoringthe electronic properties of the mixing region by doping with larger-bandgap components could reduce the density of state but elevate the filling state level, leading to improved open-circuit voltage (V OC) and reduced recombination. The monomolecular and bimolecular recombinations are shown to be intercorrelated, which show a Gaussian-like relationship with V OC and linear relationship with short-circuit current density (J SC) and fill factor (FF). The kinetics of hole transfer and exciton diffusion scale with J SC similarly, indicating the carrier generation in mixing region and crystalline domain are equally important. From the morphology perspective, the crystalline order could contribute to V OC improvement, and the fibrillar structure strongly affects the FF. These observations highlight the importance of the mixing region and its connection with crystalline domains and point out the design rules to optimize the mixing phase structure, which is an effective approach to further improve device performance.

Capture the high-efficiency non-fullerene ternary organic solar cells formula by machine-learning-assisted energy-level alignment optimization.

Appropriate energy-level alignment in non-fullerene ternary organic solar cells (OSCs) can enhance the power conversion efficiencies (PCEs), due to the simultaneous improvement in charge generation/transportation and reduction in voltage loss. Seven machine-learning (ML) algorithms were used to build the regression and classification models based on energy-level parameters to predict PCE and capture high-performance material combinations, and random forest showed the best predictive capability. Furthermore, two sets of verification experiments were designed to compare the experimental and predicted results. The outcome elucidated that a deep lowest unoccupied molecular orbital (LUMO) of the non-fullerene acceptors can slightly reduce the open-circuit voltage (V OC) but significantly improve short-circuit current density (J SC), and, to a certain extent, the V OC could be optimized by the slightly up-shifted LUMO of the third component in non-fullerene ternary OSCs. Consequently, random forest can provide an effective global optimization scheme and capture multi-component combinations for high-efficiency ternary OSCs.

Reactivity Improvement of Ca-Based CO2 Absorbent Modified with Sodium Humate in Cyclic Calcination/Carbonation.

The Ca-based sorbent cyclic calcination/carbonation reaction (CCCR) is a high-efficiency technique for capturing CO2 from combustion processes. The CO2 capture ability of CaO modified with sodium humate (HA-Na) (HA-Na/CaO) in long-term calcination/carbonation cycles was investigated. The enhancement mechanism of HA-Na on CCCR was proposed and demonstrated. The effects of carbonation temperature, reaction duration, and the addition amount of HA-Na on the carbonation rate of the CaO adsorbent were also studied. HA-Na/CaO is allowed to react 20 min at the optimum conditions for calcination (920 °C, 100% N2) and for carbonation (700 °C, 15% CO2, 85% N2), respectively. HA-Na plays a key role in the CCCR process, and the carbonation conversion rate is lifted obviously. The maximum conversion rate of HA-Na/CaO is 23% higher than that of CaO in the first cycle. After 20 cycles, the conversion rate of HA-Na/CaO is still 0.28, while that of CaO is only 0.15. The carbonation conversion rate for HA-Na/CaO is improved by 86% compared to CaO. In addition, the characteristics of calcined sorbents are analyzed by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Brunauer-Emmett-Teller (BET) methods.

A perylene diimide-containing acceptor enables high fill factor in organic solar cells.

A new non-fullerene acceptor PDFC is prepared by introducing perylene diimide into the core of an A-DA'D-A architecture. Due to the large conjugation and electron-deficient ability of perylene diimide, PDFC shows strong absorption, suitable energy levels and favorable face-on packing. The optimal device realizes a PCE of 12.56% with one of the highest fill factors (81.3%). A PCE of 9.66% is obtained in a 570 nm thick-film device based on PDFC.

Optimized active layer morphology toward efficient and polymer batch insensitive organic solar cells.

Morphology control in laboratory and industry setting remains as a major challenge for organic solar cells (OSCs) due to the difference in film-drying kinetics between spin coating and the printing process. A two-step sequential deposition method is developed to control the active layer morphology. A conjugated polymer that self-assembles into a well-defined fibril structure is used as the first layer, and then a non-fullerene acceptor is introduced into the fibril mesh as the second layer to form an optimal morphology. A benefit of the combined fibril network morphology and non-fullerene acceptor properties was that a high efficiency of 16.5% (certified as 16.1%) was achieved. The preformed fibril network layer and the sequentially deposited non-fullerene acceptor form a robust morphology that is insensitive to the polymer batches, solving a notorious issue in OSCs. Such progress demonstrates that the utilization of polymer fibril networks in a sequential deposition process is a promising approach towards the fabrication of high-efficiency OSCs.

An Optimized Fibril Network Morphology Enables High-Efficiency and Ambient-Stable Polymer Solar Cells.

Morphological stability is crucially important for the long-term stability of polymer solar cells (PSCs). Many high-efficiency PSCs suffer from metastable morphology, resulting in severe device degradation. Here, a series of copolymers is developed by manipulating the content of chlorinated benzodithiophene-4,8-dione (T1-Cl) via a random copolymerization approach. It is found that all the copolymers can self-assemble into a fibril nanostructure in films. By altering the T1-Cl content, the polymer crystallinity and fibril width can be effectively controlled. When blended with several nonfullerene acceptors, such as TTPTT-4F, O-INIC3, EH-INIC3, and Y6, the optimized fibril interpenetrating morphology can not only favor charge transport, but also inhibit the unfavorable molecular diffusion and aggregation in active layers, leading to excellent morphological stability. The work demonstrates the importance of optimization of fibril network morphology in realizing high-efficiency and ambient-stable PSCs, and also provides new insights into the effect of chemical structure on the fibril network morphology and photovoltaic performance of PSCs.

Universal and versatile morphology engineering via hot fluorous solvent soaking for organic bulk heterojunction.

After explosive growth of efficiency in organic solar cells (OSCs), achieving ideal morphology of bulk heterojunction remains crucial and challenging for advancing OSCs into consumer market. Herein, by utilizing the amphiphobic nature and temperature-dependent miscibility of fluorous solvent, hot fluorous solvent soaking method is developed to optimize the morphology with various donor/acceptor combinations including polymer/small-molecule, all-polymer and all-small-molecule systems. By immersing blend film into hot fluorous solvent which is utilized as liquid medium with better thermal conductivity, the molecular reorganization is accelerated. Furthermore, fluorous solvent can be miscible with the residue of chloroform and chloronaphthalene above upper critical solution temperature. This mixed solvent diffuses around inside the active layer and selectively promotes molecular reorganization, leading to optimized morphology. Compared to widely-used thermal annealing, this approach processed under mild conditions achieves superior photovoltaic performance, indicating the practicality and universality for morphological optimization in OSCs as well as other optoelectronic devices.

Unraveling the influence of non-fullerene acceptor molecular packing on photovoltaic performance of organic solar cells.

In non-fullerene organic solar cells, the long-range structure ordering induced by end-group π-π stacking of fused-ring non-fullerene acceptors is considered as the critical factor in realizing efficient charge transport and high power conversion efficiency. Here, we demonstrate that side-chain engineering of non-fullerene acceptors could drive the fused-ring backbone assembly from a π-π stacking mode to an intermixed packing mode, and to a non-stacking mode to refine its solid-state properties. Different from the above-mentioned understanding, we find that close atom contacts in a non-stacking mode can form efficient charge transport pathway through close side atom interactions. The intermixed solid-state packing motif in active layers could enable organic solar cells with superior efficiency and reduced non-radiative recombination loss compared with devices based on molecules with the classic end-group π-π stacking mode. Our observations open a new avenue in material design that endows better photovoltaic performance.

Effect of the Energy Offset on the Charge Dynamics in Nonfullerene Organic Solar Cells.

The energy offset, considered as the driving force for charge transfer between organic molecules, has significant effects on both charge separation and charge recombination in organic solar cells. Herein, we designed material systems with gradually shifting energy offsets, including both positive and negative values. Time-resolved spectroscopy was used to monitor the charge dynamics within the bulk heterojunction. It is striking to find that there is still charge transfer and charge generation when the energy offset reached -0.10 eV (ultraviolet photoelectron spectroscopy data). This work not only indicates the feasibility of the free carrier generation and the following charge separation under the condition of a negative offset but also elucidates the relationship between the charge transfer and the energy offset in the case of polymer chlorination.

Ternary Organic Solar Cells with Efficiency >16.5% Based on Two Compatible Nonfullerene Acceptors.

A ternary structure has been demonstrated as being an effective strategy to realize high power conversion efficiency (PCE) in organic solar cells (OSCs); however, general materials selection rules still remain incompletely understood. In this work, two nonfullerene small-molecule acceptors 3TP3T-4F and 3TP3T-IC are synthesized and incorporated as a third component in PM6:Y6 binary blends. The photovoltaic behaviors in the resultant ternary OSCs differ significantly, despite the comparable energy levels. It is found that incorporation of 15% 3TP3T-4F into the PM6:Y6 blend results in facilitating exciton dissociation, increasing charge transport, and reducing trap-assisted recombination. All these features are responsible for the enlarged PCE of 16.7% (certified as 16.2%) in the PM6:Y6:3TP3T-4F ternary OSCs, higher than that (15.6%) in the 3TP3T-IC containing ternary devices. The performance differences are mainly ascribed to the compatibility between the third component and the host materials. The 3TP3T-4F guest acceptor exhibits an excellent compatibility with Y6, tending to form well-mixed phases in the ternary blend without disrupting the favored bicontinuous transport networks, whereas 3TP3T-IC displays a morphological incompatibility with Y6. This work highlights the importance of considering the compatibility for materials selection toward high-efficiency ternary organic OSCs.

Aggregation-Induced Multilength Scaled Morphology Enabling 11.76% Efficiency in All-Polymer Solar Cells Using Printing Fabrication.

All-polymer solar cells (all-PSCs) exhibit excellent stability and readily tunable ink viscosity, and are therefore especially suitable for printing preparation of large-scale devices. At present, the efficiency of state-of-the-art all-PSCs fabricated by the spin-coating method has exceeded 11%, laying the foundation for the preparation and practical utilization of printed devices. A high power conversion efficiency (PCE) of 11.76% is achieved based on PTzBI-Si:N2200 all-PSCs processing with 2-methyltetrahydrofuran (MTHF, an environmentally friendly solvent) and preparation of active layers by slot die printing, which is the top efficient for all-PSCs. Conversely, the PCE of devices processed by high-boiling point chlorobenzene is less than 2%. Through the study of film formation kinetics, volatile solvents can freeze the morphology in a short time, and a more rigid conformation with strong intermolecular interaction combined with the solubility limit of PTzBI-Si and N2200 in MTHF results in the formation of a fibril network in the bulk heterojunction. The multilength scaled morphology ensures fast transfer of carriers and facilitates exciton separation, which boosts carrier mobility and current density, thus improving the device performance. These results are of great significance for large-scale printing fabrication of high-efficiency all-PSCs in the future.

Edge information diffusion based reconstruction (EIDR) for cone beam computed laminography.

Computed laminography (CL) is a prospective nondestructive testing technique for flat object inspection in industrial applications. However, CL image reconstruction is a challenging task because incomplete projection data are acquired from the CL scan. When a conventional computed tomography (CT) reconstruction method is applied to cone beam CL data, the vertical edges (singularities in the z-direction) in the reconstructed image would be blurred. On the contrary, the horizontal edges (singularities within slices) can be quite accurately reconstructed. Based on this key observation, an edge information diffusion method is developed, which fixes the horizontal edges and propagates their values within the slices. An effective CL reconstruction method is then proposed for flat object inspection by combining the edge information diffusion procedure, which plays the role of regularization, with conventional CT image reconstruction algorithms. Experiments on both simulated data and real data are performed to verify the effectiveness of the proposed method. The results show that the proposed method can effectively suppress the inter-slice aliasing and blurring caused by incompleteness of the CL scan data, and that it outperforms other state-of-the-art methods.

Automatic Synthesis of Panoramic Radiographs from Dental Cone Beam Computed Tomography Data.

In this paper, we propose an automatic method of synthesizing panoramic radiographs from dental cone beam computed tomography (CBCT) data for directly observing the whole dentition without the superimposition of other structures. This method consists of three major steps. First, the dental arch curve is generated from the maximum intensity projection (MIP) of 3D CBCT data. Then, based on this curve, the long axial curves of the upper and lower teeth are extracted to create a 3D panoramic curved surface describing the whole dentition. Finally, the panoramic radiograph is synthesized by developing this 3D surface. Both open-bite shaped and closed-bite shaped dental CBCT datasets were applied in this study, and the resulting images were analyzed to evaluate the effectiveness of this method. With the proposed method, a single-slice panoramic radiograph can clearly and completely show the whole dentition without the blur and superimposition of other dental structures. Moreover, thickened panoramic radiographs can also be synthesized with increased slice thickness to show more features, such as the mandibular nerve canal. One feature of the proposed method is that it is automatically performed without human intervention. Another feature of the proposed method is that it requires thinner panoramic radiographs to show the whole dentition than those produced by other existing methods, which contributes to the clarity of the anatomical structures, including the enamel, dentine and pulp. In addition, this method can rapidly process common dental CBCT data. The speed and image quality of this method make it an attractive option for observing the whole dentition in a clinical setting.