Yingzhi Jin

A nonfullerene acceptor based active layer with high halogen contents is designed to fabricate efficient thick‐film organic solar cells. The conventional structure device using chlorinated acceptor F–2Cl and fluorinated donor PM6 exhibits a power conversion efficiency over 10% with an active layer thickness of 600 nm.

Abstract

Developing efficient organic solar cells (OSCs) with relatively thick active layer compatible with the roll to roll large area printing process is an inevitable requirement for the commercialization of this field. However, typical laboratory OSCs generally exhibit active layers with optimized thickness around 100 nm and very low thickness tolerance, which cannot be suitable for roll to roll process. In this work, high performance of thick‐film organic solar cells employing a nonfullerene acceptor F–2Cl and a polymer donor PM6 is demonstrated. High power conversion efficiencies (PCEs) of 13.80% in the inverted structure device and 12.83% in the conventional structure device are achieved under optimized conditions. PCE of 9.03% is obtained for the inverted device with active layer thickness of 500 nm. It is worth noting that the conventional structure device still maintains the PCE of over 10% when the film thickness of the active layer is 600 nm, which is the highest value for the NF‐OSCs with such a large active layer thickness. It is found that the performance difference between the thick active layer films based conventional and inverted devices is attributed to their different vertical phase separation in the active layers.

Recently, sequential deposition of donor and acceptor layers has been demonstrated to be an alternative method to fabricate highly efficient bulk‐heterojunction organic solar cells. A simple “needle” model to simulate its morphology indicates a different morphological requirement which rationalizes the high exciton dissociation efficiency.

Abstract

Bulk heterojunction (BHJ) nonfullerene organic solar cells prepared from sequentially deposited donor and acceptor layers (sq‐BHJ) have recently been shown to be highly efficient, environmentally friendly, and compatible with large area and roll‐to‐roll fabrication. However, the related photophysics at donor‐acceptor interface and the vertical heterogeneity of donor‐acceptor distribution, critical for exciton dissociation and device performance, have been largely unexplored. Herein, steady‐state and time‐resolved optical and electrical techniques are employed to characterize the interfacial trap states. Correlating with the luminescent efficiency of interfacial states and its nonradiative recombination, interfacial trap states are characterized to be about 40% more populated in the sq‐BHJ devices than the as‐cast BHJ (c‐BHJ), which probably limits the device voltage output. Cross‐sectional energy‐dispersive X‐ray spectroscopy and ultraviolet photoemission spectroscopy depth profiling directly visualize the donor–acceptor vertical stratification with a precision of 1–2 nm. From the proposed “needle” model, the high exciton dissociation efficiency is rationalized. This study highlights the promise of sequential deposition to fabricate efficient solar cells, and points toward improving the voltage output and overall device performance via eliminating interfacial trap states.

Structural, electronic band structure, and electrical properties of a series of charge‐transfer cocrystals based on F₆TNAP and six planar donors are presented. Density functional theory calculations afford large conduction bandwidths and low effective masses for all six cocrystals. A few cocrystals exhibit charge‐carrier mobilities in excess of 1 cm² V⁻¹ s⁻¹, as estimated from space‐charge limited current measurements.

Abstract

The crystal structures of the charge‐transfer (CT) cocrystals formed by the π‐electron acceptor 1,3,4,5,7,8‐hexafluoro‐11,11,12,12‐tetracyanonaphtho‐2,6‐quinodimethane (F₆TNAP) with the planar π‐electron‐donor molecules triphenylene (TP), benzo[b]benzo[4,5]thieno[2,3‐d]thiophene (BTBT), benzo[1,2‐b:4,5‐b′]dithiophene (BDT), pyrene (PY), anthracene (ANT), and carbazole (CBZ) have been determined using single‐crystal X‐ray diffraction (SCXRD), along with those of two polymorphs of F₆TNAP. All six cocrystals exhibit 1:1 donor/acceptor stoichiometry and adopt mixed‐stacking motifs. Cocrystals based on BTBT and CBZ π‐electron donor molecules exhibit brickwork packing, while the other four CT cocrystals show herringbone‐type crystal packing. Infrared spectroscopy, molecular geometries determined by SCXRD, and electronic structure calculations indicate that the extent of ground‐state CT in each cocrystal is small. Density functional theory calculations predict large conduction bandwidths and, consequently, low effective masses for electrons for all six CT cocrystals, while the TP‐, BDT‐, and PY‐based cocrystals are also predicted to have large valence bandwidths and low effective masses for holes. Charge‐carrier mobility values are obtained from space‐charge limited current (SCLC) measurements and field‐effect transistor measurements, with values exceeding 1 cm² V⁻¹ s¹ being estimated from SCLC measurements for BTBT:F₆TNAP and CBZ:F₆TNAP cocrystals.

A series of high‐performance perylene diimide based molecular acceptors, namely, TPP‐PDI, TPO‐PDI, and TPS‐PDI, are smartly designed for efficient nonfullerene polymer solar cells. Combined with the optimization of the blend morphology through supramolecular molecular lock effect, the champion power conversion efficiency of 11.01% is realized in TPO‐PDI‐based devices.

Abstract

A series of perylene diimide (PDI) derivatives, TPP‐PDI, TPO‐PDI, and TPS‐PDI, are developed for nonfullerene polymer solar cells (NF‐PSCs) by flaking three PDI skeletons around 3D central cores with different configurations and electronic states, such as triphenylphosphine (TPP), triphenylphosphine monoxide (TPO), and triphenylphosphine sulfide (TPS). These small‐molecule acceptors have a “three‐wing propeller” structure due to their similar backbones. By changing the electron density of phosphorus atoms through oxidation and sulfuration, the “folding‐back” strength is decreased, resulting in a less twisted molecular conformation. The stronger electron‐withdrawing ability of the oxygen atom affords TPO‐PDI the least twisted conformation, which enhances the crystallinity of this complex. NF‐PSCs based on PTTEA:TPO‐PDI exhibit a high power conversion efficiency (PCE) of 8.65%. Ultimately, the joint “molecular lock” effect arising from OH⋅⋅⋅F and OH⋅⋅⋅OP supramolecular interactions is achieved by introducing 4,4′‐biphenol as an additive, which successfully promotes fibril‐like phase separation and blend morphology optimization to generate the highest PCE of 11.01%, which is currently the highest value recorded for NF‐PSCs based on PDI acceptors.

Effect of side chain length of central fused‐ring on the physicochemical, self‐assembly, and photovoltaic properties of the small molecule acceptors (SMAs) is investigated. Single‐crystal structure and grazing incidence wide‐angle X‐ray scattering results reveal that the longer side chains lead to different long‐range ordering in the molecular aggregation, which improves the molecular ordering in films and increases photovoltaic performance of the SMAs.

Abstract

The effects of central alkoxy side chain length of a series of narrow bandgap small molecule acceptors (SMAs) on their physicochemical properties and on the photovoltaic performance of the SMA‐based polymer solar cells (PSCs) are systematically investigated. It is found that the ordered aggregation of these SMAs in films is enhanced gradually with the increase of alkoxy chain length. The single‐crystal structures of these SMAs further reveal that small changes in the side chain length can have a dramatic impact on molecular self‐assembly. The short‐circuit current density and power conversion efficiency values of the corresponding PSCs increase with the increase of the side chain length of the SMAs. The π–π coherence length of the SMAs in the active layers is increased with the increase of the side chain length, which could be the reason for the increase of the J _sc in the PSCs. The results indicate that small changes in side chain length can have a dramatic impact on the molecular self‐assembly, morphology, and photovoltaic performance of the PSCs. The structure–performance relationship established in this study can provide important instructions for the side chain engineering and for the design of efficient SMAs materials.

Lignin as a reinforced binder is incorporated into cellulose fibers by successive infiltration and mechanical hot‐pressing. The resulting lignin‐cellulose composite exhibits an outstanding isotropic tensile strength and good water stability, while its thermostability and UV‐blocking performance are also improved. This biodegradable and sustainable composite with both components from natural wood represents a promising alternative that can potentially replace the nonbiodegradable plastics.

Abstract

Plastic waste has been increasingly transferred from land into the ocean and has accumulated within the food chain, causing a great threat to the environment and human health, indicating that fabricating an eco‐friendly and biodegradable replacement is urgent. Paper made of cellulose is attractive in terms of its favorable biodegradability, resource abundance, large manufacturing scale, and low material cost, but is usually hindered by its inferior stability against water and poor mechanical strength for plastic replacement. Here, inspired by the reinforcement principle of cellulose and lignin in natural wood, a strong and hydrostable cellulosic material is developed by integrating lignin into the cellulose. Lignin as a reinforced matrix is incorporated to the cellulose fiber scaffold by successive infiltration and mechanical hot‐pressing treatments. The resulting lignin‐cellulose composite exhibits an outstanding isotropic tensile strength of 200 MPa, which is significantly higher than that of conventional cellulose paper (40 MPa) and some commercial petroleum‐based plastics. Additionally, the composite demonstrates a superior wet strength of 50 MPa. Adding lignin also improves the thermostability and UV‐blocking performance of cellulose paper. The demonstrated lignin‐cellulose composite is biodegradable and eco‐friendly with both components from natural wood, which represents a promising alternative that can potentially replace the nonbiodegradable plastics.

Charge extraction in bulk‐heterojunction (BHJ) organic photovoltaics is most efficient when the contact area between the semiconductors and electrodes is maximized. We show that ≈99% of this area can in fact be insulating without degrading the efficiency of charge carrier extraction, provided the spacing of the conducting areas is less than or equal to twice the BHJ thickness.

Abstract

It is widely considered that charge carrier extraction in bulk‐heterojunction organic photovoltaics (BHJ OPVs) is most efficient when the area of contact between the semiconductor layers and the electrodes is maximized and the electrodes are electrically homogeneous. Herein, it is shown that ≈99% of the electrode surface can in fact be insulating without degrading the efficiency of charge carrier extraction, provided the spacing of the conducting areas is less than or equal to twice the optimal thickness of the BHJ layer. This striking result is demonstrated for BHJ OPVs with both conventional and inverted device architectures using two different types of BHJ OPVs, namely, PCDTBT:PC₇₀BM and the ternary blend PBDB‐T:ITIC‐m:PC₇₀BM. This finding opens the door to the use of a large pallet of materials for optical spacers and charge transport layers, based on a low density of conducting particles embedded in a wide bandgap insulating matrix.

Organic photodetectors (OPDs) are promising for large area image detectors. Minimizing the dark current density (J _d) is crucial in most applications; nevertheless, a wide range of J _d values has been reported. Here, possible reasons that lead to this large variation are discussed. A quantitative analysis of intrinsic J _d processes shows that charge injection from the electrodes is the dominant mechanism.

Abstract

Organic photodetectors (OPDs) have gained increasing interest as they offer cost‐effective fabrication methods using low temperature processes, making them particularly attractive for large area image detectors on lightweight flexible plastic substrates. Moreover, their photophysical and optoelectronic properties can be tuned both at a material and device level. Visible‐light OPDs are proposed for use in indirect‐conversion X‐ray detectors, fingerprint scanners, and intelligent surfaces for gesture recognition. Near‐infrared OPDs find applications in biomedical imaging and optical communications. For most applications, minimizing the OPD dark current density (J _d) is crucial to improve important figures of merits such as the signal‐to‐noise ratio, the linear dynamic range, and the specific detectivity (D *). Here, a quantitative analysis of the intrinsic dark current processes shows that charge injection from the electrodes is the dominant contribution to J _d in OPDs. J _d reduction is typically addressed by fine‐tuning the active layer energetics and stratification or by using charge blocking layers. Yet, most experimental J _d values are higher than the calculated intrinsic limit. Possible reasons for this deviation are discussed, including extrinsic defects in the photoactive layer and the presence of trap states. This provides the reader with guidelines to improve the OPD performances in view of imaging applications.

A novel sidechain‐modified 3,4‐ethylene dioxythiophene derivative is polymerized in a large‐area roll‐to‐roll process. As an electrochromic thin film, the corresponding poly(3,4‐ethylene dioxythiophene) derivative shows enhanced electrochromic properties regarding visible light transmittance change (Δτ _v = 59%, ΔL* = 54.1), coloration efficiency (η = 530 cm² C⁻¹) and color neutrality in the bleached state (L* = 83.8, a* = −4.3, b* = −4.1).

Abstract

Conjugated electrochromic (EC) polymers for flexible EC devices (ECDs) generally lack a fully colorless bleached state. A strategy to overcome this drawback is the implementation of a new sidechain‐modified poly(3,4‐ethylene dioxythiophene) derivative that can be deposited in thin‐film form in a customized high‐throughput and large‐area roll‐to‐roll polymerization process. The sidechain modification provides enhanced EC properties in terms of visible light transmittance change, Δτ_v = 59% (ΔL* = 54.1), contrast ratio (CR = 15.8), coloration efficiency (η = 530 cm² C⁻¹), and color neutrality (L* = 83.8, a* = −4.3, b* = −4.1) in the bleached state. The intense blue‐colored polymer thin films exhibit high cycle stability (10 000 cycles) and fast response times. The design, synthesis, and polymerization of the modified 3,4‐ethylene dioxythiophene derivative are discussed along with a detailed optical, electrochemical, and spectroelectrochemical characterization of the resulting EC thin films. Finally, a flexible see‐through ECD with a visible light transmittance change of Δτ_v = 47% (ΔL* = 51.9) and a neutral‐colored bleached state is developed.

An electron‐deficient unit containing B←N bonds, namely BNIDT, is developed to construct polymer acceptors for photovoltaic applications. Desirable optoelectronic properties such as broad absorption profiles, low‐lying energy levels, ambipolar charge transport properties, and strong electron‐affinity are found for these polymers. All‐polymer solar cells using these B←N embedded polymers as acceptor materials exhibit an enhanced efficiency of 8.78%.

Abstract

In the field of all‐polymer solar cells (all‐PSCs), all efficient polymer acceptors that exhibit efficiencies beyond 8% are based on either imide or dicyanoethylene. To boost the development of this promising solar cell type, creating novel electron‐deficient units to build high‐performance polymer acceptors is critical. A novel electron‐deficient unit containing B←N bonds, namely, BNIDT, is synthesized. Systematic investigation of BNIDT reveals desirable properties including good coplanarity, favorable single‐crystal structure, narrowed bandgap and downshifted energy levels, and extended absorption profiles. By copolymerizing BNIDT with thiophene and 3,4‐difluorothiophene, two novel conjugated polymers named BN‐T and BN‐2fT are developed, respectively. It is shown that these polymers possess wide absorption spectra covering 350–800 nm, low‐lying energy levels, and ambipolar film‐transistor characteristics. Using PBDB‐T as the donor and BN‐2fT as the acceptor, all‐PSCs afford an encouraging efficiency of 8.78%, which is the highest for all‐PSCs excluding the devices based on imide and dicyanoethylene‐type acceptors. Considering that the structure of BNIDT is totally different from these classical units, this work opens up a new class of electron‐deficient unit for constructing efficient polymer acceptors that can realize efficiencies beyond 8% for the first time.

An ideal materials combination based on the electron donor BSFTR and acceptor Y6 is selected to construct small‐molecule solar cells (SMSCs). By morphology optimization, an extraordinary power conversion efficiency of 13.69% with a remarkably low energy loss of 0.48 eV is achieved, which is beneficial from the matched photoelectric properties, the favorable blend morphology, and is the best binary SMSC performance reported so far.

Abstract

Compared with the quick development of polymer solar cells, achieving high‐efficiency small‐molecule solar cells (SMSCs) remains highly challenging, as they are limited by the lack of matched materials and morphology control to a great extent. Herein, two small molecules, BSFTR and Y6, which possess broad as well as matched absorption and energy levels, are applied in SMSCs. Morphology optimization with sequential solvent vapor and thermal annealing makes their blend films show proper crystallinity, balanced and high mobilities, and favorable phase separation, which is conducive for exciton dissociation, charge transport, and extraction. These contribute to a remarkable power conversion efficiency up to 13.69% with an open‐circuit voltage of 0.85 V, a high short‐circuit current of 23.16 mA cm⁻² and a fill factor of 69.66%, which is the highest value among binary SMSCs ever reported. This result indicates that a combination of materials with matched photoelectric properties and subtle morphology control is the inevitable route to high‐performance SMSCs.

Thanks to the strong electron‐donating capability of carbon–oxygen‐bridged (CO‐bridged) ladder‐type building blocks, CO‐bridged nonfullerene acceptors (NFAs) present low bandgaps and strong light‐harvesting capability, delivering high short‐circuit current density (>28 mA cm⁻²) and high power conversion efficiency (>14% for single‐junction and >17% for tandem) in organic solar cells.

Abstract

Recently, acceptor–donor–acceptor (A–D–A) small molecules have emerged as promising nonfullerene acceptors (NFAs) for organic solar cells and have attracted great attention. The carbon‐bridged (C‐bridged) ladder‐type D unit plays a crucial role in developing high‐performance A–D–A NFAs. However, the medium electron‐donating capability of C‐bridged units is unfavorable for making NFAs with strong light‐harvesting capability. In this regard, carbon–oxygen‐bridged (CO‐bridged) ladder‐type units present advantages in developing strong light‐absorbing NFAs. Here, recent progress in the newly emerging CO‐bridged NFAs is highlighted. The synthetic methods for the polycyclic CO‐bridged building blocks are introduced. The photovoltaic performance for CO‐bridged NFAs is summarized and discussed. Perspectives on developing high‐performance CO‐bridged‐NFA‐based solar cells are made.

Aromatic‐diimide‐based polymers have emerged as the most promising n‐type semiconductors and their photovoltaic performance has been significantly improved in the past decade. The recent exciting progress is highlighted and the structure–property relationship of aromatic‐diimde‐based photovoltaic polymers is revealed, which could provide important guidelines for the further design of n‐type photovoltaic polymers.

Abstract

All‐polymer solar cells (all‐PSCs) have attracted immense attention in recent years due to their advantages of tunable absorption spectra and electronic energy levels for both donor and acceptor polymers, as well as their superior thermal and mechanical stability. The exploration of the novel n‐type conjugated polymers (CPs), especially based on aromatic diimide (ADI), plays a vital role in the further improvement of power conversion efficiency (PCE) of all‐PSCs. Here, recent progress in structure modification of ADIs including naphthalene diimide (NDI), perylene diimide (PDI), and corresponding derivatives is reviewed, and the structure–property relationships of ADI‐based CPs are revealed.

Upconverted circularly polarized luminescence (UC‐CPL) via triplet–triplet annihilation‐based photon upconversion in chiral systems is an emerging topic in photochemistry and photophysics. The concept of this topic is described, and recent advances in the construction and application of UC‐CPL materials are highlighted. In addition, new functions emerging from UC‐CPL materials are presented.

Abstract

Circularly polarized luminescent materials are of increasing attention due to their potential applications in advanced optical technologies, such as chiroptical devices and optical sensing. Recently, in all reported circularly polarized luminescent materials, high‐energy excitation results in low‐energy or downconverted circularly polarized luminescence (CPL) emission. Although photon upconversion—i.e., the conversion of low‐energy light into higher‐energy emission, with a wide variety of applications—has been widely reported, the integration of photon upconversion and CPL in one chiral system to achieve higher‐energy CPL emission has never been reported. Herein, a brief review is provided of recent achievements in photon‐upconverted CPL via the triplet–triplet annihilation mechanism, focusing on the amplified dissymmetry factor g _lum through energy transfer process and dual upconverted and downconverted CPL emission through chirality and energy transfer process.

“As good as gold” is a seldom true adage, but in article number https://doi.org/10.1002/adma.2019032711903271, Bahram Nabet and co‐workers show that using a Ti₃C₂Tz (MXene) aqueous suspension, a table‐top spinner, and acetone, GaAs photodetectors that outperform conventional ones using Ti/Au can be fabricated. This ambient condition process is promising for integration into microelectronics, photonic integrated circuits, and silicon photonics technologies.

Highly flexible and conductive smart fibres and textiles with integrated multifunctionality are fabricated by assembling cellulose nanofibrils and Ti₃C₂ MXene using a facile 3D printing process. The resultant smart fibres and textiles exhibit excellent responsiveness to multiple external stimuli (electrical/photonic/mechanical). The smart textile can also be processed into a sensitive strain sensor to achieve real‐time human motion recognition.

Abstract

Fibre‐based materials have received tremendous attention due to their flexibility and wearability. Although great efforts have been devoted to achieve high‐performance fibres over the past several years, it is still challenging for multifunctional macroscopic fibres to satisfy versatile applications. 2D transition metal carbides/nitrides (MXenes) with intriguing physical/chemical properties have been explored in broad application, and may be able to reinforce synthetic fibres. Inspired by natural materials, for the first time, flexible smart fibres and textiles are fabricated using a 3D printing process with hybrid inks of TEMPO (2,2,6,6‐tetramethylpiperidine‐1‐oxylradi‐cal)‐mediated oxidized cellulose nanofibrils (TOCNFs) and Ti₃C₂ MXene. The hybrid inks display good rheological properties, which allow them to achieve accurate structures and be rapidly printed. TOCNFs/Ti₃C₂ in hybrid inks self‐assemble to fibres with an aligned structure in ethanol, mimicking the features of the natural structures of plant fibres. In contrast to conventional synthetic fibres with limited functions, smart TOCNFs/Ti₃C₂ fibres and textiles exhibit significant responsiveness to multiple external stimuli (electrical/photonic/mechanical). TOCNFs/Ti₃C₂ textiles with electromechanical performance can be processed into sensitive strain sensors. Such multifunctional smart fibres and textiles will be promising in diverse applications, including wearable heating textiles, human health monitoring, and human–machine interfaces.

A series of high‐performance perylene diimide based molecular acceptors, namely, TPP‐PDI, TPO‐PDI, and TPS‐PDI, are smartly designed for efficient nonfullerene polymer solar cells. Combined with the optimization of the blend morphology through supramolecular molecular lock effect, the champion power conversion efficiency of 11.01% is realized in TPO‐PDI‐based devices.

Abstract

A series of perylene diimide (PDI) derivatives, TPP‐PDI, TPO‐PDI, and TPS‐PDI, are developed for nonfullerene polymer solar cells (NF‐PSCs) by flaking three PDI skeletons around 3D central cores with different configurations and electronic states, such as triphenylphosphine (TPP), triphenylphosphine monoxide (TPO), and triphenylphosphine sulfide (TPS). These small‐molecule acceptors have a “three‐wing propeller” structure due to their similar backbones. By changing the electron density of phosphorus atoms through oxidation and sulfuration, the “folding‐back” strength is decreased, resulting in a less twisted molecular conformation. The stronger electron‐withdrawing ability of the oxygen atom affords TPO‐PDI the least twisted conformation, which enhances the crystallinity of this complex. NF‐PSCs based on PTTEA:TPO‐PDI exhibit a high power conversion efficiency (PCE) of 8.65%. Ultimately, the joint “molecular lock” effect arising from OH⋅⋅⋅F and OH⋅⋅⋅OP supramolecular interactions is achieved by introducing 4,4′‐biphenol as an additive, which successfully promotes fibril‐like phase separation and blend morphology optimization to generate the highest PCE of 11.01%, which is currently the highest value recorded for NF‐PSCs based on PDI acceptors.

Light‐emitting field‐effect transistors are optoelectronic devices that combine switching and amplification with light emission. They can be created with a wide range of semiconductors from organic to inorganic and even nanoscale materials. Their unique structure and properties enable applications that include plasmonic or photonic interactions as well as optical memory.

Abstract

Light‐emitting field‐effect transistors (LEFETs) combine switching and amplification with light emission and thus represent an interesting optoelectronic device. They are not limited anymore to a few examples and specific materials but are nearly universal for a wide range of semiconductors, from organic to inorganic and nanoscale. This review introduces the basic working principles of lateral unipolar and ambipolar LEFETs and discusses recent examples based on various solution‐processed semiconducting materials. Applications beyond simple light emission are presented and possible future directions for light‐emitting transistors with added functionalities are outlined.

The high‐performing single‐junction organic solar cell blend, PM6:Y6, is examined to obtain an in‐depth understanding of the voltage losses, and charge recombination and extraction dynamics. The devices exhibit remarkable extraction coupled with moderate recombination losses. This behavior can most likely be credited to a beneficial morphology as evidenced by atomically resolved ¹⁹F magic‐angle‐spinning solid‐state NMR analysis.

Abstract

The highly efficient single‐junction bulk‐heterojunction (BHJ) PM6:Y6 system can achieve high open‐circuit voltages (V _OC) while maintaining exceptional fill‐factor (FF) and short‐circuit current (J _SC) values. With a low energetic offset, the blend system is found to exhibit radiative and non‐radiative recombination losses that are among the lower reported values in the literature. Recombination and extraction dynamic studies reveal that the device shows moderate non‐geminate recombination coupled with exceptional extraction throughout the relevant operating conditions. Several surface and bulk characterization techniques are employed to understand the phase separation, long‐range ordering, as well as donor:acceptor (D:A) inter‐ and intramolecular interactions at an atomic‐level resolution. This is achieved using photo‐conductive atomic force microscopy, grazing‐incidence wide‐angle X‐ray scattering, and solid‐state ¹⁹F magic‐angle‐spinning NMR spectroscopy. The synergy of multifaceted characterization and device physics is used to uncover key insights, for the first time, on the structure–property relationships of this high‐performing BHJ blend. Detailed information about atomically resolved D:A interactions and packing reveals that the high performance of over 15% efficiency in this blend can be correlated to a beneficial morphology that allows high J _SC and FF to be retained despite the low energetic offset.

In article number https://doi.org/10.1002/adma.2019036491903649, Xiaotian Hu, Wei Ma, Yiwang Chen, and co‐workers report a general approach to upscale flexible organic photovoltaics to the module scale without obvious efficiency loss by calculating the shear impulse during the coating/printing process. Photoelectric conversion efficiencies of 9.77% for a 1 cm² single chip and 8.90% for a 15 cm² solar module are demonstrated. The mechanics of shear impulse link the spin‐coating and slot‐die printing like a small boat overcoming the obstacles of thousands of mountains to arrive at a large‐area printing ferry. This research method also opens up a new strategy of lab‐to‐manufacturing translation for organic optoelectronic devices.

In article number https://doi.org/10.1002/adma.2019029771902977, Liangqi Ouyang, Mahiar M. Hamedi, and co‐workers report the fabrication of freestanding and multifunctional nanocomposite films of 2D Ti₃C₂T _x MXene and 1D cellulose nanofibrils (CNFs) with a high mechanical strength of 341 MPa and high conductivity of 295 S cm⁻¹. These films, despite their high mechanical robustness, deliver a high capacitance of 298 F g⁻¹, which places them among the best multifunctional supercapacitor electrode materials reported to date. The stable and patternable hybrid dispersion of 2D Ti₃C₂T _x MXene and 1D CNFs is also used to fabricate micro‐supercapacitor electrodes and printed electronics with a variety of shapes. Image credit: Armin VahidMohammadi.