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Natural soft tissue achieves a rich variety of functionality through a hierarchy of molecular, microscale, and mesoscale structures and ordering. Inspired by such architectures, we introduce a soft, multifunctional composite capable of a unique combination of sensing, mechanically robust electronic connectivity, and active shape morphing. The material is composed of a compliant and deformable liquid crystal elastomer (LCE) matrix that can achieve macroscopic shape change through a liquid crystal phase transition. The matrix is dispersed with liquid metal (LM) microparticles that are used to tailor the thermal and electrical conductivity of the LCE without detrimentally altering its mechanical or shape-morphing properties. Demonstrations of this composite for sensing, actuation, circuitry, and soft robot locomotion suggest the potential for versatile, tissue-like multifunctionality.

comprised of a conjugated polymer as the electron donor and a fullerene derivative as the electron acceptor. [2,3] Conventional fullerene acceptors like [6,6]-phenyl-C61 butyric acid methyl ester (PCBM) may be unfavorable for practical application, due to the inefficient absorption in visible and near-infrared (IR) regions, fixed molecular structure, complex purification process, and other complications well-documented in the literature. [4][5][6][7][8] In addition, the morphology of polymer-fullerene blends is very sensitive to thermal annealing, solvent additive, film thickness, and especially D:A ratio, resulting in significantly different device performance. [9][10][11] Recently, people have shown that the integration of either polymeric or molecular acceptor into photovoltaic devices would be advantageous. The chemical structures of nonfullerene acceptor can be easily adjusted to tune their energy levels, and the conjugated molecule or polymer acceptor demonstrates enhanced absorption at long wavelengths relative to fullerenes. [12] Thus nonfullerene photovoltaics can have improved harvest of solar radiation, enhanced thermal and mechanical stability, and reduced open-circuit voltage loss. [13] To date, solution-processed nonfullerene solar cells based on polymer-polymer (all-polymer) and polymer-small molecule blend have achieved power conversion efficiencies (PCEs) of 10% and 13%, respectively. [14][15][16][17][18][19] Exciton dissociation and charge transport are at the core of organic photovoltaics, which is strongly affected by the BHJ blend morphology. [20][21][22][23] In fullerene-based systems, the morphology of thin films is critical to the device performance and has been extensively studied. [24] How the blend morphology of nonfullerene blend affects device efficiency and stability is of growing interest as the PCEs of many nonfullerene solar cells now exceed the best fullerene devices. It is well known that the morphology has been largely influenced by the D:A blend ratio. Early studies on fullerene-based devices observed a drastic change in film morphology when fabricating the devices with increased acceptor content. [25][26][27][28] However, for nonfullerene solar cells, recent efforts mainly focus on materials synthesis and device optimization. To the best of our knowledge, systematical study on the effect of blend ratio on the device morphology, performance, and stability has not been reported, while it is of great importance to help achieve in-depth Tuning the blend composition is an essential step to optimize the power conversion efficiency (PCE) of organic bulk heterojunction (BHJ) solar cells. PCEs from devices of unoptimized donor:acceptor (D:A) weight ratio are generally significantly lower than optimized devices. Here, two high-performance organic nonfullerene BHJ blends PBDB-T:ITIC and PBDB-T:N2200 are adopted to investigate the effect of blend ratio on device performance. It is found that the PCEs of polymer-polymer (PBDB-T:N2200) blend are more tolerant to composition changes, relati...

Nanofibers (NFs) of the prototype conjugated polymer, poly(3-hexylthiophene) (P3HT), displaying H- and J-aggregate character are studied using temperature- and pressure-dependent photoluminescence (PL) spectroscopy. Single J-aggregate NF spectra show a decrease of the 0-0/0-1 vibronic intensity ratio from ~2.0 at 300 K to ~1.3 at 4 K. Temperature-dependent PL line shape parameters (i.e., 0-0 energies and 0-0/0-1 intensity ratios) undergo an abrupt change in the range of ~110-130 K suggesting a change in NF chain packing. Pressure-dependent PL lifetimes also show increased contributions from an instrument-limited decay component which is attributed to greater torsional disorder of the P3HT backbone upon decreasing NF volume. It is proposed that the P3HT alkyl side groups change their packing arrangement from a type I to type II configuration causing a decrease in J-aggregate character (lower intrachain order) in both temperature- and pressure-dependent PL spectra. Chain packing dependent exciton and polaron relaxation and recombination dynamics in NF aggregates are next studied using transient absorption spectroscopy (TAS). TAS data reveal faster polaron recombination dynamics in H-type P3HT NFs indicative of interchain delocalization whereas J-type NFs exhibit delayed recombination suggesting that polarons (in addition to excitons) are more delocalized along individual chains. Both time-resolved and steady-state spectra confirm that excitons and polarons in J-type NFs are predominantly intrachain in nature that can acquire interchain character with small structural (chain packing) perturbations.

absorption spectra extending to the NIR region have been designed and applied to the fabrication of OSCs. [6][7][8] A critical challenge arises as one decreases optical bandgaps (E g opt ) with respect to simultaneously achieving a high external quantum efficiency (EQE) and high open-circuit voltage (V OC ). [9] This challenge is due to the counterbalance between the driving force for charge separation, which aids in photocurrent generation, and voltage loss in the cell. [10,11] Finding ways to maximize V OC requires one to reduce the energy loss (E loss = E g opt -eV OC ) that occurs as a result of the multiple states that follow exciton generation. [12] Narrow bandgap (NBG) non-fullerene acceptors (NFAs) have emerged as the next generation of electron acceptors in OSCs. [13][14][15][16][17][18] Tunability of E g opt through molecular design allows one to tailor NIR absorption characteristics. [19,20] Considering that the maximum human photopic sensitivity is 555 nm and the maximum human scotopic sensitivity is 507 nm, [21] transparent photoactive materials should predominantly absorb solar radiation from ≈650 nm into the NIR region for semitransparent solar cell applications. In addition, since ≈50% of solar radiation intensity is in the NIR region, the development of NBG-NFAs with E g opt below ≈1.35 eV is desirable to effectively harvest solar NIR radiation. [1] Another encouraging feature of NFAs is that the energetic offsets that drive charge generation are small (<0.3 eV), [18,[22][23][24] which is beneficial for maintaining low E loss . Despite these desirable features, there has been less consideration for designing NBG-NFAs for transparent/NIR absorbing OSC applications. To address this challenge and expand the design of NIR harvesting acceptor molecules, we demonstrate in this contribution a new molecular design for ultra NBG-NFA materials with strong NIR response and small E loss .The two NBG NFAs described in this contribution are COTIC-4F and SiOTIC-4F (Figure 1a). Their molecular design includes incorporation of a cyclopentadithiophene (CPDT), or dithienosilole (DTS), unit as the central donor (D) fragment, which is flanked by two alkoxythienyl units (D′) to form an electron-rich D′-D-D′ central core. The D′-D-D′ units are end-capped with Two narrow bandgap non-fullerene acceptors (NBG-NFAs), namely, COTIC-4F and SiOTIC-4F, are designed and synthesized for the fabrication of efficient near-infrared organic solar cells (OSCs). The chemical structures of the NBG-NFAs contain a D′-D-D′ electron-rich internal core based on a cyclopentadithiophene (or dithienosilole) (D) and alkoxythienyl (D′) core, end-capped with the highly electron-deficient unit 2-(5,6-difluoro-3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (A), ultimately providing a A-D′-D-D′-A molecularconfiguration that enhances the intramolecular charge transfer characteristics of the excited states. One can thereby reduce the optical bandgap (E g opt ) to as low as ≈1.10 eV, one of the smallest values for NFAs reported to date. In bulk-he...

Soft actuators that undergo programmable shape change in response to a stimulus are enabling components of future soft robots and other soft machines. Strategies to power these actuators often require the incorporation of rigid, electrically conductive materials into the soft actuator, thus limiting the compliance and shape change of the material. In this study, we develop a 4D-printable composite composed of liquid crystal elastomer (LCE) matrix with dispersed droplets of eutectic gallium indium alloy (EGaIn). Using deformable EGaIn droplets in place of rigid conductive fillers preserves the compliance and shape-morphing properties of the LCE. The process enables 4D-printed LCE actuators capable of photothermal and electrothermal actuation. At low liquid metal (LM) concentrations (71 wt %), the composite actuator exhibits a photothermal response upon irradiation of near-IR light. Printed actuators with a twisted nematic configuration are capable of bending angles of 150° at 800 mW cm–2. At higher LM concentrations (88 wt %), the embedded LM droplets can form percolating networks that conduct electricity and enable electrical Joule heating of the LCE. Actuation strain ranging from 5 to 12% is controlled by the amount of electrical power that is delivered to the composite. We also introduce a method for multimaterial printing of monolithic structures where the LM filler loading is spatially varied. These multifunctional materials exhibit innate responsivity where the actuator behaves as an electrical switch and can report one of two states (on/off). These multiresponsive, 4D-printable composites enable multifunctional, mechanically active structures that can be powered with IR light or low DC voltages.

By the introduction of different building blocks and side‐chains, a series of donor–acceptor type polymer acceptors containing naphthalene diimide have been successfully prepared. The theoretical and experimental results show that the molecular design effectively tunes the energy levels, solubility, and coplanarity of the acceptor polymers. The intermolecular packing, which has been considered as a key factor in the bulk heterojunction morphology, has been adjusted by changing the coplanarity. As a result of improved morphology and fine‐tuned energy levels, a power conversion efficiency of 6.0% has been demonstrated for the optimized devices, which is among the highest‐efficiencies for reported all‐polymer solar cells. The improved device performance may be attributed to the resemble crystallinity of the donor/acceptor polymers, which can lead to the optimal phase separation morphology balancing both charge transfer and transport.

The field effect transistor (FET) is arguably one of the most important circuit elements in modern electronics. Recently, a need has developed for flexible electronics in a variety of emerging applications. Examples include form‐fitting healthcare‐monitoring devices, flexible displays, and flexible radio frequency identification tags. Organic FETs (OFETs) are viable candidates for producing such flexible devices because they incorporate semiconducting π‐conjugated materials, including small molecules and conjugated polymers, which are intrinsically soft and mechanically compatible with flexible substrates. For OFETs to be industrially viable, however, they must achieve not only high charge carrier mobility, but also ideal and comprehensible electrical characteristics. Most recently, nonideal double‐slope characteristics in the transfer curves of OFETs (i.e., high slope at low gate voltage and low slope at high gate voltage), have stirred debate, which has led to different mechanistic rationales in the literature. This review focuses on the general observations, mechanistic understanding, and possible solutions associated with phenomena that result in FETs with double‐slope characteristics. By surveying and systematically summarizing in a single source relevant literature that deals with the issue of double slope, the experimental framework and theoretical basis for interpreting and avoiding this electrical nonideality in OFETs is provided.