Polycrystalline SnS, Sn2S3, and SnS2 were deposited onto glass substrates by vapor transport deposition, with the stoichiometry controlled by deposition temperature. In addition, epitaxial growth of orthorhombic SnS(010) films on NaCl(100) with thicknesses up to 600 nm was demonstrated. The in-plane [100] directions of SnS and NaCl are oriented approximately 45° apart, and the translational relationship between SnS and NaCl was predicted by density functional theory. The epitaxial SnS is p-type with carrier concentration on the order of 1017 cm−3 and Hall hole mobility of 385 cm2 V−1 s−1 in-plane. It has indirect and direct bandgaps of 1.0 and 2.3 eV, respectively.
The mechanical properties of π-conjugated (semiconducting) polymers are a key determinant of the stability and manufacturability of devices envisioned for applications in energy and healthcare. These propertiesincluding modulus, extensibility, toughness, and strengthare influenced by the morphology of the solid film, which depends on the method of processing. To date, the majority of work done on the mechanical properties of semiconducting polymers has been performed on films deposited by spin coating, a process not amenable to the manufacturing of largearea films. Here, we compare the mechanical properties of thin films of regioregular poly(3-heptylthiophene) (P3HpT) produced by three scalable deposition processesinterfacial spreading, solution shearing, and spray coatingand spin coating (as a reference). Our results lead to four principal conclusions. (1) Spray-coated films have poor mechanical robustness due to defects and inhomogeneous thickness. (2) Sheared films show the highest modulus, strength, and toughness, likely resulting from a decrease in free volume. (3) Interfacially spread films show a lower modulus but greater fracture strain than spin-coated films. (4) The trends observed in the tensile behavior of films cast using different deposition processes held true for both P3HpT and poly(3butylthiophene) (P3BT), an analogue with a higher glass transition temperature. Grazing incidence X-ray diffraction and ultraviolet−visible spectroscopy reveal many notable differences in the solid structures of P3HpT films generated by all four processes. While these morphological differences provide possible explanations for differences in the electronic properties (hole mobility), we find that the mechanical properties of the film are dominated by the free volume and surface topography. In field-effect transistors, spread films had mobilities more than 1 magnitude greater than any other films, likely due to a relatively high proportion of edge-on texturing and long coherence length in the crystalline domains. Overall, spread films offer the best combination of deformability and charge-transport properties.
Haptic devices are in general more adept at mimicking the bulk properties of materials than they are at mimicking the surface properties. Herein, a haptic glove is described which is capable of producing sensations reminiscent of three types of near‐surface properties: hardness, temperature, and roughness. To accomplish this mixed mode of stimulation, three types of haptic actuators are combined: vibrotactile motors, thermoelectric devices, and electrotactile electrodes made from a stretchable conductive polymer synthesized in the laboratory. This polymer consists of a stretchable polyanion which serves as a scaffold for the polymerization of poly(3,4‐ethylenedioxythiophene). The scaffold is synthesized using controlled radical polymerization to afford material of low dispersity, relatively high conductivity, and low impedance relative to metals. The glove is equipped with flex sensors to make it possible to control a robotic hand and a hand in virtual reality (VR). In psychophysical experiments, human participants are able to discern combinations of electrotactile, vibrotactile, and thermal stimulation in VR. Participants trained to associate these sensations with roughness, hardness, and temperature have an overall accuracy of 98%, whereas untrained participants have an accuracy of 85%. Sensations can similarly be conveyed using a robotic hand equipped with sensors for pressure and temperature.
The conductive polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is ubiquitous in research dealing with organic electronic devices (e.g., solar cells, wearable and implantable sensors, and electrochemical transistors). In many bioelectronic applications, the applicability of commercially available formulations of PEDOT:PSS (e.g., Clevios) is limited by its poor mechanical properties. Additives can be used to increase the compliance but pose a risk of leaching, which can result in device failure and increased toxicity (in biological settings). Thus, to increase the mechanical compliance of PEDOT:PSS without additives, we synthesized a library of intrinsically stretchable block copolymers. In particular, controlled radical polymerization using a reversible addition–fragmentation transfer process was used to generate block copolymers consisting of a block of PSS (of fixed length) appended to varying blocks of poly(poly(ethylene glycol) methyl ether acrylate) (PPEGMEA). These block copolymers (PSS(1)-b-PPEGMEA(x), where x ranges from 1 to 6) were used as scaffolds for oxidative polymerization of PEDOT. By increasing the lengths of the PPEGMEA segments on the PEDOT:[PSS(1)-b-PPEGMEA(1–6)] block copolymers, (“Block-1” to “Block-6”), or by blending these copolymers with PEDOT:PSS, the mechanical and electronic properties of the polymer can be tuned. Our results indicate that the polymer with the longest block of PPEGMEA, Block-6, had the highest fracture strain (75%) and lowest elastic modulus (9.7 MPa), though at the expense of conductivity (0.01 S cm–1). However, blending Block-6 with PEDOT:PSS to compensate for the insulating nature of the PPEGMEA resulted in increased conductivity [2.14 S cm–1 for Blend-6 (2:1)]. Finally, we showed that Block-6 outperforms a commercial formulation of PEDOT:PSS as a dry electrode for surface electromyography due to its favorable mechanical properties and better adhesion to skin.
This paper demonstrates that a thin polymeric film (10−80 nm) can be continuously drawn from the meniscus of a nonpolar polymer solution at an air−water−fluoropolymer interface using a roll-to-roll process: "interfacial drawing". With this process, it is possible to control the thickness of the film by manipulating the concentration of the solution, along with the drawing velocity of the receiving substrate. We demonstrate the formation of thin films >1 m in length and 1000 cm 2 in area, using our custom-designed apparatus. Interfacial drawing has three characteristics which compare favorably to other methods of forming and depositing polymeric thin films. First, the films are solidified prior to deposition, which means that they can be used to uniformly coat nonplanar, rough, or porous substrates. Second, these films can be stacked into multilayered architectures without risk of redissolving the layer beneath. Third, for some materials, the process yields films with superior mechanical compliance for applications such as wearable or flexible devices, compared to films produced by spin-coating. We demonstrate the utility of interfacial drawing by forming thin films of various semiconducting polymers, including the active layers of all-polymer bulk heterojunction solar cells as well as barrier coatings. As part of these demonstrations, we show how floating polymeric films can be transferred easily to diverse substrates, including those with rough and irregular surfaces, such as textiles and fabrics.
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