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Summary The future of soft, conformable, and robust wearable electronics will require elastomers to provide mechanical stabilization, a soft surface to interact with human wearers, and a crucial physical barrier to protect stretchable devices from the environment. It is a difficult challenge, however, for a single elastomer to fulfill each of these needs. Here, we present an approach that fuses a membrane of poly(dimethylsiloxane) (PDMS) onto the surface of a transparent butyl rubber (T-IIR) substrate by using an organosilane-based molecular glue. The resulting membrane-interface-elastomer (MINE) structures uniquely combine the surface chemistry of PDMS with the intrinsically low gas permeability of T-IIR for the fabrication of robust stretchable devices. Our most intriguing finding, however, is that the T-IIR-PDMS interface, buried microns below the PDMS surface, exerts a remarkable influence on metal films deposited on the PDMS membrane surface from below, improving stretching and conductance performance by orders of magnitude.

The emergence of flexible and stretchable optoelectronics has motivated the development of new transparent conductive electrodes (TCEs) to replace conventional brittle indium tin oxide. For modern optoelectronics, these new TCEs should possess six key characteristics: low cost, solution-based processing; high transparency; high electrical conductivity; a smooth surface; mechanical flexibility or stretchability; and scalable, low-cost patterning methods. Among many materials currently being studied, silver nanowires (AgNWs) are one of the most promising, with studies demonstrating AgNW films and composites that exhibit each of the key requirements. However, AgNW-based TCEs reported to date typically fulfill two or three requirements at the same time, and rare are examples of TCEs that fulfill all six requirements simultaneously. Here, we present a straightforward method to fabricate AgNW/polymer composite films that meet all six requirements simultaneously. Our fabrication process embeds a AgNW network patterned using a solution-based wetting-dewetting protocol into a flexible or stretchable polymer, which is then adhered to an elastomeric poly(dimethylsiloxane) substrate. The resulting patterned AgNW/polymer films exhibit ∼85% transmittance with an average sheet resistance of ∼15 Ω/sq, a smooth surface (a root-mean-square surface roughness value of ∼22 nm), and also withstand up to 71% bending strain or 70% stretching strain. We demonstrate the use of these new TCEs in flexible and stretchable alternating current electroluminescent devices that emit light to 20% bending strain and 60% stretching strain.

We demonstrate a simple, low-cost, and green approach to deposit a microstructured coating on the silicone elastomer polydimethylsiloxane (PDMS) that can be coated with gold to produce highly stretchable and conductive films. The microstructured coating is fabricated using an aqueous emulsion of poly(vinyl acetate) (PVAc): common, commercially available white glue. The aqueous glue emulsion self-assembles on the PDMS surface to generate clustered PVAc globules, which can be conformally coated with gold. The microstructured surface provides numerous defect sites that localize strain when the structure is stretched, resulting in the initiation of numerous microcracks. As the structure is further elongated, the microcracks interact with one another, preventing long-range crack propagation and thus preserving the conduction pathway. The resistance of PDMS/glue/gold structures remains remarkably low (23 times the initial resistance) up to 65% elongation, making these structure useful as stretchable interconnects. Decreasing the concentration of the PVAc aqueous emulsion reduces the density of defect sites of the microstructure, which increases the change in resistance of the gold films with stretching. In this way, we can tune the resistance changes of the PDMS/glue/gold structures and increase their sensitivity to strain. We demonstrate the use of these structures as wearable, soft strain sensors.

The development of stretchable electronic devices that are soft and conformable has relied heavily on a single material – polydimethylsiloxane – as the elastomeric substrate. Although polydimethylsiloxane has a number of advantageous characteristics, its high gas permeability is detrimental to stretchable devices that use materials sensitive to oxygen and water vapor, such as organic semiconductors and oxidizable metals. Failing to protect these materials from atmosphere-induced decomposition leads to premature device failure; therefore, it is imperative to develop elastomers with gas barrier properties that enable stretchable electronics with practical lifetimes. Here, we reinvent butyl rubber – a material with an intrinsically low gas permeability traditionally used in the innerliners of tires to maintain air pressure – for stretchable electronics. This new material is smooth and optically transparent, possesses the low gas permeability typical of butyl rubber, and vastly outperforms polydimethylsiloxane as an encapsulating barrier to prevent the atmospheric degradation of sensitive electronic materials and the premature failure of functioning organic devices. The merits of transparent butyl rubber presented here position this material as an important counterpart to polydimethylsiloxane that will enable future generation stretchable electronics.

Transparent butyl rubber is a new elastomer that has the potential to revolutionize stretchable electronics due to its intrinsically low gas permeability. Encapsulating organic electronic materials and devices with transparent butyl rubber protects them from problematic degradation due to oxygen and moisture, preventing premature device failure and enabling the fabrication of stretchable organic electronic devices with practical lifetimes. Here, we report a methodology to alter the surface chemistry of transparent butyl rubber to advance this material from acting as a simple device encapsulant to functioning as a substrate primed for direct device fabrication on its surface. We demonstrate a combination of plasma and chemical treatment to deposit a hydrophilic silicate layer on the transparent butyl rubber surface to create a new layered composite that combines Si-OH surface chemistry with the favorable gas-barrier properties of bulk transparent butyl rubber. We demonstrate that these surface Si-OH groups react with organosilanes to form self-assembled monolayers necessary for the deposition of electronic materials, and furthermore demonstrate the fabrication of stretchable gold wires using nanotransfer printing of gold films onto transparent butyl rubber modified with a thiol-terminated self-assembled monolayer. The surface modification of transparent butyl rubber establishes this material as an important new elastomer for stretchable electronics and opens the way to robust, stretchable devices.

We demonstrate films of single-walled carbon nanotubes (SWNTs) on the elastomer polydimethylsiloxane (PDMS) that are stretchable, conductive, and transparent. Our fabrication method uses the supramolecular functionalization of SWNTs with conjugated polyelectrolytes to generate aqueous dispersions of positively- and negatively-charged SWNTs, followed by layer-by-layer self-assembly onto a PDMS substrate. Adding bilayers of positively- and negatively-charged SWNTs to the surface causes the sheet resistance and the % transmittance of the film to both progressively decrease. The sheet resistance decreases sharply in the first five bilayers as the layer-by-layer process efficiently establishes the percolation network, whereas the % transmittance declines more gradually. Films with 25 bilayers are transparent (75% at 550 nm) and conductive (560 ± 90 ohms/sq). The combination of electrostatic and pi-stacking forces very effectively bind the SWNTs within the film, producing smooth film surfaces (root-mean-square roughness of 18 nm) and enabling the films to remain conductive up to 80% elongation. We demonstrate the use of the SWNT films as transparent conductive electrodes in light-emitting devices and as soft strain sensors that are both wearable and transparent.

We present new flexible, transparent, and conductive coatings composed of an annealed silver nanowire network embedded in a polyurethane optical adhesive. These coatings can be applied to rigid glass substrates as well as to flexible polyethylene terephthalate (PET) plastic and elastomeric polydimethylsiloxane (PDMS) substrates to produce highly flexible transparent conductive electrodes. The coatings are as conductive and transparent as indium tin oxide (ITO) films on glass, but they remain conductive at high bending strains and are more durable to marring and scratching than ITO. Coatings on PDMS withstand up to 76% tensile strain and 250 bending cycles of 15% strain with a negligible increase in electrical resistance. Since the silver nanowire network is embedded at the surface of the optical adhesive, these coatings also provide a smooth surface (root mean squared surface roughness

Remarkable progress in stretchable electronics over the past few years has produced some amazing devices: Devices that can be laminated onto skin, [ 1 ] hemispherical arrays of photodetectors that mimic the human retina, [ 2 ] and arrays of light-emitting devices for use in fldisplays [ 3 ] are just a few examples. The methodology used to impart stretchability connects rigid circuit elements with stretchable conductive interconnects that absorb applied strain. [ 4 ] A different approach to stretchability is now emerging, in which the devices themselves are fabricated to be intrinsically stretchable. Here, we describe the use of a stretchable electroluminescent material to produce a light-emitting device that exhibits intrinsic stretchability at room temperature. These devices are well-suited to new applications in stretchable and conformable lighting that require uniform, diffuse light emission over large areas. We demonstrate devices with large emission areas ( ∼ 20‐175 mm 2 ) that tolerate linear strains up to 27% and repetitive cycles of 15% strain with minimal performance degradation relative to devices fabricated using a conventional electroluminescent material. There are few examples of intrinsically stretchable devices‐ that is, systems in which the device itself operates under tensile strain. The two strategies that have been used to impart stretchability to these devices are identical to those used to fabricate stretchable device interconnects: Device materials can be either dispersed into an elastomeric matrix or deposited onto a prestretched elastomeric substrate. Kaltenbrunner et al. used the fi rst strategy to produce a stretchable battery of gel materials encased in an elastomer that can withstand uniaxial strains up