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Despite the development throughout human history of a wealth of textile materials and structures, the porous structures and non-planar surfaces of textiles are often viewed as problematic for the fabrication of wearable e-textiles and smart clothing. Here, we demonstrate a new textile-centric design paradigm in which we use the textile structure as an integral part of wearable device design. We coat the open framework structure of an ultrasheer knitted textile with a conformal gold film using solution-based metallization to form gold-coated ultrasheer electrodes that are highly conductive (3.6 ± 0.9 Ω/sq) and retain conductivity to 200% strain with R/R0 < 2. The ultrasheer electrodes produce wearable, highly stretchable light-emitting e-textiles that function to 200% strain. Stencil printing a wax resist provides patterned electrodes for patterned light emission; furthermore, incorporating soft-contact lamination produces light-emitting textiles that exhibit, for the first time, readily changeable patterns of illumination.

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.

Light-emitting electrochemical cells (LECs) are simple electroluminescent devices comprising an emissive material containing mobile ions sandwiched between two electrodes. The operating mechanism of the LEC involves both ionic and electronic transport, distinguishing it from its more well-known cousin, the organic light-emitting diode (OLED). While OLEDs have become a leading player in commercial displays, LECs have flourished in academic research due to the simple device architecture and unique features of its operating mechanism, inviting exploration of new materials and fabrication strategies. These explorations have brought LECs to an exciting frontier in advanced optoelectronics: flexible and stretchable light-emitting devices. Flexible and stretchable LECs are discussed herein, presenting the LEC system as a robust and fault-tolerant development platform. The engineering of emissive composites is highlighted to control mechanical properties, and how the tolerance of LECs to electrode work function and roughness has enabled the incorporation of new electrode materials to achieve flexibility and stretchability. As part of this story, the solution processability of LECs has led to exciting demonstrations of flexible and printed LECs. An outlook is provided for LECs that builds on these strengths, potentially leading to flexible, stretchable, low-cost devices such as illuminated tags, smart packaging, flexible signage, and wearable illumination.

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.

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