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DOE OSTI2018

Flexible Electronics: Stretchable Electrodes and Their Future

Flexible electronics, as an emerging and exciting research field, have brought great interest to the issue of how to make flexible electronic materials that offer both durability and high performance at strained states. With the advent of on-body wearable and implantable electronics, as well as increasing demands for human-friendly intelligent soft robots, enormous effort is being expended on highly flexible functional materials, especially stretchable electrodes, by both the academic and industrial communities. Among different deformation modes, stretchability is the most demanding and challenging. This review focuses on the latest advances in stretchable transparent electrodes based on a new design strategy known as kirigami (the art of paper cutting) and investigates the recent progress on novel applications, including skin-like electronics, implantable biodegradable devices, and bioinspired soft robotics. By comparing the optoelectrical and mechanical properties of different electrode materials, some of the most important outcomes with comments on their merits and demerits are raised. Key design considerations in terms of geometries, substrates, and adhesion are also discussed, offering insights into the universal strategies for engineering stretchable electrodes regardless of the material. Finally, it is suggested that highly stretchable and biocompatible electrodes will greatly boost the development of next-generation intelligent life-like electronics.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Self–Healing and Stretchable Molecular Ferroelectrics with High Expandability

The interplay between crystal ordering and stretchability is frequently encountered in contemporary materials science, particularly in the case of ferroelectrics. The inherent dilemma arises when these materials need to withstand repetitive mechanical deformations or stretching without sacrificing their crystal integrity, all while retaining their remarkable ferroelectric properties and even exhibiting self-healing capabilities. This complexity further presents a significant challenge in the design and engineering of mechanically rigid molecular ferroelectric crystals, particularly for applications where both precise crystalline structure and mechanical adaptability are crucial. In this study, the humidity-controlled expansion and contraction, dissolution, and recrystallization of a self-assembled molecular ferroelectric-in-hydrogel framework are reported. Self-healing ferroelectric-in-hydrogel networks exhibit a recyclable humidity-tailored ionic conductivity from 2.86 × 10 –6 to 1.36 × 10 –5 S cm –1 , facilitating the stretchable piezoelectric sensing. Additionally, the dynamic bond reforming interactions are observed, leading to the tailoring of Young's modulus from 452 to 170 MPa, maintaining ferroelectricity under a strain of 20% with a piezoelectric coefficient of 15.7 pC N –1 . Upon lattice contraction, the molecular contacts undergo reforming, leading to the restoration of stretchable ferroelectrics/piezoelectrics and paving the way for stretchable bioelectronics for full-body motion monitoring. The capabilities highlighted here open avenues for stretchable and self-healing ferroelectric-in-hydrogel bioelectronic technologies.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Surface Energy Modulated Self‐Assembly of Percolative Gallium Nanodroplet Films for Stretchable Electronics

Advancements in soft robotics and wearable technologies have led to an increased need for flexible and stretchable electronic systems. Liquid metals like Gallium (Ga) and its alloys offer high potential in the field of stretchable electronics and photonics due to their inherent high conductivity and malleability. However, their high surface tension and native oxide formation hinder uniform wetting and continuous film formation to get conducting films. Here, we report a fabrication strategy to realize electrically conductive Ga thin films with effective thicknesses around 100 nm on polymeric and elastomeric substrates. By enhancing the surface energy of the elastomer, we create uniform Ga nanodroplets capable of sustaining stretchability up to 200% strain. Our devices exhibit electronic conduction primarily through tunneling and display strain tunable piezoresistive characteristics, which are explained using Kirchhoff's resistive network and Simmon's analytical tunneling current model. To showcase the device's capability in fields of stretchable electronics, we demonstrate several functional prototypes, including flexible devices integrated with Light Emitting Diodes (LEDs), curvature and pressure sensors, and soft robotic grippers capable of sensing object curvature. The demonstrated devices highlight the potential of this approach for scalable integration of stretchable electronics in soft robotic and wearable platforms.

42 ENGINEERING↗

DOE OSTI2016

All-Printed, Stretchable Zn-Ag 2 O Rechargeable Battery via Hyperelastic Binder for Self-Powering Wearable Electronics

While several stretchable batteries utilizing either deterministic or random composite architectures have been described, none have been fabricated using inexpensive printing technologies. In this study, the authors printed a highly stretchable, zinc-silver oxide (Zn-Ag 2 O) battery by incorporating polystyrene-block-polyisoprene-block-polystyrene (SIS) as a hyperelastic binder for custom-made printable inks. The remarkable mechanical properties of the SIS binder lead to an all-printed, stretchable Zn-Ag 2 O rechargeable battery with a ≈2.5 mA h cm -2 reversible capacity density even after multiple iterations of 100% stretching. This battery offers the highest reversible capacity and discharge current density for intrinsically stretchable batteries reported to date. The electrochemical and mechanical properties are characterized under different strain conditions. The new stress-enduring printable inks pave ways for further developing stretchable electronics for the wide range of wearable applications.

25 ENERGY STORAGE↗

DOE OSTI2017

A highly stretchable, transparent, and conductive polymer

Previous breakthroughs in stretchable electronics stem from strain engineering and nanocomposite approaches. Routes toward intrinsically stretchable molecular materials remain scarce but, if successful, will enable simpler fabrication processes, such as direct printing and coating, mechanically robust devices, and more intimate contact with objects. We report a highly stretchable conducting polymer, realized with a range of enhancers that serve a dual function: (i) they change morphology and (ii) they act as conductivity-enhancing dopants in poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). The polymer films exhibit conductivities comparable to the best reported values for PEDOT:PSS, with over 3100 S/cm under 0% strain and over 4100 S/cm under 100% strain—among the highest for reported stretchable conductors. It is highly durable under cyclic loading, with the conductivity maintained at 3600 S/cm even after 1000 cycles to 100% strain. The conductivity remained above 100 S/cm under 600% strain, with a fracture strain of 800%, which is superior to even the best silver nanowire– or carbon nanotube–based stretchable conductor films. As a result, the combination of excellent electrical and mechanical properties allowed it to serve as interconnects for field-effect transistor arrays with a device density that is five times higher than typical lithographically patterned wavy interconnects.

36 MATERIALS SCIENCE↗

DOE OSTI2020

F4‐TCNQ as an Additive to Impart Stretchable Semiconductors with High Mobility and Stability

Abstract Numerous strategies are developed to impart stretchability to polymer semiconductors. Although these methods improve the ductility, mobility, and stability of such stretchable semiconductors, they nonetheless still need further improvement. Here, it is shown that 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4‐TCNQ) is an effective molecular additive to tune the properties of a diketopyrrolopyrrole‐based (DPP‐based) semiconductor. Specifically, the addition of F4‐TCNQ is observed to improve the ductility of the semiconductor by altering the polymer’s microstructures and dynamic motions. As a p‐type dopant additive, F4‐TCNQ can also effectively enhance the mobility and stability of the semiconductor through changing the host polymer’s packing structures and charge trap passivation. Upon fabricating fully stretchable transistors with F4‐TCNQ‐DPP blended semiconductor films, it is observed that the resulting stretchable transistors possess one of the highest initial mobility of 1.03 cm 2 V −1 s −1 . The fabricated transistors also exhibit higher stability (both bias and environmental) and mobility retention under repeated strain, compared to those without F4‐TCNQ additive. These findings offer a new direction of research on stretchable semiconductors to facilitate future practical applications.

Mun, Jaewan↗

DOE OSTI2019

Fully embedded CuNWs/PDMS conductor with high oxidation resistance and high conductivity for stretchable electronics

Currently, copper nanowires (CuNWs) based conductors have been considered as a promising candidate in the area of stretchable electronics. But the fast degradation of CuNWs in ambient conditions largely limited their practical applications. Here, the author reports a highly conductive, stable, and stretchable conductor with CuNWs fully embedded in the surface layer of poly(dimethylsiloxane) (PDMS), which not only exhibit superb stability against oxidation, but also possess good conductivity. In the fully embedded conductor, PDMS protects the CuNWs from oxidation and increases the mechanical robustness of CuNWs networks at the same time. The stretchable conductor could maintain a low sheet resistance even after 1000 cycles of stretching under 30% of strain. In addition, fully embedded CuNWs/PDMS conductors have excellent oxidation stability even in high humidity and high temperature environments (85 °C, 85 % RH). Stretchable dipole antenna was fabricated using the fully embeded CuNWs/PDMS conductors, which could retain its sensitivity to specific radio frequencies even after 500 cycles of the stretching/releasing process. At the same time, a stretchable conductive heater was demonstrated, verifying the applicability of our fully embedded conductor. We believe that this work could opens new opportunities for CuNW-based conductor into broad practical applications.

Zhang, Bowen (ORCID:000000030432745X)↗

DOE OSTI2020

Elastic Single-Ion Conducting Polymer Electrolytes: Toward a Versatile Approach for Intrinsically Stretchable Functional Polymers

Fabrication of stretchable functional polymeric materials usually relies on the physical adhesion between functional components and elastic polymers, while the interfacial resistance is a potential problem. Herein, a versatile approach on the molecular-level intrinsically stretchable polymer materials with defined functionality is reported. The single-ion conducting polymer electrolytes (SICPEs) were employed to demonstrate the proposed concept along with its potential application in stretchable batteries/electronics with improved energy efficiency and prolonged cell lifetime. The obtained membranes exhibit 88–252% elongation before breaking, and the mechanical properties are well adjustable. The galvanostatic test of the assembled cells using the obtained SICPE membrane exhibited a good cycling performance with a capacity retention of 81.5% after 100 cycles. The applicability of a proposed molecular-level design for intrinsically stretchable polymer materials is further demonstrated in other types of stretchable functional materials, including poly(vinylcarbazole)-based semiconducting polymers and poly(ethylene glycol)-based gas separation membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Intrinsically stretchable and healable semiconducting polymer for organic transistors

Developing a molecular design paradigm for conjugated polymers applicable to intrinsically stretchable semiconductors is crucial toward the next generation of wearable electronics. Current molecular design rules for high charge carrier mobility semiconducting polymers are unable to render the fabricated devices simultaneously stretchable and mechanically robust. Here in this paper, we present a new design concept to address the above challenge, while maintaining excellent electronic performance. This concept involves introducing chemical moieties to promote dynamic non-covalent crosslinking of the conjugated polymers. These non-covalent covalent crosslinking moieties are able to undergo an energy dissipation mechanism through breakage of bonds when strain is applied, while retaining its high charge transport ability. As a result, our polymer is able to recover its high mobility performance (>1 cm 2 /Vs) even after 100 cycles at 100% applied strain. Furthermore, we observed that the polymer can be efficiently repaired and/or healed with a simple heat and solvent treatment. These improved mechanical properties of our fabricated stretchable semiconductor enabled us to fabricate highly stretchable and high performance wearable organic transistors. This material design concept should illuminate and advance the pathways for future development of fully stretchable and healable skin-inspired wearable electronics.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Fully stretchable active-matrix organic light-emitting electrochemical cell array

Intrinsically and fully stretchable active-matrix-driven displays are an important element to skin electronics that can be applied to many emerging fields, such as wearable electronics, consumer electronics and biomedical devices. Here, we show for the first time a fully stretchable active-matrix-driven organic light-emitting electrochemical cell array. Briefly, it is comprised of a stretchable light-emitting electrochemical cell array driven by a solution-processed, vertically integrated stretchable organic thin-film transistor active-matrix, which is enabled by the development of chemically-orthogonal and intrinsically stretchable dielectric materials. Our resulting active-matrix-driven organic light-emitting electrochemical cell array can be readily bent, twisted and stretched without affecting its device performance. When mounted on skin, the array can tolerate to repeated cycles at 30% strain. This work demonstrates the feasibility of skin-applicable displays and lays the foundation for further materials development.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Achieving tissue-level softness on stretchable electronics through a generalizable soft interlayer design

Soft and stretchable electronics have emerged as highly promising tools for biomedical diagnosis and biological studies, as they interface intimately with the human body and other biological systems. Most stretchable electronic materials and devices, however, still have Young’s moduli orders of magnitude higher than soft bio-tissues, which limit their conformability and long-term biocompatibility. Here, we present a design strategy of soft interlayer for allowing the use of existing stretchable materials of relatively high moduli to versatilely realize stretchable devices with ultralow tissue-level moduli. We have demonstrated stretchable transistor arrays and active-matrix circuits with moduli below 10 kPa—over two orders of magnitude lower than the current state of the art. Benefiting from the increased conformability to irregular and dynamic surfaces, the ultrasoft device created with the soft interlayer design realizes electrophysiological recording on an isolated heart with high adaptability, spatial stability, and minimal influence on ventricle pressure. In vivo biocompatibility tests also demonstrate the benefit of suppressing foreign-body responses for long-term implantation. With its general applicability to diverse materials and devices, this soft-interlayer design overcomes the material-level limitation for imparting tissue-level softness to a variety of bioelectronic devices.

42 ENGINEERING↗

DOE OSTI2017

Highly stretchable polymer semiconductor films through the nanoconfinement effect

Soft and conformable wearable electronics require stretchable semiconductors, but existing ones typically sacrifice charge transport mobility to achieve stretchability. We explore a concept based on the nanoconfinement of polymers to substantially improve the stretchability of polymer semiconductors, without affecting charge transport mobility. The increased polymer chain dynamics under nanoconfinement significantly reduces the modulus of the conjugated polymer and largely delays the onset of crack formation under strain. As a result, our fabricated semiconducting film can be stretched up to 100% strain without affecting mobility, retaining values comparable to that of amorphous silicon. The fully stretchable transistors exhibit high biaxial stretchability with minimal change in on current even when poked with a sharp object. Lastly, we demonstrate a skinlike finger-wearable driver for a light-emitting diode.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Self-similar and fractal design for stretchable electronics

The present invention provides electronic circuits, devices and device components including one or more stretchable components, such as stretchable electrical interconnects, electrodes and/or semiconductor components. Stretchability of some of the present systems is achieved via a materials level integration of stretchable metallic or semiconducting structures with soft, elastomeric materials in a configuration allowing for elastic deformations to occur in a repeatable and well-defined way. The stretchable device geometries and hard-soft materials integration approaches of the invention provide a combination of advance electronic function and compliant mechanics supporting a broad range of device applications including sensing, actuation, power storage and communications.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Hyperelastic binder for printed, stretchable electronics

Disclosed are compositions, devices, systems and fabrication methods for stretchable composite materials and stretchable electronics devices. In some aspects, an elastic composite material for a stretchable electronics device includes a first material having a particular electrical, mechanical or optical property; and a multi-block copolymer configured to form a hyperelastic binder that creates contact between the first material and the multi-block copolymer, in which the elastic composite material is structured to stretch at least 500% in at least one direction of the material and to exhibit the particular electrical, mechanical or optical property imparted from the first material. In some aspects, the stretchable electronics device includes a stretchable battery, biofuel cell, sensor, supercapacitor or other device able to be mounted to skin, clothing or other surface of a user or object.

42 ENGINEERING↗

DOE OSTI2019

Self-similar and fractal design for stretchable electronics

Rogers, John A.↗

DOE OSTI2019

Controlled buckling structures in semiconductor interconnects and nanomembranes for stretchable electronics

In an aspect, the present invention provides stretchable, and optionally printable, components such as semiconductors and electronic circuits capable of providing good performance when stretched, compressed, flexed or otherwise deformed, and related methods of making or tuning such stretchable components. Stretchable semiconductors and electronic circuits preferred for some applications are flexible, in addition to being stretchable, and thus are capable of significant elongation, flexing, bending or other deformation along one or more axes. Further, stretchable semiconductors and electronic circuits of the present invention are adapted to a wide range of device configurations to provide fully flexible electronic and optoelectronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Hyperelastic binder for printed, stretchable electronics

Wang, Joseph↗

DOE OSTI2019

An Intrinsically Stretchable High-Performance Polymer Semiconductor with Low Crystallinity

For wearable and implantable electronics applications, developing intrinsically stretchable polymer semiconductor is advantageous, especially in the manufacturing of large-area and high-density devices. A prime challenge is to simultaneously achieve good electrical and mechanical properties for these semiconductor devices. Although crystalline domains are generally needed to achieve high mobility, amorphous domains are necessary to impart stretchability. Recent progresses in the design of high-performance donor–acceptor polymers that exhibit low degrees of energetic disorder, while having a high fraction of amorphous domains, appear promising for polymer semiconductors. Here, a low crystalline, i.e., near-amorphous, indacenodithiophene-co-benzothiadiazole (IDTBT) polymer and a semicrystalline thieno[3,2-b]thiophene-diketopyrrolopyrrole (DPPTT) are compared, for mechanical properties and electrical performance under strain. It is observed that IDTBT is able to achieve both a high modulus and high fracture strain, and to preserve electrical functionality under high strain. Next, fully stretchable transistors are fabricated using the IDTBT polymer and observed mobility ≈0.6 cm 2 V -1 s -1 at 100% strain along stretching direction. In addition, the morphological evolution of the stretched IDTBT films is investigated by polarized UV-vis and grazing-incidence X-ray diffraction to elucidate the molecular origins of high ductility. In summary, the near-amorphous IDTBT polymer signifies a promising direction regarding molecular design principles toward intrinsically stretchable high-performance polymer semiconductor.

36 MATERIALS SCIENCE↗