Rubbery electronics and sensors from intrinsically

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SCIENCE ADVANCES RESEARCH ARTICLE, Downloaded from http advances sciencemag org on September 13 2020. Fig 1 Intrinsically stretchable electronic materials A Schematic illustrations of a sensor upper and a TFT lower consisting of AuNP AgNW conductors P3HT. NF PDMS semiconductor composite and ion gel dielectric vertically stacked on a PDMS substrate B Schematic illustrations upper and SEM images lower of the. AgNWs before left and after right the galvanic replacement process to conformally coat AuNPs on exposed AgNWs C Sheet resistance ohms of the AuNP. AgNW PDMS conductor under different levels of mechanical strain The SEM images of the stretched conductor are shown at the bottom D AFM surface topography. left and phase mode right images of the P3HT NF PDMS film E AFM phase mode images of P3HT NF PDMS coated on a PDMS substrate upon uniaxial stretching Yellow. arrows indicate P3HT NF rupture F Photographs of the P3HT NF PDMS film on a thin PDMS substrate under various forms of mechanical deformation G Photographs of. free standing ion gel dielectric before and after stretching. to form AuNP AgNW 29 Comparison studies in transistor charac percolated nanofibrils in a rubber matrix This process not only forms. teristics are described to further emphasize the necessity of developing percolated pathways for the carriers to transport but also results in. these conductors The detailed electrode preparation process is presented P3HT NFs that significantly improve crystallinity and therefore en. in Materials and Methods Figure 1B shows the schematic illustrations hance the carrier mobility as detailed in previous studies 22 23 30. of the AgNW before upper left and after upper right AuNP con Specifically P3HT was first dissolved in the m xylene solvent at 60 C. formal coating Note that only the exposed AgNWs will be coated with fig S2A bright orange and then cooled down and kept for 10 min. AuNPs Scanning electron microscopy SEM images of AgNWs before at 20 C to form P3HT NF fig S2A dark purple Transmission elec. bottom left and after bottom right conformal AuNP coating indicate tron microscopy TEM and atomic force microscopy AFM images. the success of the galvanic replacement process fig S1 We performed of the prepared P3HT NF indicate that the diameter and length of. stretching tests to examine the electrical characteristic change associated P3HT NF are 40 nm and 1 5 mm respectively fig S2 The P3HT NF. with the applied mechanical strain Specifically the AuNP AgNW solution was blended with a solvent m xylene diluted PDMS 10 1. PDMS electrode can be elastically stretched and its sheet resistance w w prepolymer curing agent to allow thorough mixing A thin film. increases from 2 to 5 ohms upon 50 uniaxial stretching as shown P3HT NF PDMS stretchable semiconductor is achieved by spin. in Fig 1C upper The SEM images in Fig 1C lower revealed that no coating followed by solidifying at 60 C We obtained the optimized. obvious crack was observed weight composition of P3HT through systematic studies of the per. The stretchable elastomeric composite semiconductor is prepared colation behaviors morphologies and their electrical characteristics. by two major sequential steps i forming the one dimensional self fig S3 The P3HT PDMS weight ratio of 2 8 was chosen owing to the. assembled p conjugated P3HT NFs in the solvent under a cooling absence of microcracks and a moderate decrease in mobilities as shown. process and ii blending the resulting P3HT NFs with PDMS to yield in fig S4 We carried out AFM scanning to examine the microstructures. Kim et al Sci Adv 2017 3 e1701114 8 September 2017 2 of 8. SCIENCE ADVANCES RESEARCH ARTICLE, of the nanofibrils and the detailed surface morphology of the P3HT with a semiconductor from pristine P3HT and PDMS p P3HT. NF PDMS thin film spin coated on a PDMS substrate The left AFM PDMS composite on Au electrodes as a comparison The TFTs from. image in Fig 1D with a scanning area of 1 mm 1 mm shows the surface p P3HT PDMS and P3HT NF PDMS composite showed mFE of 4 5. topography of the film The right AFM image in Fig 1D under phase 10 3 and 1 3 cm2 V s and ION OFF of 1 68 102 and 3 82 102 respec. mode illustrates the stiffness contrast between P3HT NFs 0 3 GPa tively Details are illustrated in fig S9 Compared to p P3HT P3HT NFs. 31 and PDMS 1 MPa 32 The schematic illustration in fig S2E obtained through p conjugation of the thiophene rings yielded more. shows how the P3HT NFs behave upon stretching at different extent efficient carrier transport and better device performance These results. The P3HT NFs first straighten and then eventually start to rupture are also consistent with the reported P3HT NF based devices 33. which can be seen from the AFM images in Fig 1E As the yellow arrows To examine the transistor performances under mechanical strain. indicate some P3HT NFs rupture when stretched up to or beyond 50 the characteristics of the fabricated TFT were measured while different. Nevertheless majorities of the P3HT NFs remain connected at 50 levels of mechanical strain were applied using a custom made stretcher. Owing to the composite merits of elastomeric mechanical properties The strain was applied both along and perpendicular to the channel. from the elastomer PDMS and the electrical conductance from the length directions Because the TFT was constructed fully with elastomeric. percolated P3HT NFs the P3HT NF PDMS can be stretched or twisted materials whose moduli are comparable and thus with no significant. and return to its original state without any cracks as shown in Fig 1F strain isolation effect 34 35 the stretching strain applied is assumed. The stretchable ion gel dielectric was prepared by the solution casting to be evenly distributed across the whole device Figure 2 F and G. method The detailed preparation can be found in Materials and Methods shows the transfer curves of the TFTs under 10 30 and 50 mechanical. Downloaded from http advances sciencemag org on September 13 2020. The composite shows relatively stable electrical conductivity even after strain along and perpendicular to the channel length directions respec. exposure in the environment 25 C 75 relative humidity for 600 hours tively More detailed results are shown in fig S10 On the basis of the. fig S5 No obvious crack of the membrane was observed when it was linear regime of these transfer curves the m and threshold voltage Vth. stretched by 50 as shown in Fig 1G of the TFTs under different levels of mechanical strain were calculated. see the Supplementary Materials for details, Intrinsically stretchable rubbery transistors On one hand once the TFT was stretched by up to 50 along the chan. We constructed stretchable ion gel gated TFTs by using these intrinsi nel length direction a moderate decrease in m from 1 4 to 0 8 cm2 V s. cally stretchable electronic materials based on solution processes includ and a slight increase in Vth from 2 56 to 2 45 V were obtained Fig 2H. ing spin casting and stencil printing Figure 2A shows the schematic On the other hand once it was stretched by up to 50 perpendicular to. structure of an ion gel gated TFT Specifically the source and drain the channel length direction a relatively larger decrease in m from 1 4 to. AuNP AgNW PDMS electrodes and P3HT NF PDMS composite semi 0 4 cm2 V s and a slight decrease in Vth from 2 56 to 2 61 V were. conductor layer were patterned with a thin Kapton film based stencil obtained Fig 2I Note that owing to the gating effect the TFT experiences. masks which were generated by a cutting machine Silhouette Cameo less decrease in the channel current upon mechanical stretching com. A 140 mm thick ion gel film was aligned and laminated on the source pared with the devices without a gate such as strain sensors as de. and drain electrodes to serve as ion gated dielectric The detailed fabrica scribed below A similar phenomenon has been reported elsewhere 36. tion process is described in Materials and Methods and fig S6 Figure 2 B All these results suggest that the intrinsically stretchable rubbery tran. and C shows a photograph of fabricated TFT and an SEM image showing sistors can maintain normal operation and relatively stable device per. a channel length of 50 mm respectively The width of the channel was formances while undergoing large mechanical stretching. 5 mm The thicknesses of the P3HT NF PDMS composite semiconductor. and TFT were measured to be 280 nm and 430 mm respectively fig S7 Strain pressure and temperature sensors. To verify the necessity and feasibility of AuNP AgNW PDMS Various sensors such as strain pressure and temperature sensors were. electrodes for the intrinsically stretchable rubbery TFT we tested exploited by using intrinsically stretchable electronic materials Figure 3A. several different electrodes and carefully examined their corresponding shows a schematic illustration of a strain sensor with a two terminal. characteristics Specifically we constructed TFTs and tested electron configuration in which a P3HT NF PDMS stretchable semiconductor. beam evaporated Au and Ag electrodes and AgNW PDMS and is connected at both ends with AuNP AgNW PDMS electrodes The. AuNP AgNW PDMS based electrodes Only Au electrodes and length and width of the channel were 50 mm and 5 mm respectively. AuNP AgNW PDMS based TFTs showed transistor characteristics The thickness of the P3HT NF PDMS stretchable semiconductor was. The comparison results are presented in fig S8 The results suggest that 100 nm The device was fabricated in a way similar to that of the tran. only Au or AuNP AgNW can form an ohmic contact with the P3HT sistor Figure 3B presents a series of images of a device stretched from 0. NF PDMS and the Ag film or AgNW cannot 28 to 50 Upon stretching the electrical resistance increases Figure. Figure 2D shows the transfer Ids VG and corresponding jI ds j 2 VG. 3C shows the plot of the measured electrical resistance versus the. curves of the stretchable ion gated TFT without any mechanical mechanical strain from 0 to 50 for both directions When the ap. stretching The drain current was obtained while the gate voltage VG plied strain was along the channel length direction the resistance. was swept from 0 to 4 V with the drain voltage kept at 0 5 V The increased from 0 3 to 4 6 gigohms and an approximately linear increase. ION OFF was calculated to be 5 6 103 which is comparable to other of resistance was obtained upon mechanical stretching Note that the. P3HT NF based stretchable TFTs 23 Figure 2E shows the source increase of resistance was mainly attributed to the semiconductor rather. drain IDS VDS characteristics of the TFT with a gate voltage decrease than to the conductor The conductor contributes negligibly as exhibited. from 1 5 to 4 V at a voltage step of 0 5 V The drain voltage was in Fig 1C compared with the overall resistance increase. decreased from 0 to 0 5 V The drain current was as high as 0 35 mA When the applied strain was perpendicular to the channel length. at VG 4 V and VDS 0 5 V direction a much smaller increase in resistance from 0 3 to 0 64 gigohms. To verify that the TFTs from P3HT NF PDMS composite semi was observed Cyclic mechanical stretching and releasing of the strain. conductor can offer enhanced device performance we construct TFTs sensor under a cyclic mechanical tester CK 700FET CKSI Co Ltd. Kim et al Sci Adv 2017 3 e1701114 8 September 2017 3 of 8. SCIENCE ADVANCES RESEARCH ARTICLE, Downloaded from http advances sciencemag org on September 13 2020. Fig 2 Intrinsically stretchable rubbery transistors A Exploded schematic illustration of the rubbery TFT B Photograph of the TFT C SEM image of the source. drain electrodes and channel of the TFT D and E Transfer and output curves of the TFT without any mechanical strain F and G Transfer curves of the TFTs under. different levels of mechanical strain along and perpendicular to the channel length directions H and I mFE and Vth of the TFTs under different levels of mechanical. strain along and perpendicular to the channel length directions. were performed to evaluate the stability of the sensor The stretching strain sensors that can be directly stretched to a similar extent such. increased from 0 to 50 with a step increase of 10 along the channel as 50 37 38. length direction Figure 3D shows the normalized electrical resistance A similar two terminal device configuration was adopted for pres. during cyclic stretching and releasing at a rate of 1 Hz These results sure sensors because the applied pressure induces semiconductor de. agree with the measured resistance change as shown in Fig 3C The forming which results in resistance change Specifically relative electrical. inset in Fig 3D shows a magnified resistance change of the sensor at resistance R Ro was consecutively measured by applying different. 30 cyclic stretching and stable and repetitive response was achieved Hertzian contact pressures see the Supplementary Materials for details. The calculated gauge factor GF defined as the ratio between the rela As shown in Fig 3F the applied pressure ranges from 0 66 to 1 2 MPa. tive resistance change DR Ro and the extent of mechanical stretching and the resistance changes accordingly With an increase of the ap. is shown in Fig 3E A GF of 33 is achieved for the 50 stretching Note plied Hertzian pressure from 0 66 to 1 2 MPa the R Ro increases from. that this GF value is the highest to our best knowledge compared with 0 98 to 3 3 The change of R Ro corresponding to different applied. GF values of other organic material and inorganic material based pressures is plotted in Fig 3G The near hysteresis less characteristic. Rubbery electronics and sensors from intrinsically stretchable elastomeric composites of semiconductors and conductors Hae Jin Kim 1 Kyoseung Sim 2 Anish Thukral 1 Cunjiang Yu1 2 3 4 A general strategy to impart mechanical stretchability to stretchable electronics involves engineering materials into special architectures to accommodate or eliminate the mechanical strain in nonstretchable

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