Influence of Side Chain Interdigitation on Strain and Charge Mobility of Planar Indacenodithiophene Copolymers
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Anisotropic Phonon Response of Few-Layer PdSe 2 under Uniaxial Strain
PdSe 2 , an emerging 2D material with a novel anisotropic puckered pentagonal structure, has attracted growing interest due to its layer-dependent electronic bandgap, high carrier mobility, and good air stability. In this work, a detailed Raman spectroscopic study of few-layer PdSe 2 (two to five layers) under the in-plane uniaxial tensile strain up to 3.33% is performed. Two of the prominent PdSe 2 Raman peaks are influenced differently depending on the direction of strain application. Additionally, the A g 1 mode redshifts more than the A g 3 mode when the strain is applied along the a -axis of the crystal, while the A g 3 mode redshifts more than the A g 1 mode when the strain is applied along the b -axis. Such an anisotropic phonon response to strain indicates directionally dependent mechanical and thermal properties of PdSe 2 and also allows the identification of the crystal axes. The results are further supported using first-principles density-functional theory. Interestingly, the near-zero Poisson’s ratios for few-layer PdSe 2 are found, suggesting that the uniaxial tensile strain can easily be applied to few-layer PdSe 2 without significantly altering their dimensions at the perpendicular directions, which is a major contributing factor to the observed distinct phonon behavior. The findings pave the way for further development of 2D PdSe 2 -based flexible electronics.
36 MATERIALS SCIENCE↗
Tunneling Barrier-Integrated Gold Nanofilms for Negative Strain Gauging with Near-Zero Energy Consumption
Wireless strain sensors with minimal power needs are essential for long-term monitoring in energy-limited environments. We present a soft tunneling barrier-integrated gold thin film for negative strain sensing with near-zero energy consumption. The device features a strain-induced transition from an insulating to a metallic state, increasing conductivity by 9 orders of magnitude under a controlled strain. It consists of Au-PDMS-Au nanofilm layers, where the Au structures are near the percolation threshold and the PDMS layer acts as a tunneling barrier. Under strain, thinning due to the Poisson effect lowers the barrier’s potential height, enabling electron tunneling and forming an electrical path. Further, with a standby power consumption of ~10 –5 mW over 10 6 times lower than conventional sensors (~12.5 mW), this device is ideal for real-time, long-term stationary structural monitoring in multiple locations.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Comparing the Effects of Side Chain Dipole–Dipole Interactions and Hydrogen Bonding on the Mechanical and Electrical Properties of Poly(3-hexylthiophene)
Poly(3-alkylthiophenes) are simple conjugated polymers with good electrical properties, but tend to be brittle, limiting their application. Here, we investigate how side chain modifications can improve their toughness without compromising their charge transport. Specifically, we compare a weak dipole–dipole interaction of ester groups with a stronger hydrogen-bonding interaction of the hydroxyl groups. Two copolymers with targeted 5 and 10 mol % ester-functionalized side chains were synthesized and hydrolyzed in the solid state to introduce hydroxyl groups. Both hydrolyzed polymers became insoluble in most organic solvents, providing a path to layer-by-layer solution processing. All polymers’ optical, thermal, structural, electrical, and mechanical properties were investigated. Optical spectroscopy revealed that functionalization at these low levels did not significantly affect aggregation or π–π stacking. Differential scanning calorimetry indicated reduced crystallinity in the functionalized copolymers compared to that of P3HT. Grazing-incidence wide-angle X-ray diffraction data showed that functionalization led to an increase in lamellar spacing without altering molecular orientation or π–π stacking. Mechanical testing highlighted that at the lower functionalization level, both ester and hydroxyl groups similarly enhanced toughness, suggesting that disorder, rather than the specific nature of the functional group, was responsible for these improvements. At the higher functionalization level, hydroxyl groups significantly increased the elastic modulus while also negatively impacting charge carrier mobility. This study suggests that with stronger hydrogen-bonding groups, only very small amounts can improve P3HT’s toughness. For a wider tunable range, it may be a better strategy to use weak interactions such as dipole–dipole interactions of ester groups.
36 MATERIALS SCIENCE↗
Directly Probing the Fracture Behavior of Ultrathin Polymeric Films
Understanding fracture mechanics of ultrathin polymeric films is crucial for modern technologies, including semiconductor and coating industries. However, up to now, the fracture behavior of sub-100 nm polymeric thin films is rarely explored due to challenges in handling samples and limited testing methods available. In this work, we report a new testing methodology that can not only visualize the evolution of the local stress distribution through wrinkling patterns and crack propagation during the deformation of ultrathin films but also directly measure their fracture energies. Using ultrathin polystyrene films as a model system, we both experimentally and computationally investigate the effect of the film thickness and molecular weight on their fracture behavior, both of which show a ductile-to-brittle transition. Furthermore, we demonstrate the broad applicability of this testing method in semicrystalline semiconducting polymers. We anticipate our methodology described here could provide new ways of studying the fracture behavior of ultrathin films under confinement.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Recent Trends and Innovation in Additive Manufacturing of Soft Functional Materials
The growing demand for wearable devices, soft robotics, and tissue engineering in recent years has led to an increased effort in the field of soft materials. With the advent of personalized devices, the one-shape-fits-all manufacturing methods may soon no longer be the standard for the rapidly increasing market of soft devices. Recent findings have pushed technology and materials in the area of additive manufacturing (AM) as an alternative fabrication method for soft functional devices, taking geometrical designs and functionality to greater heights. For this reason, this review aims to highlights recent development and advances in AM processable soft materials with self-healing, shape memory, electronic, chromic or any combination of these functional properties. Furthermore, the influence of AM on the mechanical and physical properties on the functionality of these materials is expanded upon. Additionally, advances in soft devices in the fields of soft robotics, biomaterials, sensors, energy harvesters, and optoelectronics are discussed. Lastly, current challenges in AM for soft functional materials and future trends are discussed.
36 MATERIALS SCIENCE↗