Adopting self-healing, robust, and stretchable materials is a promising method to enable next-generation wearable electronic devices, touch screens, and soft robotics. Both elasticity and self-healing are important qualities for substrate materials as they comprise the majority of device components. However, most autonomous self-healing materials reported to date have poor elastic properties, i.e., they possess only modest mechanical strength and recoverability. Here, a substrate material designed is reported based on a combination of dynamic metal-coordinated bonds (β-diketone-europium interaction) and hydrogen bonds together in a multiphase separated network. Importantly, this material is able to undergo self-healing and exhibits excellent elasticity. The polymer network forms a microphase-separated structure and exhibits a high stress at break (≈1.8 MPa) and high fracture strain (≈900%). Additionally, it is observed that the substrate can achieve up to 98% self-healing efficiency after 48 h at 25 °C, without the need of any external stimuli. A stretchable and self-healable dielectric layer is fabricated with a dual-dynamic bonding polymer system and self-healable conductive layers are created using polymer as a matrix for a silver composite. These materials are employed to prepare capacitive sensors to demonstrate a stretchable and self-healable touch pad.

Applying the density matrix renormalization group (DRMG) method to a nonempirical valence bond (VB) model Hamiltonian, we studied polyacene oligomers of different lengths in the strong electron correlation limit. Geometrical optimizations were performed for the lowest singlet and triplet states of oligomers up to [40]-acene, and a convergence of the bond lengths toward the polymer limit is observed in the interior of the oligomer. For large oligomers, as well as for the polymer, the ground state can be reasonably determined to be a singlet. Furthermore, a high similarity between the singlet geometries and triplet geometries suggests an open-shell character for the singlet ground state. A reasonable speculation of the soliton-antisoliton pair character of the singlet ground state was supported by a spin distribution analysis of the triplet state wave function of large oligomers, with each of the two solitons being broadly delocalized over the upper or bottom edge of the oligomers, respectively.

The hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) play an important role in hydrogenbased energy conversion. Recently, the frustrating performance in alkaline media raised debates on the relevant mechanism, especially on the role of surface hydroxyl (OH * ). We present a full pH range electrode/electrolyte kinetics simulation for HER/HOR on Pt (111), with the potential-related rate constants been calculated with density functional theory methods. The polarization curves agree well with the experimental observations. The stability of OH * is found to be unlikely an effective activity descriptor since it is irrelevant to the onset potential of HOR/HER. Degree of rate control analyses reveal that the alkaline current is controlled jointly by Tafel and Volmer steps, while the acidic current solely by Tafel step, which explains the observed pH-dependent kinetics. Therefore, it is also possible to reduce the overpotential of alkaline HER/HOR by accelerating the Tafel step besides tuning the hydrogen binding energy. arXiv:1912.01152v1 [cond-mat.mtrl-sci]

The geometric and electronic structures of oligothiophene dications (with 6 to 12 monomers) have been revisited using the spin-unrestricted broken symmetry hybrid density functional B3LYP method. It is found that there exists a transition region of bipolaron to two-polaron structure conversion in the moderately sized oligomers, as that had been reported earlier in an AM1-CI calculation. According to our calculation, the transition region should be from hexamer to octamer. TD-DFT simulation led to a different rationalization of the experimental UV/visible spectra, which suggested the coexistence of bipolaron and two-polaron state in the transition region.

Electronic and/or vibronic coherence has been found by recent ultrafast spectroscopy experiments in many chemical, biological and material systems. This indicates that there are strong and complicated interactions between electronic states and vibration modes in realistic chemical systems. Therefore, simulations of quantum dynamics with a large number of electronic and vibrational degrees of freedom are highly desirable. Due to the efficient compression and localized representation of quantum states in the matrix-product state (MPS) formulation, time-evolution methods based on the MPS framework, which we summarily refer to as tDMRG (time-dependent density-matrix renormalization group) methods, are considered to be promising candidates to study the quantum dynamics of realistic chemical systems. In this work, we benchmark the performances of four different tDMRG methods, including global Taylor, global Krylov, local one-site and two-site time-dependent variational principle (1TDVP and 2TDVP), with a comparison to multiconfiguration time-dependent Hartree (MCTDH) and experimental results. Two typical chemical systems of internal conversion and singlet fission are investigated, one containing strong and high-order local and non-local electron-vibration couplings, the other exhibiting a continuous phonon bath. The comparison shows that the tDMRG methods (particularly, the 2TDVP method) can describe the full quantum dynamics in large chemical systems accurately and efficiently. Several key parameters in the tDMRG calculation including the truncation error threshold, time interval and ordering of local sites were also investigated to strike the balance between efficiency and accuracy of results. a) Electronic