Electron-electron interactions can render an otherwise conducting material insulating, with the insulator-metal phase transition in correlated-electron materials being the canonical macroscopic manifestation of the competition between charge-carrier itinerancy and localization. The transition can arise from underlying microscopic interactions among the charge, lattice, orbital and spin degrees of freedom, the complexity of which leads to multiple phase-transition pathways. For example, in many transition metal oxides, the insulator-metal transition has been achieved with external stimuli, including temperature, light, electric field, mechanical strain or magnetic field. Vanadium dioxide is particularly intriguing because both the lattice and on-site Coulomb repulsion contribute to the insulator-to-metal transition at 340 K (ref. 8). Thus, although the precise microscopic origin of the phase transition remains elusive, vanadium dioxide serves as a testbed for correlated-electron phase-transition dynamics. Here we report the observation of an insulator-metal transition in vanadium dioxide induced by a terahertz electric field. This is achieved using metamaterial-enhanced picosecond, high-field terahertz pulses to reduce the Coulomb-induced potential barrier for carrier transport. A nonlinear metamaterial response is observed through the phase transition, demonstrating that high-field terahertz pulses provide alternative pathways to induce collective electronic and structural rearrangements. The metamaterial resonators play a dual role, providing sub-wavelength field enhancement that locally drives the nonlinear response, and global sensitivity to the local changes, thereby enabling macroscopic observation of the dynamics. This methodology provides a powerful platform to investigate low-energy dynamics in condensed matter and, further, demonstrates that integration of metamaterials with complex matter is a viable pathway to realize functional nonlinear electromagnetic composites.
A new synthetic route to poly-3,4-ethylenedioxythiophene (PEDT) with a conductivity exceeding 1000 S/cm is described. The method is based on base-inhibited vapor-phase polymerization, where a surface covered with ferric p-toluenesulfonate as oxidant mixed with a volatile base (pyridine) is exposed to 3,4-ethylenedioxythiophene (EDT) vapors. The base is added to suppress an acid-initiated polymerization of EDT, leading to a product with little or no conjugation. The product of the base-inhibited vapor-phase polymerization is confirmed to be virtually identical to PEDT obtained by wet chemical oxidation by both spectroscopic and electrochemical methods. A possible reaction scheme for the acid-initiated polymerization is discussed.
We show that the main mechanism for the dc voltage or dc current induced insulator-metal transition in vanadium dioxide VO(2) is due to local Joule heating and not a purely electronic effect. This "tour de force" experiment was accomplished by using the fluorescence spectra of rare-earth doped micron sized particles as local temperature sensors. As the insulator-metal transition is induced by a dc voltage or dc current, the local temperature reaches the transition temperature indicating that Joule heating plays a predominant role. This has critical implications for the understanding of the dc voltage or dc current induced insulator-metal transition and has a direct impact on applications which use dc voltage or dc current to externally drive the transition.
Conducting polymers expand or contract when their redox state is changed. This expansion/contraction effect can be separated in an intrinsic part because of changes of the polymer backbone on reduction/oxidation and a part depending on the surrounding electrolyte phase, because of osmotic expansion of the polymer phase. The osmotic effect causes solvent molecules to move into the polymer in a number far in excess of those bound strongly in the solvation shell of the mobile ion, resulting in large volume changes. In this paper, a thermodynamic description of the osmotic expansion is worked out. The model is compared with measurements on PPy(DBS) films. The experiments show that the expansion decreases as the electrolyte concentration is increased. This means that a considerable part of the total expansion is due to the osmotic effect. The osmotic effect should be taken into account when interpreting and designing actuator experiments and when comparing experimental results from different sources.
A highly elastic and stretchable conductive polymer material resulted from blending the conductive polymer poly(3,4‐ethylenedioxythiophene):p‐tosylate and an aliphatic polyurethane elastomer. The blend inherited advantageous properties from its constituents, namely high conductivity of 120 S cm–1 from its conductive polymer component, and elastomeric mechanical properties resembling those of the polyurethane, including good adhesion to various substrates. Stretching of the blend material by up to 50 % resulted in increased conductivity, while subsequent relaxation to the unstretched state caused a decrease of conductivity compared to the pristine blend. These initial changes in conductivity were reproducible on further cycling between 50 % stretching and the unstretched state for at least 10 cycles. Stretching beyond 50 % resulted in decreasing conductivity of the blend but with substantial conductivity remaining even when stretched by 200 %. Optical, mechanical, and thermal properties of the blend, as well as high resolution electron microscopy of bulk cross‐sections, suggest that the system is a single phase and not two separate phases. Ageing experiments indicate that the material retains substantial conductivity for at least a few years at room temperature.
Recently Armstrong and Bruce' reported a layered modification of lithium manganese oxide, LiMnO7, isostructural with LiCoO2. LiMnO1 obtained by ion exchange from ct-NaMnO1 synthesized in air is characterized by x-ray diffraction and by electrochemical insertion and extraction of lithium in a series of voltage ranges between 1.5 and 4.5 V relative to a lithium electrode. During cycling, voltage plateaus at 3.0 and 4.0 V vs. Li develop, indicating that the material is converted from its original layered structure to a spinel structure. This finding is confirmed by x-ray diffraction. Contrary to expectations based on thermodynamics, insertion of larger amounts of lithium leads to a more complete conversion. We suggest that a relatively high mobility of manganese leaves Li and Mn randomly distributed in the close-packed oxygen lattice after a deep discharge. This isotropic Mn distribution can relatively easily relax to the Mn distribution characteristic of spinels whereas the anisotropic distribution characteristic of layered structures is not reformed when excess lithium is extracted.
A soft polymer actuator has been constructed based on the volume change of a conducting polymer. The linear expansion (12 % at a load of 0.5 MPa) is the highest yet reported for a centimeter‐scale conducting polymer actuator. This is achieved by controlling the structure on several length scales: Choice of molecular structure, synthesis from a structured medium, and forming the polymer actuator on a compliant, microstructured gold electrode.
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