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Precise determination of structural organization of semi-conducting polymers is of paramount importance for the further development of these materials in organic electronic technologies. Yet, prior characterization of some of the best-performing materials for transistor and photovoltaic applications, which are based on polymers with rigid backbones, often resulted in conundrums in which X-ray scattering and microscopy yielded seemingly contradicting results. Here we solve the paradox by introducing a new structural model, i.e. , semi-paracrystalline organization. The model establishes that the microstructure of these materials relies on a dense array of small paracrystalline domains embedded in a more disordered matrix. Thus, the overall structural order relies on two parameters: the novel concept of degree of paracrystallinity ( i.e. , paracrystalline volume/mass fraction, introduced here for the first time) and the lattice distortion parameter of paracrystalline domains ( g -parameter from X-ray scattering). Structural parameters of the model are correlated with long-range charge carrier transport, revealing that charge transport in semi-paracrystalline materials is particularly sensitive to the interconnection of paracrystalline domains. 

Abstract A charge density wave (CDW) represents an exotic state in which electrons are arranged in a long‐range ordered pattern in low‐dimensional materials. Although the understanding of the fundamental character of CDW is enriched after extensive studies, its practical application remains limited. Here, an unprecedented demonstration of a tunable charge‐spin interconversion (CSI) in graphene/1T‐TaS₂van der Waals heterostructures is shown by manipulating the distinct CDW phases in 1T‐TaS₂. Whereas CSI from spins polarized in all three directions is observed in the heterostructure when the CDW phase does not show commensurability, the output of one of the components disappears, and the other two are enhanced when the CDW phase becomes commensurate. The experimental observation is supported by first‐principles calculations, which evidence that chiral CDW multidomains in the heterostructure are at the origin of the switching of CSI. The results uncover a new approach for on‐demand CSI in low‐dimensional systems, paving the way for advanced spin‐orbitronic devices.