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Creators/Authors contains: "Ke, Jun"

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  1. Electron-doped cuprates consistently exhibit strong antiferromagnetic correlations, leading to the prevalent belief that antiferromagnetic spin fluctuations mediate Cooper pairing in these unconventional superconductors. However, early investigations showed that although antiferromagnetic spin fluctuations create the largest pseudogap at hot spots in momentum space, the superconducting gap is also maximized at these locations. This presented a paradox for spin-fluctuation-mediated pairing: Cooper pairing is strongest at momenta where the normal-state low-energy spectral weight is most suppressed. Here we investigate this paradox and find evidence that a gossamer—meaning very faint—Fermi surface can provide an explanation for these observations. We study Nd2–xCexCuO4 using angle-resolved photoemission spectroscopy and directly observe the Bogoliubov quasiparticles. First, we resolve the previously observed reconstructed main band and the states gapped by the antiferromagnetic pseudogap around the hot spots. Within the antiferromagnetic pseudogap, we also observe gossamer states with distinct dispersion, from which coherence peaks of Bogoliubov quasiparticles emerge below the superconducting critical temperature. Moreover, the direct observation of a Bogoliubov quasiparticle permits an accurate determination of the superconducting gap, yielding a maximum value an order of magnitude smaller than the pseudogap, establishing the distinct nature of these two gaps. We propose that orientation fluctuations in the antiferromagnetic order parameter are responsible for the gossamer states. 
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  2. Recent progress on stretchable, tough dual-dynamic polymer single networks (SN) and interpenetrated networks (IPN) has broadened the potential applications of dynamic polymers. However, the impact of macromolecular structure on the material mechanics remains poorly understood. Here, rapidly exchanging hydrogen bonds and thermoresponsive Diels–Alder bonds were included into molecularly engineered interpenetrated network materials. RAFT polymerization was used to make well-defined polymers with control over macromolecular architecture. The IPN materials were assessed by gel permeation chromatography, differential scanning calorimetry, tensile testing and rheology. The mechanical properties of these IPN materials can be tuned by varying the crosslinker content and chain length. All materials are elastic and have dynamic behavior at both ambient temperature and elevated temperature (90 °C), owing to the presence of the dual dynamic noncovalent and covalent bonds. 100% self-healing recovery was achieved and a maximum stress level of up to 6 MPa was obtained. The data suggested the material's healing properties are inversely proportional to the content of the crosslinker or the degree of polymerization at both room and elevated temperature. The thermoresponsive crosslinker restricted deformation to some extent in an ambient environment but gave excellent malleability upon heating. The underlying mechanism was explored by the computational simulations. Furthermore, a single network material with the same crosslinker content and degree of polymerization as the IPN was made. The SN was substantially weaker than the comparable IPN material. 
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  3. Transiently crosslinked dynamic polymer networks are developed, using carbodiimide hydration to link carboxylic acids as anhydrides. From aqueous polymer solutions, non-equilibrium hydrogels are transiently formed, which dissolve upon anhydride hydrolysis. The materials can be refueled using a subsequent injection of carbodiimide. The gels exhibit higher storage moduli compared to transient supramolecular gels as a result of their covalent crosslinks. 
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