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Publisher: [London] : Nature Publishing Group UK × Subject: lattice dynamics ×

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    Control of coordinatively unsaturated Zr sites in ZrO2 for efficient C–H bond activation
    ([London] : Nature Publishing Group UK, 2018) Zhang, Yaoyuan; Zhao, Yun; Otroshchenko, Tatiana; Lund, Henrik; Pohl, Marga-Martina; Rodemerck, Uwe; Linke, David; Jiao, Haijun; Jiang, Guiyuan; Kondratenko, Evgenii V.
    Due to the complexity of heterogeneous catalysts, identification of active sites and the ways for their experimental design are not inherently straightforward but important for tailored catalyst preparation. The present study reveals the active sites for efficient C–H bond activation in C1–C4 alkanes over ZrO2 free of any metals or metal oxides usually catalysing this reaction. Quantum chemical calculations suggest that two Zr cations located at an oxygen vacancy are responsible for the homolytic C–H bond dissociation. This pathway differs from that reported for other metal oxides used for alkane activation, where metal cation and neighbouring lattice oxygen form the active site. The concentration of anion vacancies in ZrO2 can be controlled through adjusting the crystallite size. Accordingly designed ZrO2 shows industrially relevant activity and durability in non-oxidative propane dehydrogenation and performs superior to state-of-the-art catalysts possessing Pt, CrOx, GaOx or VOx species.
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    Topological protection versus degree of entanglement of two-photon light in photonic topological insulators
    ([London] : Nature Publishing Group UK, 2021) Tschernig, Konrad; Jimenez-Galán, Álvaro; Christodoulides, Demetrios N.; Ivanov, Misha; Busch, Kurt; Bandres, Miguel A.; Perez-Leija, Armando
    Topological insulators combine insulating properties in the bulk with scattering-free transport along edges, supporting dissipationless unidirectional energy and information flow even in the presence of defects and disorder. The feasibility of engineering quantum Hamiltonians with photonic tools, combined with the availability of entangled photons, raises the intriguing possibility of employing topologically protected entangled states in optical quantum computing and information processing. However, while two-photon states built as a product of two topologically protected single-photon states inherit full protection from their single-photon “parents”, a high degree of non-separability may lead to rapid deterioration of the two-photon states after propagation through disorder. In this work, we identify physical mechanisms which contribute to the vulnerability of entangled states in topological photonic lattices. Further, we show that in order to maximize entanglement without sacrificing topological protection, the joint spectral correlation map of two-photon states must fit inside a well-defined topological window of protection.