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- ItemNear-real-time monitoring of global CO2 emissions reveals the effects of the COVID-19 pandemic([London] : Nature Publishing Group UK, 2020) Liu, Zhu; Ciais, Philippe; Deng, Zhu; Lei, Ruixue; Davis, Steven J.; Feng, Sha; Zheng, Bo; Cui, Duo; Dou, Xinyu; Zhu, Biqing; Guo, Rui; Ke, Piyu; Sun, Taochun; Lu, Chenxi; He, Pan; Wang, Yuan; Yue, Xu; Wang, Yilong; Lei, Yadong; Zhou, Hao; Cai, Zhaonan; Wu, Yuhui; Guo, Runtao; Han, Tingxuan; Xue, Jinjun; Boucher, Olivier; Boucher, Eulalie; Chevallier, Frédéric; Tanaka, Katsumasa; Wei, Yiming; Zhong, Haiwang; Kang, Chongqing; Zhang, Ning; Chen, Bin; Xi, Fengming; Liu, Miaomiao; Bréon, François-Marie; Lu, Yonglong; Zhang, Qiang; Guan, Dabo; Gong, Peng; Kammen, Daniel M.; He, Kebin; Schellnhuber, Hans JoachimThe COVID-19 pandemic is impacting human activities, and in turn energy use and carbon dioxide (CO2) emissions. Here we present daily estimates of country-level CO2 emissions for different sectors based on near-real-time activity data. The key result is an abrupt 8.8% decrease in global CO2 emissions (−1551 Mt CO2) in the first half of 2020 compared to the same period in 2019. The magnitude of this decrease is larger than during previous economic downturns or World War II. The timing of emissions decreases corresponds to lockdown measures in each country. By July 1st, the pandemic’s effects on global emissions diminished as lockdown restrictions relaxed and some economic activities restarted, especially in China and several European countries, but substantial differences persist between countries, with continuing emission declines in the U.S. where coronavirus cases are still increasing substantially.
- ItemControl 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.
- ItemAnharmonic strong-coupling effects at the origin of the charge density wave in CsV3Sb5([London] : Nature Publishing Group UK, 2024) He, Ge; Peis, Leander; Cuddy, Emma Frances; Zhao, Zhen; Li, Dong; Zhang, Yuhang; Stumberger, Romona; Moritz, Brian; Yang, Haitao; Gao, Hongjun; Devereaux, Thomas Peter; Hackl, RudiThe formation of charge density waves is a long-standing open problem, particularly in dimensions higher than one. Various observations in the vanadium antimonides discovered recently further underpin this notion. Here, we study the Kagome metal CsV3Sb5 using polarized inelastic light scattering and density functional theory calculations. We observe a significant gap anisotropy with 2Δmax/kBTCDW≈20, far beyond the prediction of mean-field theory. The analysis of the A1g and E2g phonons, including those emerging below TCDW, indicates strong phonon-phonon coupling, presumably mediated by a strong electron-phonon interaction. Similarly, the asymmetric Fano-type lineshape of the A1g amplitude mode suggests strong electron-phonon coupling below TCDW. The large electronic gap, the enhanced anharmonic phonon-phonon coupling, and the Fano shape of the amplitude mode combined are more supportive of a strong-coupling phonon-driven charge density wave transition than of a Fermi surface instability or an exotic mechanism in CsV3Sb5.
- ItemFew-femtosecond passage of conical intersections in the benzene cation([London] : Nature Publishing Group UK, 2017) Galbraith, M.C.E.; Scheit, S.; Golubev, N.V.; Reitsma, G.; Zhavoronkov, N.; Despré, V.; Lépine, F.; Kuleff, A.I.; Vrakking, M.J.J.; Kornilov, O.; Köppel, H.; Mikosch, J.Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system - the excited benzene cation. We use few-femtosecond duration extreme ultraviolet and visible/near-infrared laser pulses to prepare and probe excited cationic states and observe two relaxation timescales of 11 ± 3 fs and 110 ± 20 fs. These are interpreted in terms of population transfer via two sequential conical intersections. The experimental results are quantitatively compared with state-of-the-art multi-configuration time-dependent Hartree calculations showing convincing agreement in the timescales. By characterising one of the fastest internal conversion processes studied to date, we enter an extreme regime of ultrafast molecular dynamics, paving the way to tracking and controlling purely electronic dynamics in complex molecules.