Browsing by Author "Wang, S."
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- ItemA diuranium carbide cluster stabilized inside a C80 fullerene cage(London : Nature Publishing Group, 2018) Zhang, X.; Li, W.; Feng, L.; Chen, X.; Hansen, A.; Grimme, S.; Fortier, S.; Sergentu, D.-C.; Duignan, T.J.; Autschbach, J.; Wang, S.; Wang, Y.; Velkos, G.; Popov, A.A.; Aghdassi, N.; Duhm, S.; Li, X.; Li, J.; Echegoyen, L.; Schwarz, W.H.E.; Chen, N.Unsupported non-bridged uranium-carbon double bonds have long been sought after in actinide chemistry as fundamental synthetic targets in the study of actinide-ligand multiple bonding. Here we report that, utilizing I h(7)-C80 fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@I h(7)-C80. This endohedral fullerene was prepared utilizing the Krätschmer-Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (NiII-OEP) to produce UCU@I h(7)-C80·[NiII-OEP] as single crystals. X-ray diffraction analysis reveals a cage-stabilized, carbide-bridged, bent UCU cluster with unexpectedly short uranium-carbon distances (2.03 Å) indicative of covalent U=C double-bond character. The quantum-chemical results suggest that both U atoms in the UCU unit have formal oxidation state of +5. The structural features of UCU@I h(7)-C80 and the covalent nature of the U(f1)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.
- ItemExperimental Observation of Dirac Nodal Links in Centrosymmetric Semimetal TiB2(College Park, MD : American Physical Society, 2018) Liu, Z.; Lou, R.; Guo, P.; Wang, Q.; Sun, S.; Li, C.; Thirupathaiah, S.; Fedorov, A.; Shen, D.; Liu, K.; Lei, H.; Wang, S.The topological nodal-line semimetal state, serving as a fertile ground for various topological quantum phases, where a topological insulator, Dirac semimetal, or Weyl semimetal can be realized when the certain protecting symmetry is broken, has only been experimentally studied in very few materials. In contrast to discrete nodes, nodal lines with rich topological configurations can lead to more unusual transport phenomena. Utilizing angle-resolved photoemission spectroscopy and first-principles calculations, here, we provide compelling evidence of nodal-line fermions in centrosymmetric semimetal TiB2 with a negligible spin-orbit coupling effect. With the band crossings just below the Fermi energy, two groups of Dirac nodal rings are clearly observed without any interference from other bands, one surrounding the Brillouin zone (BZ) corner in the horizontal mirror plane σh and the other surrounding the BZ center in the vertical mirror plane σv. The linear dispersions forming Dirac nodal rings are as wide as 2 eV. We further observe that the two groups of nodal rings link together along the Γ-K direction, composing a nodal-link configuration. The simple electronic structure with Dirac nodal links mainly constituting the Fermi surfaces suggests TiB2 as a remarkable platform for studying and applying the novel physical properties related to nodal-line fermions.
- ItemExperimental strategies for optical pump - Soft x-ray probe experiments at the LCLS(Bristol : Institute of Physics Publishing, 2014) McFarland, B.K.; Berrah, N.; Bostedt, C.; Bozek, J.; Bucksbaum, P.H.; Castagna, J.C.; Coffee, R.N.; Cryan, J.P.; Fang, L.; Farrell, J.P.; Feifel, R.; Gaffney, K.J.; Glownia, J.M.; Martinez, T.J.; Miyabe, S.; Mucke, M.; Murphy, B.; Natan, A.; Osipov, T.; Petrovic, V.S.; Schorb, S.; Schultz, T.; Spector, L.S.; Swiggers, M.; Tarantelli, F.; Tenney, I.; Wang, S.; White, J.L.; White, W.; Gühr, M.Free electron laser (FEL) based x-ray sources show great promise for use in ultrafast molecular studies due to the short pulse durations and site/element sensitivity in this spectral range. However, the self amplified spontaneous emission (SASE) process mostly used in FELs is intrinsically noisy resulting in highly fluctuating beam parameters. Additionally timing synchronization of optical and FEL sources adds delay jitter in pump-probe experiments. We show how we mitigate the effects of source noise for the case of ultrafast molecular spectroscopy of the nucleobase thymine. Using binning and resorting techniques allows us to increase time and spectral resolution. In addition, choosing observables independent of noisy beam parameters enhances the signal fidelity.
- ItemThe influence of Arctic amplification on mid-latitude summer circulation([London] : Nature Publishing Group UK, 2018) Coumou, D.; Di Capua, G.; Vavrus, S.; Wang, L.; Wang, S.Accelerated warming in the Arctic, as compared to the rest of the globe, might have profound impacts on mid-latitude weather. Most studies analyzing Arctic links to mid-latitude weather focused on winter, yet recent summers have seen strong reductions in sea-ice extent and snow cover, a weakened equator-to-pole thermal gradient and associated weakening of the mid-latitude circulation. We review the scientific evidence behind three leading hypotheses on the influence of Arctic changes on mid-latitude summer weather: Weakened storm tracks, shifted jet streams, and amplified quasi-stationary waves. We show that interactions between Arctic teleconnections and other remote and regional feedback processes could lead to more persistent hot-dry extremes in the mid-latitudes. The exact nature of these non-linear interactions is not well quantified but they provide potential high-impact risks for society.
- ItemProbing nucleobase photoprotection with soft x-rays(Les Ulis : EDP Sciences, 2013) McFarland, B.K.; Farrell, J.P.; Berrah, N.; Bostedt, C.; Bozek, J.; Bucksbaum, P.H.; Coffee, R.; Cryan, J.; Fang, L.; Feifel, R.; Gaffney, K.; Glownia, J.; Martinez, T.; Mucke, M.; Murphy, B.; Miyabe, S.; Natan, A.; Osipov, T.; Petrovic, V.; Schorb, S.; Schultz, T.; Spector, L.; Tarantelli, F.; Tenney, I.; Wang, S.; White, W.; White, J.; Gühr, M.Nucleobases absorb strongly in the ultraviolet region, leading to molecular excitation into reactive states. The molecules avoid the photoreactions by funnelling the electronic energy into less reactive states on an ultrafast timescale via non-Born-Oppenheimer dynamics. Current theory on the nucleobase thymine discusses two conflicting pathways for the photoprotective dynamics. We present our first results of our free electron laser based UV-pump soft x-ray-probe study of the photoprotection mechanism of thymine. We use the high spatial sensitivity of the Auger electrons emitted after the soft x-ray pulse induced core ionization. Our transient spetra show two timescales on the order of 200 fs and 5 ps, in agreement with previous (all UV) ultrafast experiments. The timescales appear at different Auger kinetic energies which will help us to decipher the molecular dynamics.