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| 2. |
- Canton, Sophie, et al.
(författare)
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Toward Highlighting the Ultrafast Electron Transfer Dynamics at the Optically Dark Sites of Photocatalysts
- 2013
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Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 4:11, s. 1972-1976
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Tidskriftsartikel (refereegranskat)abstract
- Building a detailed understanding of the structure function relationship is a crucial step in the optimization of molecular photocatalysts employed in water splitting schemes. The optically dark nature of their active sites usually prevents a complete mapping of the photoinduced dynamics. In this work, transient X-ray absorption spectroscopy highlights the electronic and geometric changes that affect such a center in a bimetallic model complex. Upon selective excitation of the ruthenium chromophore, the cobalt moiety is reduced through intramolecular electron transfer and undergoes a spin flip accompanied by an average bond elongation of 0.20 +/- 0.03 angstrom. The analysis is supported by simulations based on density functional theory structures (B3LYP*/TZVP) and FEFF 9.0 multiple scattering calculations. More generally, these results exemplify the large potential of the technique for tracking elusive intermediates that impart unique functionalities in photochemical devices.
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| 3. |
- Canton, Sophie, et al.
(författare)
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Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses.
- 2015
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 6
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Tidskriftsartikel (refereegranskat)abstract
- Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor-acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.
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| 4. |
- Fransson, Claes, et al.
(författare)
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Late spectral evolution of the ejecta and reverse shock in SN 1987a
- 2013
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Ingår i: Astrophysical Journal. - 0004-637X .- 1538-4357. ; 768:1, s. 88-
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Tidskriftsartikel (refereegranskat)abstract
- We present observations with the Very Large Telescope and Hubble Space Telescope (HST) of the broad emission lines from the inner ejecta and reverse shock of SN 1987A from 1999 February until 2012 January (days 4381-9100 after explosion). We detect broad lines from H alpha, H beta, Mg I], Na I, [O I], [Ca II], and a feature at similar to 9220 angstrom. We identify the latter line with Mg II lambda lambda 9218, 9244, which is most likely pumped by Ly alpha fluorescence. H alpha and H beta both have a centrally peaked component extending to similar to 4500 km s(-1) and a very broad component extending to greater than or similar to 11,000 km s(-1), while the other lines have only the central component. The low-velocity component comes from unshocked ejecta, heated mainly by X-rays from the circumstellar environment, whereas the very broad component comes from faster ejecta passing through the reverse shock, created by the collision with the circumstellar ring. The flux in H alpha from the reverse shock has increased by a factor of four to six from 2000 to 2007. After that there is a tendency of flattening of the light curve, similar to what may be seen in the optical lines from the shocked ring. The core component seen in H alpha, [Ca II], and Mg II has experienced a similar increase, which is consistent with that found from HST photometry. The energy deposition of the external X-rays is calculated using explosion models for SN 1987A and we predict that the outer parts of the unshocked ejecta will continue to brighten because of this. The external X-ray illumination also explains the edge-brightened morphology of the ejecta seen in the HST images. We finally discuss evidence for dust in the ejecta from line asymmetries.
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| 5. |
- Gröningsson, Per, et al.
(författare)
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High resolution spectroscopy of the inner ring of SN 1987A
- 2008
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Ingår i: Astronomy and Astrophysics. - : EDP Sciences. - 0004-6361 .- 1432-0746. ; 479:3, s. 761-777
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Tidskriftsartikel (refereegranskat)abstract
- We discuss high resolution VLT/UVES observations (FWHM similar to 6 kms(-1)) from October 2002 (day similar to 5700 past explosion) of the shock interaction of SN 1987A and its circumstellar ring. A large number of narrow emission lines from the unshocked ring, with ion stages from neutral up to Ne V and Fe VII, have been identified. A nebular analysis of the narrow lines from the unshocked gas indicates gas densities of (similar to 1.5 - 5.0) x 10(3) cm(-3) and temperatures of similar to 6.5 x 10(3) - 2.4 x 104 K. This is consistent with the thermal widths of the lines. From the shocked component we observe a large range of ionization stages from neutral lines to [FeXIV]. From a nebular analysis we find that the density in the low ionization region is 4 x 10(6) - 10(7) cm-3. There is a clear difference in the high velocity extension of the low ionization lines and that of lines from [Fe X - XIV], with the latter extending up to similar to- 390 km s(-1) in the blue wing for [Fe XIV], while the low ionization lines extend to typically similar to- 260 km s(-1). For H alpha a faint extension up to similar to- 450 km s(-1) can be seen probably arising from a small fraction of shocked high density clumps. We discuss these observations in the context of radiative shock models, which are qualitatively consistent with the observations. A fraction of the high ionization lines may originate in gas which has yet not had time to cool, explaining the difference in width between the low and high ionization lines. The maximum shock velocities seen in the optical lines are similar to 510 km s(-1). We expect the maximum width of especially the low ionization lines to increase with time.
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| 6. |
- Gröningsson, Per, et al.
(författare)
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High resolution spectroscopy of the line emission from the inner circumstellar ring of SN 1987A and its hot spots
- 2007
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Rapport (övrigt vetenskapligt/konstnärligt)abstract
- We discuss high resolution VLT/UVES observations (FWHM ~ 6 km/s) from October 2002 (day ~5700 past explosion) of the shock interaction of SN 1987A and its circumstellar ring. A nebular analysis of the narrow lines from the unshocked gas indicates gas densities of (1.5-5.0)E3 cm-3 and temperatures of 6.5E3-2.4E4 K. This is consistent with the thermal widths of the lines. From the shocked component we observe a large range of ionization stages from neutral lines to [Fe XIV]. From a nebular analysis we find that the density in the low ionization region is 4E6-1E7 cm-3. There is a clear difference in the high velocity extension of the low ionization lines and that of lines from [Fe X-XIV], with the latter extending up to ~ -390 km/s in the blue wing for [Fe XIV], while the low ionization lines extend to typically ~ -260 km/s. For H-alpha a faint extension up to ~ -450 km/s can be seen probably arising from a small fraction of shocked high density clumps. We discuss these observations in the context of radiative shock models, which are qualitatively consistent with the observations. A fraction of the high ionization lines may originate in gas which has yet not had time to cool down, explaining the difference in width between the low and high ionization lines. The maximum shock velocities seen in the optical lines are ~ 510 km/s. We expect the maximum width of especially the low ionization lines to increase with time.
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| 7. |
- Kjær, Kurt H., et al.
(författare)
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A 2-million-year-old ecosystem in Greenland uncovered by environmental DNA
- 2022
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Ingår i: Nature. - : Springer Nature. - 0028-0836 .- 1476-4687. ; 612:7939, s. 283-291
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Tidskriftsartikel (refereegranskat)abstract
- Late Pliocene and Early Pleistocene epochs 3.6 to 0.8 million years ago1 had climates resembling those forecasted under future warming2. Palaeoclimatic records show strong polar amplification with mean annual temperatures of 11–19 °C above contemporary values3,4. The biological communities inhabiting the Arctic during this time remain poorly known because fossils are rare5. Here we report an ancient environmental DNA6 (eDNA) record describing the rich plant and animal assemblages of the Kap København Formation in North Greenland, dated to around two million years ago. The record shows an open boreal forest ecosystem with mixed vegetation of poplar, birch and thuja trees, as well as a variety of Arctic and boreal shrubs and herbs, many of which had not previously been detected at the site from macrofossil and pollen records. The DNA record confirms the presence of hare and mitochondrial DNA from animals including mastodons, reindeer, rodents and geese, all ancestral to their present-day and late Pleistocene relatives. The presence of marine species including horseshoe crab and green algae support a warmer climate than today. The reconstructed ecosystem has no modern analogue. The survival of such ancient eDNA probably relates to its binding to mineral surfaces. Our findings open new areas of genetic research, demonstrating that it is possible to track the ecology and evolution of biological communities from two million years ago using ancient eDNA.
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| 8. |
- Kjær, Karina, et al.
(författare)
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SN 1987A at the end of its second decade
- 2007
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Ingår i: AIP Conference Proceedings. - : American Institute of Physics. - 0094-243X.
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Konferensbidrag (övrigt vetenskapligt/konstnärligt)
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| 9. |
- Larsson, Josefin, et al.
(författare)
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The morphology of the ejecta in supernova 1987a : A study over time and wavelength
- 2013
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Ingår i: Astrophysical Journal. - 0004-637X .- 1538-4357. ; 768:1, s. 89-
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Tidskriftsartikel (refereegranskat)abstract
- We present a study of the morphology of the ejecta in Supernova 1987A based on images and spectra from the Hubble Space Telescope (HST) as well as integral field spectroscopy from VLT/SINFONI. The HST observations were obtained between 1994 and 2011 and primarily probe the outer H-rich zones of the ejecta. The SINFONI observations were obtained in 2005 and 2011 and instead probe the [Si I]+[Fe II] emission from the inner regions. We find a strong temporal evolution of the morphology in the HST images, from a roughly elliptical shape before similar to 5000 days, to a more irregular, edge-brightened morphology with a "hole" in the middle thereafter. This transition is a natural consequence of the change in the dominant energy source powering the ejecta, from radioactive decay before similar to 5000 days to X-ray input from the circumstellar interaction thereafter. The [Si I]+[Fe II] images display a more uniform morphology, which may be due to a remaining significant contribution from radioactivity in the inner ejecta and the higher abundance of these elements in the core. Both the Ha and the [Si I]+[Fe II] line profiles show that the ejecta are distributed fairly close to the plane of the inner circumstellar ring, which is assumed to define the rotational axis of the progenitor star. The Ha emission extends to higher velocities than [Si I]+[Fe II], as expected from theoretical models. There is no clear symmetry axis for all the emission. Instead, we find that the emission is concentrated to clumps and that the emission is distributed somewhat closer to the ring in the north than in the south. This north-south asymmetry may be partially explained by dust absorption. We compare our results with explosion models and find some qualitative agreement, but note that the observations show a higher degree of large-scale asymmetry.
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| 10. |
- Marouli, Eirini, et al.
(författare)
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Rare and low-frequency coding variants alter human adult height
- 2017
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 542:7640, s. 186-190
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Tidskriftsartikel (refereegranskat)abstract
- Height is a highly heritable, classic polygenic trait with approximately 700 common associated variants identified through genome-wide association studies so far. Here, we report 83 height-associated coding variants with lower minor-allele frequencies (in the range of 0.1-4.8%) and effects of up to 2 centimetres per allele (such as those in IHH, STC2, AR and CRISPLD2), greater than ten times the average effect of common variants. In functional follow-up studies, rare height increasing alleles of STC2 (giving an increase of 1-2 centimetres per allele) compromised proteolytic inhibition of PAPP-A and increased cleavage of IGFBP-4 in vitro, resulting in higher bioavailability of insulin-like growth factors. These 83 height-associated variants overlap genes that are mutated in monogenic growth disorders and highlight new biological candidates (such as ADAMTS3, IL11RA and NOX4) and pathways (such as proteoglycan and glycosaminoglycan synthesis) involved in growth. Our results demonstrate that sufficiently large sample sizes can uncover rare and low-frequency variants of moderate-to-large effect associated with polygenic human phenotypes, and that these variants implicate relevant genes and pathways.
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