| 1. |
- Czapla-Masztafiak, Joanna, et al.
(författare)
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Investigating DNA Radiation Damage Using X-Ray Absorption Spectroscopy
- 2016
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Ingår i: Biophysical Journal. - : Elsevier BV. - 0006-3495 .- 1542-0086. ; 110:6, s. 1304-1311
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Tidskriftsartikel (refereegranskat)abstract
- The biological influence of radiation on living matter has been studied for years; however, several questions about the detailed mechanism of radiation damage formation remain largely unanswered. Among all biomolecules exposed to radiation, DNA plays an important role because any damage to its molecular structure can affect the whole cell and may lead to chromosomal rearrangements resulting in genomic instability or cell death. To identify and characterize damage induced in the DNA sugar-phosphate backbone, in this work we performed x-ray absorption spectroscopy at the P K-edge on DNA irradiated with either UVA light or protons. By combining the experimental results with theoretical calculations, we were able to establish the types and relative ratio of lesions produced by both UVA and protons around the phosphorus atoms in DNA.
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| 2. |
- Bartels-Rausch, T., et al.
(författare)
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A review of air-ice chemical and physical interactions (AICI): Liquids, quasi-liquids, and solids in snow
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:3, s. 1587-1633
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Tidskriftsartikel (refereegranskat)abstract
- Snow in the environment acts as a host to rich chemistry and provides a matrix for physical exchange of contaminants within the ecosystem. The goal of this review is to summarise the current state of knowledge of physical processes and chemical reactivity in surface snow with relevance to polar regions. It focuses on a description of impurities in distinct compartments present in surface snow, such as snow crystals, grain boundaries, crystal surfaces, and liquid parts. It emphasises the microscopic description of the ice surface and its link with the environment. Distinct differences between the disordered air-ice interface, often termed quasi-liquid layer, and a liquid phase are highlighted. The reactivity in these different compartments of surface snow is discussed using many experimental studies, simulations, and selected snow models from the molecular to the macro-scale. Although new experimental techniques have extended our knowledge of the surface properties of ice and their impact on some single reactions and processes, others occurring on, at or within snow grains remain unquantified. The presence of liquid or liquid-like compartments either due to the formation of brine or disorder at surfaces of snow crystals below the freezing point may strongly modify reaction rates. Therefore, future experiments should include a detailed characterisation of the surface properties of the ice matrices. A further point that remains largely unresolved is the distribution of impurities between the different domains of the condensed phase inside the snowpack, i.e. in the bulk solid, in liquid at the surface or trapped in confined pockets within or between grains, or at the surface. While surface-sensitive laboratory techniques may in the future help to resolve this point for equilibrium conditions, additional uncertainty for the environmental snowpack may be caused by the highly dynamic nature of the snowpack due to the fast metamorphism occurring under certain environmental conditions. Due to these gaps in knowledge the first snow chemistry models have attempted to reproduce certain processes like the long-term incorporation of volatile compounds in snow and firn or the release of reactive species from the snowpack. Although so far none of the models offers a coupled approach of physical and chemical processes or a detailed representation of the different compartments, they have successfully been used to reproduce some field experiments. A fully coupled snow chemistry and physics model remains to be developed. © Author(s) 2014.
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| 3. |
- Dey, Ananta, et al.
(författare)
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Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system
- 2024
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 15
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Tidskriftsartikel (refereegranskat)abstract
- Plasmonic systems convert light into electrical charges and heat, mediating catalytic transformations. However, there is ongoing controversy regarding the involvement of hot carriers in the catalytic process. In this study, we demonstrate the direct utilisation of plasmon hot electrons in the hydrogen evolution reaction with visible light. We intentionally assemble a plasmonic nanohybrid system comprising NiO/Au/[Co(1,10-Phenanthrolin-5-amine)2(H2O)2], which is unstable at water thermolysis temperatures. This assembly limits the plasmon thermal contribution while ensuring that hot carriers are the primary contributors to the catalytic process. By combining photoelectrocatalysis with advanced in situ spectroscopies, we can substantiate a reaction mechanism in which plasmon-induced hot electrons play a crucial role. These plasmonic hot electrons are directed into phenanthroline ligands, facilitating the rapid, concerted proton-electron transfer steps essential for hydrogen generation. The catalytic response to light modulation aligns with the distinctive profile of a hot carrier-mediated process, featuring a positive, though non-essential, heat contribution. Direct participation of plasmon-induced hot electrons in the photoelectrocatalytic synthesis of hydrogen. This report solves a long-lasting contentious issue surrounding plasmonic materials on catalytic applications.
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| 4. |
- Jay, Raphael, et al.
(författare)
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Tracking C–H activation with orbital resolution
- 2023
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 380:6648, s. 955-960
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Tidskriftsartikel (refereegranskat)abstract
- Transition metal reactivity toward carbon-hydrogen (C-H) bonds hinges on the interplay of electron donation and withdrawal at the metal center. Manipulating this reactivity in a controlled way is difficult because the hypothesized metal-alkane charge-transfer interactions are challenging to access experimentally. Using time-resolved x-ray spectroscopy, we track the charge-transfer interactions during C-H activation of octane by a cyclopentadienyl rhodium carbonyl complex. Changes in oxidation state as well as valence-orbital energies and character emerge in the data on a femtosecond to nanosecond timescale. The x-ray spectroscopic signatures reflect how alkane-to-metal donation determines metal-alkane complex stability and how metal-to-alkane back-donation facilitates C-H bond cleavage by oxidative addition. The ability to dissect charge-transfer interactions on an orbital level provides opportunities for manipulating C-H reactivity at transition metals.
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| 5. |
- Man, Gabriel, et al.
(författare)
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Electronic coupling between the unoccupied states of the organic and inorganic sublattices of methylammonium lead iodide : A hybrid organic-inorganic perovskite single crystal
- 2021
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 104:4
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Tidskriftsartikel (refereegranskat)abstract
- Organic-inorganic halide perovskites have been intensively reinvestigated due to their applications, yet the optoelectronic function of the organic cation remains unclear. Through organic-selective resonant Auger electron spectroscopy measurements on well-defined single-crystal surfaces, we find evidence for electronic coupling in the unoccupied states between the organic and inorganic sublattices of the prototypical hybrid perovskite, which is contrary to the notion based on previous studies that the organic cation is electronically inert. The coupling is relevant for electron dynamics in the material and for understanding optoelectronic functionality.
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| 6. |
- Plakhova, Tatiana V., et al.
(författare)
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Towards the surface hydroxyl species in CeO2 nanoparticles
- 2019
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Ingår i: Nanoscale. - : ROYAL SOC CHEMISTRY. - 2040-3364 .- 2040-3372. ; 11:39, s. 18142-18149
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Tidskriftsartikel (refereegranskat)abstract
- Understanding the complex chemistry of functional nanomaterials is of fundamental importance. Controlled synthesis and characterization at the atomic level is essential to gain deeper insight into the unique chemical reactivity exhibited by many nanomaterials. Cerium oxide nanoparticles have many industrial and commercial applications, resulting from very strong catalytic, pro- and anti-oxidant activity. However, the identity of the active species and the chemical mechanisms imparted by nanoceria remain elusive, impeding the further development of new applications. Here, we explore the behavior of cerium oxide nanoparticles of different sizes at different temperatures and trace the electronic structure changes by state-of-the-art soft and hard X-ray experiments combined with computational methods. We confirm the absence of the Ce(III) oxidation state at the surface of CeO2 nanoparticles, even for particles as small as 2 nm. Synchrotron X-ray absorption experiments at Ce L-3 and M-5 edges, combined with X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM) and small angle X-ray scattering (SAXS) and theoretical calculations demonstrate that in addition to the nanoceria charge stability, the formation of hydroxyl groups at the surface profoundly affects the chemical performance of these nanomaterials.
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| 7. |
- Sterling, Cody M., et al.
(författare)
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Sensitivity of Nitrogen K-Edge X-ray Absorption to Halide Substitution and Thermal Fluctuations in Methylammonium Lead-Halide Perovskites
- 2021
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 125:15, s. 8360-8368
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Tidskriftsartikel (refereegranskat)abstract
- The performance of hybrid perovskite materials in solar cells crucially depends on their electronic properties, and it is important to investigate contributions to the total electronic structure from specific components in the material. In a combined theoretical and experimental study of CH3NH3PbI3-methylammonium lead triiodide (MAPI)-and its bromide cousin CH3NH3PbBr3 (MAPB), we analyze nitrogen K-edge (N Is-to-2p*) X-ray absorption (XA) spectra measured in MAPI and MAPB single crystals. This permits comparison of spectral features to the local character of unoccupied molecular orbitals on the CH3NH3+ (MA(+)) counterions and allows us to investigate how thermal fluctuations, hydrogen bonding, and halide-ion substitution influence the XA spectra as a measure of the local electronic structure. In agreement with the experiment, the simulated spectra for MAPI and MAPB show close similarity, except that the MAPB spectral features are blue-shifted by +0.31 eV. The shift is shown to arise from the intrinsic difference in the electronic structure of the two halide atoms rather than from structural differences between the materials. In addition, from the spectral sampling analysis of molecular dynamics simulations, clear correlations between geometric descriptors(N-C, N-H, and H center dot center dot center dot I/Br distances) and spectral features are identified and used to explain the spectral shapes.
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| 8. |
- Zeeshan, Faisal, et al.
(författare)
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Synchrotron measurements of Sulphonation degree from Chemimechanical pulp (CTMP) to optimize the pulping process for packaging products
- 2022
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Konferensbidrag (övrigt vetenskapligt/konstnärligt)abstract
- The manufacturing of CTMP has a significant role in producing sustainable packaging products. But the strategy to improve the impregnation technology is still challenging due to the uneven distribution of Na2SO3. Our aim was to investigate the oxidation states of Sulphonate present in our handmade paper samples which consist of different CTMP percentages. Therefore, XANES measurements were done to investigate the oxidation states and XRF measurements were done to see the presence of other elements. XRF mapping was also done to know the distribution of Na in the samples.
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