| 1. |
- Devid, E. J., et al.
(author)
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The influence of molecular mobility on the properties of networks of gold nanoparticles and organic ligands
- 2014
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In: Beilstein Journal of Nanotechnology. - : Beilstein Institut. - 2190-4286. ; 5:1, s. 1664-1674
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Journal article (peer-reviewed)abstract
- We prepare and investigate two-dimensional (2D) single-layer arrays and multilayered networks of gold nanoparticles derivatized with conjugated hetero-aromatic molecules, i.e., S-(4-{[2,6-bipyrazol-1-yl)pyrid-4-yl]ethynyl}phenyl) thiolate (herein S-BPP), as capping ligands. These structures are fabricated by a combination of self-assembly and microcontact printing techniques, and are characterized by electron microscopy, UV-visible spectroscopy and Raman spectroscopy. Selective binding of the S-BPP molecules to the gold nanoparticles through Au-S bonds is found, with no evidence for the formation of N-Au bonds between the pyridine or pyrazole groups of BPP and the gold surface. Subtle, but significant shifts with temperature of specific Raman S-BPP modes are also observed. We attribute these to dynamic changes in the orientation and/or increased mobility of the molecules on the gold nanoparticle facets. As for their conductance, the temperature-dependence for S-BPP networks differs significantly from standard alkanethiol-capped networks, especially above 220 K. Relating the latter two observations, we propose that dynamic changes in the molecular layers effectively lower the molecular tunnel barrier for BPP-based arrays at higher temperatures.
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| 2. |
- Dods, Robert, 1989, et al.
(author)
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Ultrafast structural changes within a photosynthetic reaction centre.
- 2021
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In: Nature. - : Springer Science and Business Media LLC. - 1476-4687 .- 0028-0836. ; 589:7841, s. 310-314
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Journal article (peer-reviewed)abstract
- Photosynthetic reaction centres harvest the energy content of sunlight by transporting electrons across an energy-transducing biological membrane. Here we use time-resolved serial femtosecond crystallography1 using an X-ray free-electron laser2 to observe light-induced structural changes in the photosynthetic reaction centre of Blastochloris viridis on a timescale of picoseconds. Structural perturbations first occur at the special pair of chlorophyll molecules of the photosynthetic reaction centre that are photo-oxidized by light. Electron transfer to the menaquinone acceptor on the opposite side of the membrane induces a movement of this cofactor together with lower amplitude protein rearrangements. These observations reveal how proteins use conformational dynamics to stabilize the charge-separation steps of electron-transfer reactions.
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| 3. |
- Dollmann, Antje, et al.
(author)
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Deformation twins as a probe for tribologically induced stress states
- 2024
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In: Communications Materials. - 2662-4443. ; 5:1
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Journal article (peer-reviewed)abstract
- Friction and wear of metals are critically influenced by the microstructures of the bodies constituting the tribological contact. Understanding the microstructural evolution taking place over the lifetime of a tribological system therefore is crucial for strategically designing tribological systems with tailored friction and wear properties. Here, we focus on the single-crystalline High-Entropy Alloy CoCrFeMnNi that is prone to form twins at room temperature. Deformation twins feature a pronounced orientation dependence with a tension-compression anisotropy, a distinct strain release in an extended volume and robust onset stresses. This makes deformation twinning an ideal probe to experimentally investigate the complex stress fields occurring in a tribological contact. Our results unambiguously show a grain orientation dependence of twinning under tribological load. It is clearly shown, that twinning cannot be attributed to a single crystal direction parallel to a sample coordinate axes. With deformation twins in the microstructure, stress field models can be validated to make them useable for all different tribological systems.
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| 4. |
- Klein, Andreas, et al.
(author)
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The Fermi energy as common parameter to describe charge compensation mechanisms: A path to Fermi level engineering of oxide electroceramics
- 2023
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In: Journal of Electroceramics. - 1573-8663 .- 1385-3449. ; 51
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Journal article (peer-reviewed)abstract
- Chemical substitution, which can be iso- or heterovalent, is the primary strategy to tailor material properties. There are various ways how a material can react to substitution. Isovalent substitution changes the density of states while heterovalent substitution, i.e. doping, can induce electronic compensation, ionic compensation, valence changes of cations or anions, or result in the segregation or neutralization of the dopant. While all these can, in principle, occur simultaneously, it is often desirable to select a certain mechanism in order to determine material properties. Being able to predict and control the individual compensation mechanism should therefore be a key target of materials science. This contribution outlines the perspective that this could be achieved by taking the Fermi energy as a common descriptor for the different compensation mechanisms. This generalization becomes possible since the formation enthalpies of the defects involved in the various compensation mechanisms do all depend on the Fermi energy. In order to control material properties, it is then necessary to adjust the formation enthalpies and charge transition levels of the involved defects. Understanding how these depend on material composition will open up a new path for the design of materials by Fermi level engineering.
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| 5. |
- Schäfer, David, et al.
(author)
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Multiscale Investigation of Sodium-Ion Battery Anodes: Analytical Techniques and Applications
- 2024
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In: Advanced Energy Materials. - 1614-6840 .- 1614-6832. ; 14:15
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Journal article (peer-reviewed)abstract
- The anode/electrolyte interface behavior, and by extension, the overall cell performance of sodium-ion batteries is determined by a complex interaction of processes that occur at all components of the electrochemical cell across a wide range of size- and timescales. Single-scale studies may provide incomplete insights, as they cannot capture the full picture of this complex and intertwined behavior. Broad, multiscale studies are essential to elucidate these processes. Within this perspectives article, several analytical and theoretical techniques are introduced, and described how they can be combined to provide a more complete and comprehensive understanding of sodium-ion battery (SIB) performance throughout its lifetime, with a special focus on the interfaces of hard carbon anodes. These methods target various length- and time scales, ranging from micro to nano, from cell level to atomistic structures, and account for a broad spectrum of physical and (electro)chemical characteristics. Specifically, how mass spectrometric, microscopic, spectroscopic, electrochemical, thermodynamic, and physical methods can be employed to obtain the various types of information required to understand battery behavior will be explored. Ways are then discussed how these methods can be coupled together in order to elucidate the multiscale phenomena at the anode interface and develop a holistic understanding of their relationship to overall sodium-ion battery function.
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