| 1. |
- Bahn, Emanuel, et al.
(författare)
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The structure of deuterated benzene films adsorbed on the graphite (0001) basal plane: what happens below and above the monolayer coverage?
- 2014
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Ingår i: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9084. ; 16:40, s. 22116-22121
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Tidskriftsartikel (refereegranskat)abstract
- An exact description of the interactions in aromatic carbon systems is a key condition for the design of carbon based nanomaterials. In this paper we investigate the binding and adsorbate structure of the simplest prototype system in this class the single aromatic ring molecule benzene on graphite. We have collected neutron diffraction data of the ordered phase of deuterated benzene, C6D6, adsorbed on the graphite (0001) basal plane surface. We examined relative coverages from 0.15 up to 1.3 monolayers (ML) in a temperature range of 80 to 250 K. The results confirm the flat lying commensurate (root 7 x root 7)R19.1 degrees monolayer with lattice constants a = b = 6.5 angstrom at coverages of less than 1 ML. For this structure we observe a progressive melting well below the desorption temperature. At higher coverages we do neither observe an ordered second layer nor a densification of the structure by upright tilting of first layer molecules, as generally assumed up to now. Instead, we see the formation of clusters with a bulk crystalline structure for coverages only weakly exceeding 1 ML.
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| 2. |
- Gao, Shang, et al.
(författare)
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Dipolar Spin Ice States with a Fast Monopole Hopping Rate in CdEr2X4 (X = Se, S)
- 2018
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 120:13
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Tidskriftsartikel (refereegranskat)abstract
- Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr2Se4 is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three orders of magnitude faster than the canonical spin ice Dy2Ti2O7. In this Letter we use diffuse neutron scattering to show that both CdEr2Se4 and CdEr2S4 support a dipolar spin ice state-the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to those in Dy2Ti2O7, i.e., dilute and uncorrelated, and so cannot provide three orders faster dynamics through a larger monopole population alone. We investigate the monopole dynamics using ac susceptometry and neutron spin echo spectroscopy, and verify the crystal electric field Hamiltonian of the Er3+ ions using inelastic neutron scattering. A quantitative calculation of the monopole hopping rate using our Coulomb gas and crystal electric field parameters shows that the fast dynamics in CdEr2X4 (X = Se, S) are primarily due to much faster monopole hopping. Our work suggests that CdEr2X4 offer the possibility to study alternative spin ice ground states and dynamics, with equilibration possible at much lower temperatures than the rare earth pyrochlore examples.
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| 3. |
- Perrichon, Adrien, 1988, et al.
(författare)
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Proton Diffusion Mechanism in Hydrated Barium Indate Oxides
- 2023
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Ingår i: Chemistry of Materials. - 1520-5002 .- 0897-4756. ; 35:17, s. 6713-6725
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Tidskriftsartikel (refereegranskat)abstract
- We report on quasielastic neutron scattering (QENS) andab initiomolecular dynamics (AIMD) simulations of the mechanism of proton diffusionin the partially and fully hydrated barium indate oxide proton conductorsBa(2)In(2)O(5)(H2O)( x ) (x = 0.30 and 0.92). Structurally,these materials are featured by an intergrowth of cubic and "pseudo-cubic"layers of InO6 octahedra, wherein two distinct proton sites,H(1) and H(2), are present. We show that the main localized dynamicsof these protons can be described as rotational diffusion of O-H(1)species and H(2) proton transfers between neighboring oxygen atoms.The mean residence times of both processes are in the order of picosecondsin the two studied materials. For the fully hydrated material, Ba2In2O5(H2O)(0.92), we also reveal the presence of a third proton site, H(3), whichbecomes occupied upon increasing the temperature and serves as a saddlestate for the interexchange between H(1) and H(2) protons. Crucially,the occupation of the H(3) site enables long-range diffusion of protons,which is highly anisotropic in nature and occurs through a two-dimensionalpathway. For the partially hydrated material, Ba2In2O5(H2O)(0.30), the occupationof the H(3) site and subsequent long-range diffusion are not observed,which is rationalized by hindered dynamics of H(2) protons in thevicinity of oxygen vacancies. A comparison to state-of-the-art proton-conductingoxides, such as barium zirconate-based materials, suggests that thegenerally lower proton conductivity in Ba2In2O5(H2O)( x ) is dueto a large occupation of the H(1) and H(2) sites, which, in turn,means that there are few sites available for proton diffusion. Thisinsight suggests that the chemical substitution of indium by cationswith higher oxidation states offers a novel route toward higher protonconductivity because it reduces the proton site occupancy while preservingan oxygen-vacancy-free structure.
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