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Proximity effects on the H absorption in ultra-thin V layers
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Physics.
University of Iceland. (Department of Physics)
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Physics.
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2014 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 90, no 4, 045420- p.Article in journal (Refereed) Published
Abstract [en]

We discuss proximity effects on the hydrogen uptake in 14 atomic layers of vanadium. The enthalpy and entropy of solution were measured and compared to ab initio density functional calculations. We show that there exists a large difference in the hydrogen uptake of V in Cr/V and Fe/V superlattices, in which the V is under close to identical strain states. The calculations show that neither local strain effects nor charge redistributions can be the cause for the observed effect. This leaves magnetic and long ranged elastic strain fields-neither captured by the current calculations-as possible mechanisms for the observed effects.

Place, publisher, year, edition, pages
2014. Vol. 90, no 4, 045420- p.
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-140284DOI: 10.1103/PhysRevB.90.045420ISI: 000339482200006OAI: oai:DiVA.org:uu-140284DiVA: diva2:383370
Available from: 2011-01-04 Created: 2011-01-04 Last updated: 2017-12-11Bibliographically approved
In thesis
1. Influence of Self-trapping, Clamping and Confinement on Hydrogen Absorption
Open this publication in new window or tab >>Influence of Self-trapping, Clamping and Confinement on Hydrogen Absorption
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The dissociation of hydrogen molecules at surfaces is the first step in the absorption process. If the absorbing material is covered by an oxide, this layer will determine the effective uptake rate of an underlying absorbing material. This effect is illustrated when determining the rate of transport of hydrogen through amorphous aluminium oxide layers. The transport rate was determined to be strongly thickness dependent.

Hydrogen absorbed in a transition metal causes a volume expansion generated by a strain field around the absorbed hydrogen. This strain field causes a self-trapping of the hydrogen and a temperature dependent distribution in the atomic distances. The local strain field generated by the self-trapping process is found to be crucial for understanding both the hydrogen induced volume expansion as well as the diffusion of hydrogen. Ab-initio molecular dynamics simulations were used to reveal the temperature dependence of the unbinding of the hydrogen and the local strain field and its influence on the diffusion rate. The symmetry of the local strain field is also important for phase formation in metallic films and superlattices which are clamped to a substrate. As the thicknesses reduced from 50 to 10 nm thick vanadium films, substantial finite size effects become apparent in the phase diagrams. The volume change associated with the strain field cannot be accurately measured using x-ray diffraction because of its sensitivity to local arrangements of atoms. X-ray and neutron reflectivity were found to be more reliable probes of global effects of the sumof the local strainfields.

Finite size effects in extremely thin V layers were also explored in metallic superlattices composed of iron and vanadium. The co-existence region, composed of a hydrogen gas and a solid-like phase, was found to be suppressed by at least 100 K to below 300 K. The hydrogen-hydrogen interaction can also be influenced by the electronic states in the non hydrogen absorbing layers, as demonstrated when comparing hydrogen absorption in Fe/V and Cr/V superlattices.

 

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2011. 59 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 798
Keyword
hydrogen diffusion, thin films, superlattices, phase transitions, confinement, clamping, self-trapping, finite-size effect
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-140329 (URN)978-91-554-7983-1 (ISBN)
Public defence
2011-02-18, Häggsalen, Ångström laboratory, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Note
Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 728Available from: 2011-01-31 Created: 2011-01-04 Last updated: 2011-03-21Bibliographically approved
2. Thermodynamics of Hydrogen in Confined Lattice
Open this publication in new window or tab >>Thermodynamics of Hydrogen in Confined Lattice
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Three of the most important questions concerning hydrogen storage in metals are how much hydrogen can be absorbed, how fast it can be absorbed (or released) and finally how strongly the hydrogen is bonded. In transition metals hydrogen occupies interstitial sites and the absorption as well as desorption of hydrogen can be fast. The enthalpy of the hydride formation is determined by the electronic structure of the absorbing material, which determines the amount of energy released in the hydrogen uptake and the energy needed to release the hydrogen.

This thesis concerns the possibility of tuning hydrogen uptake by changing the extension of the absorbing material and the boundary conditions of extremely thin layers. When working with extremely thin layers, it is possible to alter the strain state of the absorbing material, which is used to influence the site occupancy of hydrogen isotopes. Vanadium is chosen as a model system for these studies. V can be grown in the form of thin films as well as superlattices using MgO as a substrate. Special emphasis are on Fe/V(001) and Cr/V(001) superlattices as these can be grown as high quality single crystals on a routine basis. The use of high quality samples ensured well-defined conditions for all the measurements.

In these experiments the hydrogen concentration is determined by the light transmittance of the thin films.  By changing the temperature and the pressure of the hydrogen gas, it is possible to determine the thermodynamic properties of hydrogen in the samples, from the obtained concentrations.  Measurements of the electrical resistivity is used to increase the accuracy in the measurements at low concentrations as well as to provide information on ordering at intermediate and high hydrogen concentrations. The thermodynamic properties and the electrical resistivity of VH are strongly affected by the choice of boundary layers. For example, when hydrogen is absorbed in V embedded by Fe, Cr or Mo in the form of superlattices, both the thermodynamic properties and the changes in the resistivity are strongly influenced.

The critical temperature and H-H interactions of hydrogen in thin V(001) layers are found to increase with thickness of the thin films and superlattices. The observed finite size effects resemble same scaling with the thickness of the layers as does the magnetic ordering temperature. The results were validated by investigations of isotope effects in the obtained thermodynamic properties. Close to negligible effects are obtained when replacing hydrogen by deuterium, with respect to the thermodynamic properties. These observations are rationalised by an octahedral occupancy in the strained layers, as compared to tetrahedral occupancy in unstrained bulk. The octahedral site occupancy is found to strongly alter the diffusion coefficient of hydrogen in thin V layers.

 

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2016. 59 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1344
Keyword
thermodynamics hydrogen superlattice
National Category
Condensed Matter Physics Nano Technology
Identifiers
urn:nbn:se:uu:diva-275629 (URN)978-91-554-9473-5 (ISBN)
Public defence
2016-03-17, Häggsalen, Ångströmlaboratoriet, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2016-02-22 Created: 2016-02-04 Last updated: 2016-03-09

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Pálsson, Gunnar K.Amft, MartinXin, XiaoHjörvarsson, Björgvin

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