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Electronic structure of water molecules confined in a micelle lattice
Uppsala universitet, Medicinska och farmaceutiska vetenskapsområdet, Farmaceutiska fakulteten, Institutionen för farmaci.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och materialvetenskap, Mjukröntgenfysik.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Fysiska sektionen, Institutionen för fysik och materialvetenskap, Mjukröntgenfysik.
Visa övriga samt affilieringar
2009 (Engelska)Ingår i: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 113, nr 24, s. 8201-8205Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Oxygen K absorption and emission spectra of water molecules confined in dodecyltrimethyl ammonium chloride micelle structures are presented. The local electronic structure of the water molecules is found to be dramatically different from the electronic structure of water molecules in the gas-phase as well as in liquid water. Hybridization with states of the ions in the surrounding ions is directly observed, and evidence for stabilization of the water molecules relative to molecules in bulk water is found.

Ort, förlag, år, upplaga, sidor
2009. Vol. 113, nr 24, s. 8201-8205
Nationell ämneskategori
Fysik
Identifikatorer
URN: urn:nbn:se:uu:diva-109461DOI: 10.1021/jp902058wISI: 000266930200001PubMedID: 19473020OAI: oai:DiVA.org:uu-109461DiVA, id: diva2:272503
Tillgänglig från: 2009-10-15 Skapad: 2009-10-15 Senast uppdaterad: 2017-12-12Bibliografiskt granskad
Ingår i avhandling
1. In Situ Soft X-ray Spectroscopies Applied to Atmospheric Corrosion And Related Systems
Öppna denna publikation i ny flik eller fönster >>In Situ Soft X-ray Spectroscopies Applied to Atmospheric Corrosion And Related Systems
2009 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

This thesis concerns the application of various soft x-ray spectroscopic methods (soft x-ray absorption, SXA, and emission, SXE) to complex, non-vacuum compatible systems, including liquids and multi-phase systems.

The design, construction, and application of new instrumentation for in situ spectroscopy is described in detail. This includes sample holders using thin soft x-ray transparent membranes to enable measurements on systems completely isolated from vacuum, enabling flow of e.g. liquid or gas. In particular, a versatile setup for time resolved in situ chemical contrast x-ray transmission microscopy (CCXTM) was constructed and implemented. These instruments are expected to be applicable to a wide range of situations, for example in situ studies of chemical reactions, or biological specimen.

The main project concerns atmospheric corrosion of iron in a saline environment, a process that requires the simultaneous presence of the solid (iron, NaCl), liquid (water) and gaseous (air) phases. It is also a highly inhomogeneous process, where lateral and time resolution is important. Using the CCXTM instrumentation, we were able to follow the distribution of all present elements over the sample with time resolution of a few minutes, and also to extract significant chemical information from the absorption edges. We observed e.g. the initial formation of corrosion products and transport of chlorine.

Results from SXE measurements on water molecules in micelle structures are presented. A comparison with calculations reveal influence from the counter-ions, but also some spectral changes that may be attributed to water confinement.

Also presented are angle dependent soft x-ray emission of liquid water, measuring scattered x-rays from different directions respect to the incident x-ray polarization. Existing preliminary theoretical expectations for the polarization dependence are contradictory. Our experiments show that a small angular anisotropy seems to be retained from the free molecule case.

Ort, förlag, år, upplaga, sidor
Uppsala: Universitetsbiblioteket, 2009. s. ix, 85
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 595
Nationell ämneskategori
Fysik
Identifikatorer
urn:nbn:se:uu:diva-9540 (URN)978-91-554-7397-6 (ISBN)
Disputation
2009-02-27, Häggsalen, Ångström Laboratory, Lägerhyddsvägen 1, Polacksbacken, Uppsala, 13:15 (Engelska)
Opponent
Handledare
Tillgänglig från: 2009-02-06 Skapad: 2009-02-06 Senast uppdaterad: 2010-05-05Bibliografiskt granskad
2. Molecular Arrangement, Electronic Structure and Transport Properties in Surfactant Gel- and Related Systems Studied by Soft X-ray and Dielectric Spectroscopy
Öppna denna publikation i ny flik eller fönster >>Molecular Arrangement, Electronic Structure and Transport Properties in Surfactant Gel- and Related Systems Studied by Soft X-ray and Dielectric Spectroscopy
2013 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

This thesis concerns studies of aqueous soft matter systems, especially surfactant micelle systems.

The aim has been to study the molecular arrangement and electronic structure of the constituents of, as well as transport properties in such a system. The molecular arrangement and electronic structure has been studied by means of X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray spectroscopy (RIXS). The transport properties have been investigated by low-frequency dielectric spectroscopy (LFDS) and small angle X-ray scattering (SAXS) as well as a theoretical modelling. The latter was based on Fick’s laws of the release from binary surfactant system and was validated by experiments.

The RIXS and XAS measurements show the electronic structure in bulk water and the influence of the chemical surrounding of the water molecule in bulk water and of the water molecules confined in a micelle lattice. The spectra are highly dependent on the molecular arrangement in such systems. For glycine and sodium polyacrylate RIXS and XAS spectra show features which are unique for carboxyl and carboxylate groups and such measurements can thus be used for fingerprinting.

The LFDS and SAXS measurements show a strong correlation between structure in a surfactant/poly-ion system and apparent mobility of surfactants. This conclusion is in line with earlier observations.

By the theoretical modelling a predictive model for the surfactant release from a binary surfactant micelle system has been obtained and the importance of different factors for surfactant release has been further clarified.

Ort, förlag, år, upplaga, sidor
Uppsala: Acta Universitatis Upsaliensis, 2013. s. 77
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1060
Nyckelord
surfactants, surfactant/poly-ion gel, water, confined water, XAS, RIXS, dielectric spectroscopy, SAXS, pKa, transport, Fick’s law
Nationell ämneskategori
Nanoteknik
Forskningsämne
Teknisk fysik med inriktning mot nanoteknologi och funktionella material
Identifikatorer
urn:nbn:se:uu:diva-205072 (URN)978-91-554-8721-8 (ISBN)
Disputation
2013-09-27, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:30 (Svenska)
Opponent
Handledare
Tillgänglig från: 2013-09-04 Skapad: 2013-08-13 Senast uppdaterad: 2014-01-08

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Andersson, EgilForsberg, JohanBrena, BarbaraHennies, Franz

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