liu.seSök publikationer i DiVA
Ändra sökning
RefereraExporteraLänk till posten
Permanent länk

Direktlänk
Referera
Referensformat
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • oxford
  • Annat format
Fler format
Språk
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Annat språk
Fler språk
Utmatningsformat
  • html
  • text
  • asciidoc
  • rtf
Computational studies of the stability of the (H2O)100 nanodrop
Linköpings universitet, Institutionen för fysik, kemi och biologi, Fysikalisk Kemi. Linköpings universitet, Tekniska högskolan.
Linköpings universitet, Institutionen för fysik, kemi och biologi, Fysikalisk Kemi. Linköpings universitet, Tekniska högskolan.ORCID-id: 0000-0002-5341-2637
2010 (Engelska)Ingår i: Journal of Molecular Structure: THEOCHEM, ISSN 0166-1280, Vol. 944, nr 1-3, s. 163-167Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

The stability of the (H2O)100 nanodrop, experimentally known from a polyoxomolybdatecrystal structure (Müller et al. Inorg. Chem. Commun., 2003, 6, 52) and other structuresinferred from clathrate structures, are studied by quantum-chemical B3LYP computations.The free energies are compared to the trends for smaller clusters with 15-30 molecules. Forthe small clusters both cage-based structures and denser structures with a larger number of Hbondsobtained by an evolutionary algorithm (Bandow and Hartke, J. Phys. Chem. A, 2006,110, 5809) are used. The dense structures are most often found to be lower in electronicenergy. The cage-based structures, to which the structure of the experimentally found(H2O)100 cluster can be categorized, become more stable when Gibbs free energy is calculatedat 298 K. Additional cage-based clusters in the 35-81 molecular range were constructed forcomparison. The experimental cluster with 100 molecules (C2h/Ci-symmetry for oxygens/allatoms) and the constructed cluster with 42 molecules are found to be lower in energy than aplausible overall trend. The (H2O)42 cluster has an extraordinary high symmetry (S6), evenwhen the hydrogens are considered. The (H2O)100 cluster is the only of the studied clusters forwhich ΔG is negative at 298 K.

Ort, förlag, år, upplaga, sidor
2010. Vol. 944, nr 1-3, s. 163-167
Nyckelord [en]
Water clusters, Quantum-chemical computations, Hydrogen bonding, B3LYP calculations, Gibbs free energy
Nationell ämneskategori
Naturvetenskap
Identifikatorer
URN: urn:nbn:se:liu:diva-53176DOI: 10.1016/j.theochem.2009.12.033ISI: 000275688200022OAI: oai:DiVA.org:liu-53176DiVA, id: diva2:287413
Anmärkning
Original Publication: Annika Lenz and Lars Ojamäe, Computational studies of the stability of the (H2O)100 nanodrop, 2010, Journal of Molecular Structure: THEOCHEM, (944), 1-3, 163-167. http://dx.doi.org/10.1016/j.theochem.2009.12.033 Copyright: Elsevier Science B.V., Amsterdam http://www.elsevier.com/ Tillgänglig från: 2010-01-18 Skapad: 2010-01-18 Senast uppdaterad: 2017-12-12
Ingår i avhandling
1. Theoretical Investigations of Water Clusters, Ice Clathrates and Functionalized Nanoparticles
Öppna denna publikation i ny flik eller fönster >>Theoretical Investigations of Water Clusters, Ice Clathrates and Functionalized Nanoparticles
2009 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

Nanosized structures are of intermediate size between individual molecules and bulkmaterials which gives them several unique properties. At the same time their relative limitedsizes make them suitable for studies by the methods of computational chemistry. In this thesiswater clusters, ice clathrates and functionalized metal-oxide nanoparticles have been studiedby quantum-chemical calculations and statistical thermodynamics.

The stabilities of water clusters composed of up to 100 molecules have been investigated. Themultitude of possible H-bonded topologies and their importance for determining theproperties of the clusters have been highlighted. Several structural characteristics of thehydrogen bonded network have been examined and the structural factors that determine thestability of an H-bonded network have been identified. The stability of two kinds of oxygenframeworks for water clusters have been analyzed, taking into account thermal energy andentropy corrections. Clusters with many 4-coordinated molecules have been found to be lowerin energy at low temperatures whereas the clusters with less-coordinated molecules dominateat higher temperatures. The equilibrium size distribution of water clusters as a function oftemperature and pressure has been computed using statistical thermodynamics. Themicroscopic local structure of liquid water has been probed by utilizing information from thestudied water clusters. The average number of H-bonds in liquid water has been predicted byfitting calculated average IR spectra for different coordination types in water clusters toexperimental IR spectra.

Water can form an ice-like structure that encloses various molecules such as methane. Thesemethane hydrates are found naturally at the ocean floor and in permafrost regions and canconstitute a large unemployed energy resource as well as a source of an effective green-housegas. The pressure dependencies of the crystal structures, lattice energies and phase transitionsfor the three methane hydrates with the clathrate structures I, II and H have been mapped out.

Zinc oxide is a semiconducting material with interesting luminescence properties that can beutilized in optical devices, such as photodetectors, light emitting devices and biomarkers. Theeffect of water molecules adsorbed on the ZnO surface when adsorbing organic acids havebeen investigated. Changes in optical properties by the adsorption of carboxylic acids havebeen studied and compared with experimental results. Aromatic alcohols at TiO2 metal-oxidenanoparticles have been studied as model systems for dye-sensitizied solar cells. Adsorptiongeometries are predicted and the influence from the adsorbed molecules on the electronicproperties has been studied.

Ort, förlag, år, upplaga, sidor
Linköping: Linköping University Electronic Press, 2009. s. 52
Serie
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1254
Nationell ämneskategori
Annan medicinsk grundvetenskap
Identifikatorer
urn:nbn:se:liu:diva-52746 (URN)978-91-7393-636-1 (ISBN)
Disputation
2009-06-09, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (Svenska)
Opponent
Handledare
Tillgänglig från: 2010-01-18 Skapad: 2010-01-12 Senast uppdaterad: 2018-01-12Bibliografiskt granskad

Open Access i DiVA

fulltext(802 kB)668 nedladdningar
Filinformation
Filnamn FULLTEXT01.pdfFilstorlek 802 kBChecksumma SHA-512
1af39555870ed8f0215ed3f0093dc3b1726fdf13eed1beb167798a3a9437d588a730df1e79d6c78048f0a65df409a51a729abdefc007a11f128c40b510314fad
Typ fulltextMimetyp application/pdf

Övriga länkar

Förlagets fulltext

Personposter BETA

Lenz, AnnikaOjamäe, Lars

Sök vidare i DiVA

Av författaren/redaktören
Lenz, AnnikaOjamäe, Lars
Av organisationen
Fysikalisk KemiTekniska högskolan
I samma tidskrift
Journal of Molecular Structure: THEOCHEM
Naturvetenskap

Sök vidare utanför DiVA

GoogleGoogle Scholar
Totalt: 668 nedladdningar
Antalet nedladdningar är summan av nedladdningar för alla fulltexter. Det kan inkludera t.ex tidigare versioner som nu inte längre är tillgängliga.

doi
urn-nbn

Altmetricpoäng

doi
urn-nbn
Totalt: 268 träffar
RefereraExporteraLänk till posten
Permanent länk

Direktlänk
Referera
Referensformat
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • oxford
  • Annat format
Fler format
Språk
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Annat språk
Fler språk
Utmatningsformat
  • html
  • text
  • asciidoc
  • rtf