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First Principle Study of Water: From Fundamental Properties to Photocatalytic Reaction

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dc.contributor.advisor Maria Victoria Fernandez-Serra. en_US
dc.contributor.author Wang, Jue en_US
dc.contributor.other Department of Physics en_US
dc.date.accessioned 2012-05-17T12:23:06Z
dc.date.accessioned 2015-04-24T14:48:53Z
dc.date.available 2012-05-17T12:23:06Z
dc.date.available 2015-04-24T14:48:53Z
dc.date.issued 2011-05-01 en_US
dc.identifier Wang_grad.sunysb_0771E_10479.pdf en_US
dc.identifier.uri http://hdl.handle.net/1951/56149 en_US
dc.identifier.uri http://hdl.handle.net/11401/71723 en_US
dc.description.abstract Ab initio molecular dynamics (AIMD) simulations of liquid water, based on density functional theory (DFT), yield structural and diffusive properties in reasonable agreement with experiment when artificially high temperatures are used in the simulations for gradient-corrected (GGA) functionals, with NVT ensemble. A series of simulations with GGA functionals is performed and underestimation of equilibrium density, at ambient conditions, is found. Electronic density of water molecules with several GGA functionals is examined and used to explain structural and dynamical property differences. Dispersive non-local electron-electron correlations are studied with a van der Waals density functional (vdW-DF) of Dion et al. When a vdW-DF is used, the density improves drastically and the experimental diffusivity is reproduced without the need of thermal corrections. The origin of the density differences between all the functionals is analyzed. It has been shown the vdW-DF increases the population of non-H-bonded interstitial sites, at distances between the first and second coordination shells. However, it excessively weakens the H-bond network, collapsing the second coordination shell. GaN/ZnO alloy semiconductors have been shown to be promising materials to serve as photo-anode in photocatalytical fuel cells. A thorough AIMD study of the non polar GaN(1010) surface with aqueous interface is carried out. It has been shown that water dissociation happens very fast within 1ps. Interacting OH dimers are found to account for around 80% of the dissociated water molecules through a hydrogen bond. A detailed study of the OH dimers shows their distinguishable structural, dynamical and electronic properties. Solvent water molecules interacting with a dissociating wet surface is also studied in detail, especially the hydrogen bond network. Proton diffusion is found starting from non-dissociated surface water molecules. The effective free energy barrier of proton diffusion is shown to be near room temperature thermal energy. en_US
dc.description.sponsorship This work is sponsored by the Stony Brook University Graduate School in compliance with the requirements for completion of degree. en_US
dc.format Monograph en_US
dc.format.medium Electronic Resource en_US
dc.language.iso en_US en_US
dc.publisher The Graduate School, Stony Brook University: Stony Brook, NY. en_US
dc.subject.lcsh Physics en_US
dc.title First Principle Study of Water: From Fundamental Properties to Photocatalytic Reaction en_US
dc.type Dissertation en_US
dc.mimetype Application/PDF en_US
dc.contributor.committeemember Philip B. Allen en_US
dc.contributor.committeemember Thomas C. Weinacht en_US
dc.contributor.committeemember Michael G. White en_US

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