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Structure and dynamics of electronic defects in liquid water
Maršálek, Ondřej ; Jungwirth, Pavel (advisor) ; Horáček, Jiří (referee) ; Pittner, Jiří (referee)
Title: Structure and dynamics of electronic defects in liquid water Author: Ondřej Maršálek Institute: Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic Supervisor: prof. Mgr. Pavel Jungwirth, DSc. Supervisor's e-mail address: pavel.jungwirth@uochb.cas.cz Abstract: In this thesis we present ab inito molecular dynamics simulations of two different electronic defects in water. Photoionization of liquid water produces a cationic hole, which undergoes ultrafast dynamics and forms the hydrated proton and the hydroxyl radical as its products. We study both the dynamics and spectroscopy of this process. The hydrated electron is a key intermediate in radiation chemistry of aqueous systems. We simulate its equilibrium properties in anionic water clusters as well as the dynamics of vertical electron attachment to cold and warm clusters. The hydrated electron reacts with a hydrated proton to form a hydrogen atom. We examine this reaction at a finite temperature in a larger cluster as well as in more detail in a smaller cluster. Because both of the electronic defects studied here are challenging open-shell species, we put emphasis on benchmarking and testing our computational setup. Six published articles are attached to the thesis. Keywords: density functional theory,...
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Structure, dynamics and reactivity of the hydrated electron
Uhlig, Frank ; Jungwirth, Pavel (advisor) ; Pittner, Jiří (referee) ; Sebastiani, Daniel (referee)
Structure, dynamics and reactivity of the hydrated electron Frank Uhlig In this work, one of the products of ionization of water, namely the hydrated electron, has been investigated. The hydrated electron is a key-intermediate in aqueous radiation chemistry. Although known to exist for over 50 years, its structure remained elusive and under discussion up to the present day. We show in this work, that we can obtain a faithful picture of the hydrated electron, its equilibrium structure, dynamics after attachment to water, and its reactivity, using ab initio methods. To this end, small cluster models and extended bulk and slab geometries of water including an excess electron have been investigated.
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Structure and dynamics of electronic defects in liquid water
Maršálek, Ondřej
Title: Structure and dynamics of electronic defects in liquid water Author: Ondřej Maršálek Institute: Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic Supervisor: prof. Mgr. Pavel Jungwirth, DSc. Supervisor's e-mail address: pavel.jungwirth@uochb.cas.cz Abstract: In this thesis we present ab inito molecular dynamics simulations of two different electronic defects in water. Photoionization of liquid water produces a cationic hole, which undergoes ultrafast dynamics and forms the hydrated proton and the hydroxyl radical as its products. We study both the dynamics and spectroscopy of this process. The hydrated electron is a key intermediate in radiation chemistry of aqueous systems. We simulate its equilibrium properties in anionic water clusters as well as the dynamics of vertical electron attachment to cold and warm clusters. The hydrated electron reacts with a hydrated proton to form a hydrogen atom. We examine this reaction at a finite temperature in a larger cluster as well as in more detail in a smaller cluster. Because both of the electronic defects studied here are challenging open-shell species, we put emphasis on benchmarking and testing our computational setup. Six published articles are attached to the thesis. Keywords: density functional theory,...
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Structure, dynamics and reactivity of the hydrated electron
Uhlig, Frank ; Jungwirth, Pavel (advisor) ; Pittner, Jiří (referee) ; Sebastiani, Daniel (referee)
Structure, dynamics and reactivity of the hydrated electron Frank Uhlig In this work, one of the products of ionization of water, namely the hydrated electron, has been investigated. The hydrated electron is a key-intermediate in aqueous radiation chemistry. Although known to exist for over 50 years, its structure remained elusive and under discussion up to the present day. We show in this work, that we can obtain a faithful picture of the hydrated electron, its equilibrium structure, dynamics after attachment to water, and its reactivity, using ab initio methods. To this end, small cluster models and extended bulk and slab geometries of water including an excess electron have been investigated.
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Structure and dynamics of electronic defects in liquid water
Maršálek, Ondřej
Title: Structure and dynamics of electronic defects in liquid water Author: Ondřej Maršálek Institute: Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic Supervisor: prof. Mgr. Pavel Jungwirth, DSc. Supervisor's e-mail address: pavel.jungwirth@uochb.cas.cz Abstract: In this thesis we present ab inito molecular dynamics simulations of two different electronic defects in water. Photoionization of liquid water produces a cationic hole, which undergoes ultrafast dynamics and forms the hydrated proton and the hydroxyl radical as its products. We study both the dynamics and spectroscopy of this process. The hydrated electron is a key intermediate in radiation chemistry of aqueous systems. We simulate its equilibrium properties in anionic water clusters as well as the dynamics of vertical electron attachment to cold and warm clusters. The hydrated electron reacts with a hydrated proton to form a hydrogen atom. We examine this reaction at a finite temperature in a larger cluster as well as in more detail in a smaller cluster. Because both of the electronic defects studied here are challenging open-shell species, we put emphasis on benchmarking and testing our computational setup. Six published articles are attached to the thesis. Keywords: density functional theory,...
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Structure and dynamics of electronic defects in liquid water
Maršálek, Ondřej ; Jungwirth, Pavel (advisor) ; Horáček, Jiří (referee) ; Pittner, Jiří (referee)
Title: Structure and dynamics of electronic defects in liquid water Author: Ondřej Maršálek Institute: Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic Supervisor: prof. Mgr. Pavel Jungwirth, DSc. Supervisor's e-mail address: pavel.jungwirth@uochb.cas.cz Abstract: In this thesis we present ab inito molecular dynamics simulations of two different electronic defects in water. Photoionization of liquid water produces a cationic hole, which undergoes ultrafast dynamics and forms the hydrated proton and the hydroxyl radical as its products. We study both the dynamics and spectroscopy of this process. The hydrated electron is a key intermediate in radiation chemistry of aqueous systems. We simulate its equilibrium properties in anionic water clusters as well as the dynamics of vertical electron attachment to cold and warm clusters. The hydrated electron reacts with a hydrated proton to form a hydrogen atom. We examine this reaction at a finite temperature in a larger cluster as well as in more detail in a smaller cluster. Because both of the electronic defects studied here are challenging open-shell species, we put emphasis on benchmarking and testing our computational setup. Six published articles are attached to the thesis. Keywords: density functional theory,...
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