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The properties and nature of water clusters studied with novel spectroscopic approaches are presented in this thesis. Following a general introduction on the chemistry of water and water clusters, detailed descriptions of the experiments and analyses are given. All the experimental results, including first size-selective spectra of large clusters consisting of 200 water molecules, are presented with corresponding analyses. Hitherto unidentified hydrogen bond network structures, dynamics, and reactivity of various water clusters have been characterized at the molecular level. The main targets…mehr
The properties and nature of water clusters studied with novel spectroscopic approaches are presented in this thesis. Following a general introduction on the chemistry of water and water clusters, detailed descriptions of the experiments and analyses are given. All the experimental results, including first size-selective spectra of large clusters consisting of 200 water molecules, are presented with corresponding analyses. Hitherto unidentified hydrogen bond network structures, dynamics, and reactivity of various water clusters have been characterized at the molecular level. The main targets of this book are physical chemists and chemical physicists who are interested in water chemistry or cluster chemistry.
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Department of Photo-Molecular Science (Prof. Yasuhiro Ohshima's Lab.), Institute for Molecular Science, Japan
Assistant professor
April 2008-March 2011
The Japan Society for the Promotion of Science (JSPS) Research fellow
April 2006-March 2011
Department of Chemistry, Graduate School of Science, Tohoku University, Japan
Ph.D. student
Supervisor: Professor Asuka Fujii
Degree obtained: Ph.D. in Science
April 2002-March 2006
Department of Chemistry, Faculty of Science, Tohoku University, Japan
Undergraduate student
Supervisor: Professor Naohiko Mikami
Publications
1 Mizuse, K. & Fujii, A. Infrared Spectroscopy of Large Protonated Water Clusters H+(H2O)20-50 Cooled by Inert Gas Attachment. Chem. Phys. in press, doi:10.1016/j.chemphys.2012.07.012 (2013).
2 Mizuse, K. & Fujii, A. Tuning of the Internal Energy and Isomer Distribution in Small Protonated Water Clusters H+(H2O)4-8: An Application of the Inert Gas Messenger Technique. J. Phys. Chem. A 116, 4868-4877 (2012).
3 Mizuse, K., Suzuki, Y., Mikami, N. & Fujii, A. Solvation-Induced s-Complex Structure Formation in the Gas Phase: A Revisit to the Infrared Spectroscopy of [C6H6-(CH3OH)2]+. J. Phys. Chem. A 115, 11156-11161 (2011).
4 Mizuse, K., Kuo, J.-L. & Fujii, A. Structural trends of ionized water networks: Infrared spectroscopy of water cluster radical cations (H2O)n+ (n = 3-11). Chem. Sci. 2, 868-876 (2011).
5 Mizuse, K. & Fujii, A. Structural Origin of the Antimagic Number in Protonated Water Clusters H+(H2O)n: Spectroscopic Observation of the "Missing" Water Molecule in the Outermost Hydration Shell. J. Phys. Chem. Lett. 2, 2130-2134 (2011).
6 Mizuse, K. & Fujii, A. Infrared photodissociation spectroscopy of H+(H2O)6·Mm (M = Ne, Ar, Kr, Xe, H2, N2, and CH4): messenger-dependent balance between H3O+ and H5O2+ core isomers. Phys. Chem. Chem. Phys. 13, 7129-7135 (2011).
7 Hamashima, T., Mizuse, K. & Fujii, A. Spectral Signatures of Four-Coordinated Sites in Water Clusters: Infrared Spectroscopy of Phenol-(H2O)n (~20 = n = ~50). J. Phys. Chem. A 115, 620-625 (2011).
8 Mizuse, K., Mikami, N. & Fujii, A. Infrared Spectra and Hydrogen-Bonded Network Structures of Large Protonated Water Clusters H+(H2O)n (n=20-200). Angew. Chem. Int. Ed. 49, 10119-10122 (2010).
9 Mizuse, K., Hasegawa, H., Mikami, N. & Fujii, A. Infrared and Electronic Spectroscopy of Benzene-Ammonia Cluster Radical Cations [C6H6(NH3)1,2]+: Observation of Isolated and Microsolvated s-Complexes+. J. Phys. Chem. A 114, 11060-11069 (2010).
10 Mizuse, K., Hamashima, T. & Fujii, A. Infrared Spectroscopy of Phenol-(H2O)n>10: Structural Strains in Hydrogen Bond Networks of Neutral Water Clusters. J. Phys. Chem. A 113, 12134-12141 (2009).
11 Hasegawa, H. et al. Observation of an isolated intermediate of the nucleophilic aromatic substition reaction by infrared spectroscopy. Angew. Chem. Int. Ed. 47, 6008-6010 (2008).
12 Suhara, K., Fujii, A., Mizuse, K., Mikami, N. & Kuo, J. L. Compatibility between methanol and water in the three-dimensional cage formation of large-sized protonated methanol-water mixed clusters. J. Chem. Phys. 126, 194306 (2007).
13 Mizuse, K., Fujii, A. & Mikami, N. Long range influence of an excess proton on the architecture of the hydrogen bond network in large-sized water clusters. J. Chem. Phys. 126, 231101 (2007).
14 Mizuse, K., Fujii, A. & Mikami, N. Infrared and electronic spectroscopy of a model system for the nucleophilic substitution intermediate in the gas phase: The C-N valence bond formation in the benzene-ammonia cluster cation. J. Phys. Chem. A 110, 6387-6390 (2006).
Inhaltsangabe
General Introduction.- Infrared spectroscopy of chromophore-labeled water clusters phenol-(H2O)n (n < ~50).- Infrared pectroscopy of large protonated water clusters H+(H2O)n (n 221).- Tuning of the Internal Energy and Isomer Distribution in Protonated Water Clusters H+(H2O)n (n 50): Towards a more detailed understanding of structures and dynamics.- Infrared spectroscopy of water cluster radical cations (H2O)n+ (n 11).- Conclusions and future work.
General Introduction.- Infrared spectroscopy of chromophore-labeled water clusters phenol-(H2O)n (n < ~50).- Infrared pectroscopy of large protonated water clusters H+(H2O)n (n 221).- Tuning of the Internal Energy and Isomer Distribution in Protonated Water Clusters H+(H2O)n (n 50): Towards a more detailed understanding of structures and dynamics.- Infrared spectroscopy of water cluster radical cations (H2O)n+ (n 11).- Conclusions and future work.
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