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Title: Probing Properties of Glassy Water and Other Liquids with Site Selective Spectroscopies

Thesis/Dissertation ·
DOI:https://doi.org/10.2172/850147· OSTI ID:850147
 [1]
  1. Iowa State Univ., Ames, IA (United States)

The standard non-photochemical hole burning (NPHB) mechanism, which involves phonon-assisted tunneling in the electronically excited state, was originally proposed to explain the light-induced frequency change of chemically stable molecules in glassy solids at liquid helium temperatures by this research group more than two decades ago. The NPHB mechanism was then further elucidated and the concept of intrinsic to glass configurational relaxation processes as pre-mediating step to the hole burning process was introduced. The latter provided the theoretical basis for NPHB to evolve into a powerful tool probing the dynamics and nature of amorphous media, which aside from ''simple'' inorganic glasses may include also ''complex'' biological systems such as living cells and cancerous/normal tissues. Presented in this dissertation are the experimental and theoretical results of hole burning properties of aluminum phthalocyanine tetrasulphonate (APT) in several different matrices: (1) hyperquenched glassy water (HGW); (2) cubic ice (Ic); and (3) water confined into poly(2-hydroxyethylmethacrylate) (poly-HEMA). In addition, results of photochemical hole burning (PHB) studies obtained for phthalocyanine tetrasulphonate (PcT) in HGW and free base phthalocyanine (Pc) in ortho-dichlorobenzene (DCB) glass are reported. The goal of this dissertation was to provide further evidence supporting the NPHB mechanism and to provide more insight that leads to a better understanding of the kinetic events (dynamics) in glasses, and various dynamical processes of different fluorescent chromorphores in various amorphous solids and the liquid that exist above the glass transition temperature (Tg). The following issues are addressed in detail: (1) time evolution of hole being burned under different conditions and in different hole burning systems; (2) temperature dependent hole profile; and (3) the structure/dynamics of water in confined space, which has been studied, in part because of the importance of non-freezable water in biological systems.

Research Organization:
Ames Lab., Ames, IA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
DOE Contract Number:
W-7405-Eng-82
OSTI ID:
850147
Report Number(s):
IS-T 2674; TRN: US200614%%702
Country of Publication:
United States
Language:
English