FDMR in low-temperature solids. 1. Theory

Journal Article · Thu Dec 15 04:00:00 EST 1994 · Journal of Physical Chemistry; (United States)

DOI:https://doi.org/10.1021/j100101a027· OSTI ID:6617653

Shkrob, I A; Trifunac, A D ^[1]

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1. Argonne National Lab., IL (United States)

Various mechanisms of geminate recombination in spin-correlated radical ion pairs produced by radiolysis of organic solids under cryogenic conditions are considered and compared with experimental data. Single-step electron tunneling and slow resonant hole transfer are examined from the viewpoint of their manifestation in pulsed time-resolved fluorescence-detected magnetic resonance (FDMR). Two theoretical models treating the phenomenon are developed, and their predictions are compared with the experimental results. These models are found to be consistent with many observed features: t[sup [minus]1] decay kinetics, unusual evolution of the FDMR spectra with time, narrow radial distribution of the FDMR-active pairs, and efficient spin memory transfer from the primary pairs. However, with very few exceptions the tunneling theories fail to reproduce the exact scale of the effect and its dependence on solute concentration and thermalization distance of electrons. This discrepancy suggests that the negative charge is more mobile than predicted by the single-step tunneling model. 31 refs., 8 figs.

• OSTI ID: 6617653
• Journal Information: Journal of Physical Chemistry; (United States), Journal Name: Journal of Physical Chemistry; (United States) Vol. 98:50; ISSN JPCHAX; ISSN 0022-3654
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
400102 -- Chemical & Spectral Procedures
400201* -- Chemical & Physicochemical Properties
400600 -- Radiation Chemistry
99 GENERAL AND MISCELLANEOUS
990200 -- Mathematics & Computers
CHARGE TRANSPORT
CHARGED PARTICLES
CHEMICAL RADIATION EFFECTS
CHEMICAL REACTIONS
CRYOGENICS
DECOMPOSITION
DEUTERIUM
ELECTRON TRANSFER
FLUORESCENCE
HYDROGEN ISOTOPES
IONS
ISOTOPE EFFECTS
ISOTOPES
LIGHT NUCLEI
LUMINESCENCE
MAGNETIC RESONANCE
MATHEMATICAL MODELS
NUCLEI
ODD-ODD NUCLEI
ORGANIC COMPOUNDS
RADIATION EFFECTS
RADICALS
RADIOLYSIS
RECOMBINATION
RESONANCE
SPECTROSCOPY
STABLE ISOTOPES
TUNNEL EFFECT