H/D isotope effects in water radiolysis. 1. Chemically induced dynamic electron polarization of spurs
Journal Article
·
· Journal of Physical Chemistry; (USA)
- Argonne National Lab., IL (USA)
The authors report pulsed electron paramagnetic resonance (EPR) measurements of atomic hydrogen and deuterium magnetization at 30-50 ns after radiolysis of aqueous solutions with short pulses of 3-MeV electrons. The H and D EPR spectra are strongly polarized by radical pair mechanism chemically induced dynamic electron polarization (RPM CIDEP) generated by spin-dependent recombination reactions in radiolysis spurs. The amplitude of the initial H and D magnetization has been measured as a function of pH (pD) and N{sub 2}O saturation in both H{sub 2}O and D{sub 2}O. The major polarization mechanisms are identified as (a) H + H (or D + D) CIDEP, (b) H (or D) + e{sub aq}{sup {minus}} -CIDEP, (c) fast OH thermal relaxation followed by Heisenberg spin exchange with H (or D), and OH, e{sub aq}{sup {minus}} spin exchange followed by reaction of e{sub aq}{sup {minus}} with H{sub 3}O{sup +} (or D{sub 3}O{sup +}) to give H (or D). A crude model of the polarization dynamics based on a diffusion kinetics description of the spur chemistry is proposed and evaluated. It is concluded that the observations can be accounted for with the standard theories of RPM CIDEP and Heisenberg spin exchange.
- DOE Contract Number:
- W-31109-ENG-38
- OSTI ID:
- 5110468
- Journal Information:
- Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 93:6; ISSN 0022-3654; ISSN JPCHA
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
400600* -- Radiation Chemistry
AQUEOUS SOLUTIONS
BEAMS
CHEMICAL RADIATION EFFECTS
CHEMICAL REACTIONS
CHEMISTRY
DATA
DECOMPOSITION
DIFFUSION
DISPERSIONS
ELECTRON BEAMS
ELECTRON SPIN RESONANCE
ELECTRONS
ELEMENTARY PARTICLES
ENERGY RANGE
EXPERIMENTAL DATA
FERMIONS
HEAVY WATER
HYDROGEN COMPOUNDS
INFORMATION
IRRADIATION
LEPTON BEAMS
LEPTONS
MAGNETIC RESONANCE
MAGNETIZATION
MEV RANGE
MEV RANGE 01-10
MIXTURES
NUMERICAL DATA
OXYGEN COMPOUNDS
PARTICLE BEAMS
POLARIZATION
PULSED IRRADIATION
RADIATION CHEMISTRY
RADIATION EFFECTS
RADIOLYSIS
RESONANCE
SOLUTIONS
WATER
400600* -- Radiation Chemistry
AQUEOUS SOLUTIONS
BEAMS
CHEMICAL RADIATION EFFECTS
CHEMICAL REACTIONS
CHEMISTRY
DATA
DECOMPOSITION
DIFFUSION
DISPERSIONS
ELECTRON BEAMS
ELECTRON SPIN RESONANCE
ELECTRONS
ELEMENTARY PARTICLES
ENERGY RANGE
EXPERIMENTAL DATA
FERMIONS
HEAVY WATER
HYDROGEN COMPOUNDS
INFORMATION
IRRADIATION
LEPTON BEAMS
LEPTONS
MAGNETIC RESONANCE
MAGNETIZATION
MEV RANGE
MEV RANGE 01-10
MIXTURES
NUMERICAL DATA
OXYGEN COMPOUNDS
PARTICLE BEAMS
POLARIZATION
PULSED IRRADIATION
RADIATION CHEMISTRY
RADIATION EFFECTS
RADIOLYSIS
RESONANCE
SOLUTIONS
WATER