In sufficiently large magnetic fields, the weakly bound levels of H2 acquire finite lifetimes owing to hyperfine predissociation and become manifest as scattering resonances in spin-polarized atomic hydrogen (H↓). In this work we investigate in detail the contribution to the reaction kinetics in H↓ due to the resonance, denoted [Formula: see text], arising from the predissociation of the (v,J) = (14,4) level of H2. To characterize the formation and disintegration of [Formula: see text], we calculate the predissociation as a function of both the applied magnetic field and the dissociation energy, D, of the level. Recombination occurs when [Formula: see text] is stabilized in collisions that cause transitions to lower molecular levels. For low H↓, densities, collisions with atoms of the saturated 4He vapour dominate; we calculate the cross section in the distorted wave Born approximation and also use a coupled-channels approach. At higher densities, stabilization occurs in collisions with H↓ as well; the effect of proton exchange between the atom and the molecule is derived. Previous experiments, analyzed neglecting proton exchange, are reanalyzed including this; the dissociation energy D is not as well determined by the data as was previously thought. Prospects for future experiments are discussed.
We have studied relaxation and recombination processes in compressed, doubly polarized atomic hydrogen at temperatures from 0.13 to 0.60 K and magnetic fields from 3 to 9 T. The gas and surface dipole three-body recombination rate constants at a field of 7.6 T are measured to be, respectively,
Lg=8.9(8)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}39}$
cm6 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ and
Ls=1.2(4)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}24}$
cm4 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$. They decrease slowly with field and
Ls exhibits no significant angular dependence. The three-body recombination rate due to hyperfine mixing has also been measured. Electronic and nuclear relaxation rates have been measured; the b-c electronic relaxation rate constant in the gas is
Gbc=1.03(7)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}15}$
cm3 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$exp(-
Ebc/
kBT). The temperature and field dependence of the nuclear relaxation rate in the gas are observed to be in excellent agreement with recent theoretical calculations. Three-body surface recombination-rate measurements using $^{3}\mathrm{\ensuremath{-}}^{4}$He surfaces indicate that as little as one monolayer of
3He on the liquid
4He surface appreciably decreases the adsorption energy of atomic hydrogen. Densities achieved include 4.5\ifmmode\times\else\texttimes\fi{}
1018 atoms${\mathrm{?}}^{\mathrm{\ensuremath{-}}3}$ at 0.55 K (pure
4He walls), and 1.4\ifmmode\times\else\texttimes\fi{}
1018 atoms${\mathrm{?}}^{\mathrm{\ensuremath{-}}3}$ at 0.19 K (8 at. ? sup 3---He).
The three-body recombination rate in spin-polarized hydrogen has been measured at temperatures from 0.25 to 0.60 K in magnetic fields from 5 to 9 T. In contrast to theoretical expectation, the three-body rate is a weakly decreasing function of field in this region. At 7.6 T the gas and surface three-body rate constants are ${L}_{g}=7.5(3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}39}$
cm6 ${\mathrm{s}}^{\ensuremath{-}1}$ and ${L}_{s}=2.0(6)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}24}$
cm4 ${\mathrm{s}}^{\ensuremath{-}1}$. The large value of
Ls can account for effects previously attributed to an anomalously large surface two-body nuclear relaxation rate.
In this thesis we describe the results of two sets of experiments on spin-polarized atomic hydrogen at temperatures below 1 K using a 115 GHz heterodyne ESR spectrometer. First, we have made measurements of the rates of the two-body recombination processes in spin-polarized atomic hydrogen gas and spin-polarized atomic deuterium gas in a 41 kG field. In the second set of experiments, we examined the ESR absorption line associated with the spin-polarized atomic hydrogen atoms adsorbed on surfaces of liquid helium. In hydrogen, a comparision of the measured recombination rates in 41 kG with the corresponding rates measured in different magnetic fields showed that an additional recombination process is activate for the conditions of these experiments. We demonstrate that this is due to a resonant recombination process via the (v,J) = (14,4) level of molecular hydrogen. In spin-polarized deuterium, we found that the recombination rate are much larger than the analogous rates in hydrogen, and therefore that atomic deuterium gas is much less stable than the hydrogen system under comparable conditions. We report the first observation and study of doubly spin-polarized deuterium, a gas in which both the deuteron and electron spins are aligned. At temperatures near 0.1 K, the absorption line of doubly spin-polarized H atoms changes drastically as a peak appears on both sides of the peak associated with the bulk atoms. We have shown that these new peaks are due to the atoms which are adsorbed onto the surface of the liquid helium film that coats the walls of the microwave cavity. The geometry dependent non-zero average magnetic dipolar field due to aligned spins on a planar surface results in a shift of the position of the ESR absorption lines. The lineshapes of the side peaks are very unusual and are best described as ramp-like. Even after extensive attempts to explain this lineshape, we still do not know what mechanism is responsible.
Spin-aligned hydrogen (H \ensuremath{\uparrow}) and deuterium (D \ensuremath{\uparrow}) are generally predicted to be stable for $\frac{\mathcal{H}}{T}\ensuremath{\gtrsim}{10}^{6}$ G/K. Magnetic-field-dependent resonances (inverse to field-induced predissociations of high vibrational-rotational levels of HD and
D2) provide exceptions to this general rule. Their existence suggests 50 kG (H \ensuremath{\uparrow} + D \ensuremath{\uparrow}) and 19 kG (D \ensuremath{\uparrow} + D \ensuremath{\uparrow}) should be avoided for stable H \ensuremath{\uparrow} and D \ensuremath{\uparrow}. Induced predissociation observations should yield ultraprecise resonance information and dissociation limits.