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.
An experiment for studying a gas of atomic hydrogen at temperatures between 0.9 K and 1.3 K is described. The field dependence of the recombination rate of H atoms into H₂ molecules and the spin-exchange cross-section are investigated. Atoms are produced in situ in a low temperature discharge and are confined in a pyrex cell. The walls of this cell are covered with a film of superfluid ⁴He for preventing recombination. The detection and the study of the hydrogen atoms is done using the technique of pulsed magnetic resonance between the lowest two hyperfine levels of the 1s hydrogen atoms. The frequency is about 765.5 MHz and corresponds to a shallow minimum in the difference between the lowest two hyperfine levels, which occurs at 6481 kGauss. A simple model is also derived for explaining the field dependence of the recombination in the presence of a relatively large ⁴He density. In fact, due to the vapour pressure, the helium density will be above 10¹⁸ atoms/cm³ in the range of temperatures in which we are interested, while the density of hydrogen atoms will be about 10¹¹ -10¹² atoms/cm³. The relaxation mechanism assumed is spin-exchange. The parameters of the model are fit to the existing data. It is found in particular that the asymptotic behavior of the hyperfine populations depends sensitively on the initial populations.
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).
A calculation is presented of the relaxation rate ${{T}_{1}}^{\ensuremath{-}1}$ between the lowest two hyperfine states of a dilute gas of H atoms in high magnetic field at low temperatures. Dipole-dipole interactions dominate ${{T}_{1}}^{\ensuremath{-}1}$, leading to long relaxation times at low temperatures (${{T}_{1}}^{\ensuremath{-}1}\ensuremath{\approx}{10}^{\ensuremath{-}2}{n}_{\mathrm{H}}{T}^{\frac{1}{2}}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ at $H\ensuremath{\approx}100$ kG). The recombination rate due to wall collisions is much greater than ${{T}_{1}}^{\ensuremath{-}1}$ and can lead to a depletion of the lowest hyperfine state from thermal equilibrium and an effective recombination rate equal to ${{T}_{1}}^{\ensuremath{-}1}$.
The contents of this thesis include several experiments and a theory, the unifying theme of which is resonant recombination of atomic hydrogen (H) and deuterium (D) at low temperatures. Measurements of the interaction of H and D with the liquid helium (l-⁴He) wall coating used in low-temperature experiments are also included. Atomic hydrogen and deuterium were studied by ESR in a field of 41 kG at temperatures below 1 K, in a second generation of experiments on an existing apparatus. The binding energy of H on l-⁴He was measured, by direct observation of the physisorbed atoms, to be E[sub B]= 1.00(5) K. Extensive meaurements of recombination rate constants were made. Resonant recombination of H via the (v, J) = (14,4) level of H₂ was observed and identified. Atomic deuterium was also observed to recombine in a resonant process. At low temperatures, resonant recombination is possible due to the predissociation of weakly bound molecular levels by the intra-atomic hyperfine interaction. The theory of resonant recombination of H and D due to hyperfine predissociation is developed in detail. In order to keep the development self-contained, it is presented as appendix D of this thesis. The theory is combined with our ESR data in order to predict the magnetic-field dependence of resonant recombination of D. It is shown that observation of the threshold magnetic fields for resonant recombination will permit accurate measurement of the dissociation energy of the (v, J) = (21,0) and perhaps (21,1) levels of the D₂ molecule. An apparatus was constructed to study atomic deuterium by hyperfine magnetic resonance at temperatures near 1 K. The D atoms were produced from D₂ of 99.65% isotopic purity by an RF discharge in a bulb coated with a film of superfluid l-⁴He. Magnetic resonance in a field of 39 G on the longitudinal β-δ transition at its minimum frequency of 309 MHz was used to observe the atoms. The experiment was designed with the capability of measuring the recombination rate as a function of magnetic field for fields up to 30 kG by moving the sample between the 309 MHz resonator and a superconducting solenoid. A number of preliminary experiments were made using this apparatus. It was discovered that the D atom density decays away exponentially in time. The decay rate was measured as a function of temperature and found to follow an Arrhenius (thermally-activated) form, with an activation energy of about 15 K. No second-order decay was seen, permitting an upper bound to be placed on the D-D recombination rate. The exponential decay of the D atom density was due to the penetration by the atoms of the l-⁴He film coating their container. Our measurement of the temperature dependence of the density decay rate gives the energy required to dissolve a D atom in l-⁴He, Es[sub s] ≃ 14 K. This is the first experimental determination of this quantity. The longitudinal relaxation time T₁ for the β-δ transition was found to be too short to be due to D-D spin-exchange. It was conjectured that the sample was contaminated with substantial amounts of H, spin-exchange in H-D collisions causing the short T₁. Measurements in an existing 1420 MHz apparatus showed directly, by magnetic resonance on the hydrogen zero-field transition, that H atoms were, in fact, present. By varying the H concentration, we were able to show that the decay of the D density by was not due to recombination of H with D. Several attempts to substantially reduce the H impurity have failed. The penetration of the l-⁴He film is undoubtedly one reason why the D is so susceptible to contamination by H, since the film is permeable to D but not to H. For use in interpreting these experiments, the effects of spin-exchange relaxation on hyperfine resonance in mixtures of H and D were calculated.
Electron-spin resonance at 114 GHz is used to measure the three-body recombination rate (
L3) and the two-body surface relaxation rate (
G2s) for doubly-spin-polarized H between 100 and 200 mK. Our results for
L3 confirm and extend those of Cline, Greytak, and Kleppner. We find that
G2s is much smaller than previously reported and in reasonable agreement with theory. Around 100 mK, we also observe sidebands due to surface atoms whose frequency is shifted by dipole-dipole interactions.