For molecular systems, spin relaxation is expected to be suppressed compared to the case of atoms, since the paired electrons in a hydrogen or deuterium molecule are chemically stable, and only weakly interact with the spin of the nucleus. Such systems would be largely insensitive to polarization losses due to spin-exchange collisions, to the interaction of the electron spins with external fields (e.g. the RF-field of a bunched charged-particle beam), and/or to the presence of container walls. Here, we discuss the results of a recent experiment where we obtained evidence that nuclear polarization is maintained, when polarized atoms recombine to molecules on a copper surface (in a magnetic field of 23 mT and at a density of about 1012 molecules⋅cm−3).
Polarized atomic beam sources have been in operation for many years to produce either nuclear polarized atomic hydrogen or deuterium beams. In recent experiments, such a source was used to polarize both isotopes independently at the same time. By recombination of the atoms, hydrogen-deuterium molecules with all possible nuclear spin combinations can be created. Those spin isomers are useful for further applications, like precision spectroscopy, as polarized targets for laser-particle acceleration, polarized fuel for fusion reactors, or as an option for future measurements of electric dipole moments.
We analyze and reinterpret experiments with electron- and nuclear-spin (``doubly'')-polarized hydrogen (H\ensuremath{\downarrow}?) in a cell with a very low concentration of magnetic impurities. The destabilizing magnetic relaxation due to remaining impurities (
Gis) is found to be suppressed by increasing the thickness of the helium film covering the walls of the cell. Using recent information on surface three-body recombination, we obtain good quantitative agreement with more recent experiments if we assume thermal gradients, up to \ensuremath{\Delta}T/T\ensuremath{\simeq}0.1. We extract both the value and field dependence for the three-body surface recombination [
L3s=1.5(2)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}24}$
cm4 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ at B=8 T]. We also extract the magnetic field dependence of the impurity relaxation.
The electron polarization of hydrogen (H) and deuterium (D) atoms in a spin-exchange optical-pumping apparatus has been measured as a function of H (D) density and magnetic-field strength. The atomic density was varied between 4\ifmmode\times\else\texttimes\fi{}
1013 and 2.6\ifmmode\times\else\texttimes\fi{}
1014 atoms/
cm3 and the magnetic-field strength from 120 to 400 mT. The results suggest that the atoms approach spin-temperature equilibrium even though the magnetic fields are large compared to the critical fields of the atoms.
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).
We study the polarization dynamics of the molecular rotation and the nuclear spin in the presence of magnetic fields, in the hydrogen isotope molecules,
H2,D2, and HD. If only the rotational or the nuclear angular momentum is polarized, polarization is transferred from one to the other and back in a oscillatory fashion, due to hyperfine quantum beats. Application of magnetic fields is shown to increase the frequencies of these oscillations and reduce their amplitude so that the polarization exchange can be strongly suppressed. We derive the time-averaged polarization as a function of the (static) magnetic field. Finally, we show, using continuous lasers, molecular beams, and static magnetic fields, that the molecular rotation polarization can be transferred and maintained in the nuclear spin, providing highly nuclear-spin-polarized molecules.
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.