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arXiv:1312.4270 · The Journal of Chemical Physics

Spin-polarized hydrogen adsorbed on the surface of superfluid 4He

J. M. Marín, Leandra Vranješ Markić, Jordi Boronat

Published Dec 13, 2013• 1 citation
arXivHTMLPDF

Abstract

The experimental realization of a thin layer of spin-polarized hydrogen H↓ adsorbed on top of the surface of superfluid (4)He provides one of the best examples of a stable, nearly two-dimensional (2D) quantum Bose gas. We report a theoretical study of this system using quantum Monte Carlo methods in the limit of zero temperature. Using the full Hamiltonian of the system, composed of a superfluid (4)He slab and the adsorbed H↓ layer, we calculate the main properties of its ground state using accurate models for the pair interatomic potentials. Comparing the results for the layer with the ones obtained for a strictly 2D setup, we analyze the departure from the 2D character when the density increases. Only when the coverage is rather small the use of a purely 2D model is justified. The condensate fraction of the layer is significantly larger than in 2D at the same surface density, being as large as 60% at the largest coverage studied.

DOI
10.1063/1.4843375

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•Jan 1, 2003•0 citations
The experimental realization of a thin layer of spin-polarized hydrogen H↓ adsorbed on top of the surface of superfluid (4)He provides one of the best examples of a stable, nearly two-dimensional (2D) quantum Bose gas. We report a theoretical study of this system using quantum Monte Carlo methods in the limit of zero temperature. Using the full Hamiltonian of the system, composed of a superfluid (4)He slab and the adsorbed H↓ layer, we calculate the main properties of its ground state using accurate models for the pair interatomic potentials. Comparing the results for the layer with the ones obtained for a strictly 2D setup, we analyze the departure from the 2D character when the density increases. Only when the coverage is rather small the use of a purely 2D model is justified. The condensate fraction of the layer is significantly larger than in 2D at the same surface density, being as large as 60% at the largest coverage studied.
The binding energy of a hydrogen atom to the surface of liquid 4He has been calculated to be at least 0.6K by Mantz and Edwards. This means that the properties of adsorbed spin-polarized hydrogen (H↑), a 2D Bose fluid, may soon be observed experimentally. Since 4He is used as a neutral coating for vessels to contain H↑ gas, adsorption onto the 4He surface may enhance the rate of recombination into H2 molecules. For given temperature and density in the gas, the amount of H↑ adsorbed depends strongly on the H↑-H↑ interaction on the 4He surface. We estimate the interaction in a simple approximation, and find that it limits the surface density to not more than 1014 cm-2. Nevertheless this density should be sufficient for a 2D superfluid transition to be observed, under conditions close to those achieved experimentally.
We review the recent activity in the theoretical description of spin-polarized atomic hydrogen and its isotopes at very low temperatures. Spin-polarized hydrogen is the only system in nature that remains stable in the gas phase even in the zero temperature limit due to its small mass and weak interatomic interaction. Hydrogen and its heavier isotope tritium are bosons, the heavier mass of tritium producing a self-bound (liquid) system at zero temperature. The other isotope, deuterium, is a fermion with nuclear spin one making possible the study of three different quantum systems depending on the population of the three degenerate spin states. From the theoretical point of view, spin-polarized hydrogen is specially appealing because its interatomic potential is very accurately known making possible its precise quantum many-body study. The experimental study of atomic hydrogen has been very difficult due to its high recombination rate, but it finally led to its Bose-Einstein condensate state in 1998. Degeneracy has also been observed in thin films of hydrogen adsorbed on the 4He surface allowing for the possibility of observing the Berezinskii–Kosterlitz–Thouless superfluid transition.
We study three-body recombination in the gas of spin-polarized atomic hydrogen adsorbed on the surface of superfluid helium at temperatures from 45to130mK45\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}130\phantom{\rule{0.3em}{0ex}}\mathrm{mK}45to130mK. The two-dimensional gas is thermally compressed to densities up to $\ensuremath{\approx}4\ifmmode\times\else\texttimes\fi{}{10}^{12}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$ using the ``cold spot'' method which makes the three-body process the dominant decay channel in the system. We measure the loss rate and surface density of atoms directly and independently and observe the former to be proportional to the third power of the latter. The result for the surface three-body recombination rate constant at 4.6T4.6\phantom{\rule{0.3em}{0ex}}\mathrm{T}4.6T, ${L}_{s}=2.0(7)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}25}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{4}∕\mathrm{s}$, significantly reduces the discrepancy between the theory and earlier measurements where the surface density was inferred from the adsorption isotherm. We also measured the three-body rate constant on a 0.1% $^{3}\mathrm{He}\text{\ensuremath{-}}^{4}\mathrm{He}$ film and found ${L}_{s}=1.3(4)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}24}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{4}∕\mathrm{s}$. This larger value is attributed to an increased delocalization of adsorbed hydrogen atoms in the direction normal to the surface.
Experimental results on the achievement of high degrees of quantum degeneration in two-dimensional atomic hydrogen (2D H↓) by the magnetic-compression method are analyzed by taking into account current data on the binding energy E a = 1.14(1) K of hydrogen atoms with the 4He surface and the constant K ab of the two-particle exchange recombination of adsorbed H atoms. The behavior of pair and three-particle correlation functions, as well as the transverse delocalization of the wavefunction of adsorbed atoms due to their interaction with each other, is taken into account self-consistently. A new mechanism of cooling of the compression region by means of the flow of H atoms on the helium surface with the subsequent evaporation and emission from a magnetic trap is proposed. This mechanism prevails at high densities, whereas the heat transfer at low densities occurs owing mainly to the interaction of ripplons with the phonons of the helium film. Existing data corroborate the achievement of the phase density σλ2 ≳ 10, which is certainly higher than the density necessary for both the arrangement of local coherence in 2D H↓ and its transition to the superfluid state. The results agree with the representations on quasi-condensation; however, direct evidence of this phenomenon is not revealed. The probability of three-particle dipole recombination that is corrected for the quantum correlation and delocalization is equal to 7(2) × 10−26 cm4 s−1 (T = 0.15, …, 0.21 K, B = 6.6 T, and σλ2 = 1, …, 9). The results are compared with other theoretical and experimental data.
Path Integral Monte Carlo was used to calculate the Bose-Einstein condensate fraction at the surface of a helium film at T = 0:77 K, as a function of density. Moving from the center of the slab to the surface, the condensate fraction was found to initially increase with decreasing density to a maximum value of 0.9, before decreasing. Long wavelength density correlations were observed in the static structure factor at the surface of the slab. A surface dispersion relation was calculated from imaginary-time density-density correlations. Similar calculations of the superfluid density throughout He-4 droplets doped with linear impurities (HCN)(sub n) are presented. After deriving a local estimator for the superfluid density distribution, we find a decreased superfluid response in the first solvation layer. This effective normal fluid exhibits temperature dependence similar to that of a two-dimensional helium system.