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Theory of the magnetic resonance spectrum of spin-polarized hydrogen gas

Zhou, Haosheng

Published Jan 1, 2010• 1 citation
Publisher

Abstract

The Green's function method is applied to investigate the magnetic spin resonance spectra of three-dimensional and two-dimensional spin-polarized quantum gases. The Hartree-Fock approximation is employed to calculate the one-particle Green's function of the atoms, then this one-particle Green's function is used for the calculation of the vertex part of the Green's function. Such a combination yields a self-consistent result. The absorption spectra are obtained from the calculation of the susceptibility in terms of the two-particle Green's function (bubble diagram). Some general expressions for the dispersion relation, for the effective mass of a spin wave, and for the dipolar frequency shift are given in the calculation. In order to estimate the shift of the electron-spin-resonance (ESR) frequency, the effective dipole-dipole interactions among the hydrogen atoms are included in the calculation. These effective interactions are deduced from the ladder approximation, and hence are characterized by the scattering amplitude. The scattering amplitude is calculated numerically. The result shows that the theoretical value of the shift is smaller than the experimentally observed value by about 35%.

DOI
10.14288/1.0097151

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The Green's function method is applied to investigate the magnetic spin resonance spectra of three-dimensional and two-dimensional spin-polarized quantum gases. The Hartree-Fock approximation is employed to calculate the one-particle Green's function of the atoms, then this one-particle Green's function is used for the calculation of the vertex part of the Green's function. Such a combination yields a self-consistent result. The absorption spectra are obtained from the calculation of the susceptibility in terms of the two-particle Green's function (bubble diagram). Some general expressions for the dispersion relation, for the effective mass of a spin wave, and for the dipolar frequency shift are given in the calculation. In order to estimate the shift of the electron-spin-resonance (ESR) frequency, the effective dipole-dipole interactions among the hydrogen atoms are included in the calculation. These effective interactions are deduced from the ladder approximation, and hence are characterized by the scattering amplitude. The scattering amplitude is calculated numerically. The result shows that the theoretical value of the shift is smaller than the experimentally observed value by about 35%.
We present an experimental study of the quantum gas of atomic hydrogen in a strong magnetic field (4.6 T). The gas is compressed to densities of ~1018 cm−3 at temperatures of 0.2–0.5 K. We observed shifts of the electron spin resonance (ESR) lines caused by the exchange interaction in atomic collisions (clock shift) and the long-range dipolar interactions. The clock shift was found to be vanishingly small in a doubly polarized gas, in contrast to a mixture of two hyperfine states. The difference is explained by properly including quantum statistical effects in the treatment of atomic collisions. From our data, we extract the difference between the triplet and singlet s-wave scattering lengths, at−as=60(10) pm, in agreement with existing theories. At densities above 1017 cm−3, weakly resolved structures appeared in the ESR spectra, interpreted in terms of electron spin waves. We consider exchange and dipolar interactions to possibly induce the spin waves.
In this thesis three experiments with atomic hydrogen (H) at low temperatures T<1 K are presented. Experiments were carried out with two- (2D) and three-dimensional (3D) H gas, and with H atoms trapped in solid H2 matrix. The main focus of this work is on interatomic interactions, which have certain specific features in these three systems considered. A common feature is the very high density of atomic hydrogen, the systems are close to quantum degeneracy. Short range interactions in collisions between atoms are important in gaseous H. The system of H in H2 differ dramatically because atoms remain fixed in the H2 lattice and properties are governed by long-range interactions with the solid matrix and with H atoms. The main tools in our studies were the methods of magnetic resonance, with electron spin resonance (ESR) at 128 GHz being used as the principal detection method. For the first time in experiments with H in high magnetic fields and at low temperatures we combined ESR and NMR to perform electron-nuclear double resonance (ENDOR) as well as coherent two-photon spectroscopy. This allowed to distinguish between different types of interactions in the magnetic resonance spectra. Experiments with 2D H gas utilized the thermal compression method in homogeneous magnetic field, developed in our laboratory. In this work methods were developed for direct studies of 3D H at high density, and for creating high density samples of H in H2. We measured magnetic resonance line shifts due to collisions in the 2D and 3D H gases. First we observed that the cold collision shift in 2D H gas composed of atoms in a single hyperfine state is much smaller than predicted by the mean-field theory. This motivated us to carry out similar experiments with 3D H. In 3D H the cold collision shift was found to be an order of magnitude smaller for atoms in a single hyperfine state than that for a mixture of atoms in two different hyperfine states. The collisional shifts were found to be in fair agreement with the theory, which takes into account symmetrization of the wave functions of the colliding atoms. The origin of the small shift in the 2D H composed of single hyperfine state atoms is not yet understood. The measurement of the shift in 3D H provides experimental determination for the difference of the scattering lengths of ground state atoms. The experiment with H atoms captured in H2 matrix at temperatures below 1 K originated from our work with H gas. We found out that samples of H in H2 were formed during recombination of gas phase H, enabling sample preparation at temperatures below 0.5 K. Alternatively, we created the samples by electron impact dissociation of H2 molecules in situ in the solid. By the latter method we reached highest densities of H atoms reported so far, 3.5(5)x1019 cm-3. The H atoms were found to be stable for weeks at temperatures below 0.5 K. The observation of dipolar interaction effects provides a verification for the density measurement. Our results point to two different sites for H atoms in H2 lattice. The steady-state nuclear polarizations of the atoms were found to be non-thermal. The possibility for further increase of the impurity H density is considered. At higher densities and lower temperatures it might be possible to observe phenomena related to quantum degeneracy in solid.
The problem of the many-body enhancement of the static spin susceptibility at long wavelengths and its relation to the quasiparticle effective mass is investigated for a normal electron gas in two-dimensional space as a function of the electronic density. We start from a discussion of the results of the simple Hartree-Fock approximation for various interaction potentials and proceed to develop a complete theory. We find that the effects of the electron-electron interaction are significantly larger than in the familiar three-dimensional case. Our approach is based on a new self-consistent scheme which goes beyond the simple random-phase approximation by explicitly allowing for charge- and spin-fluctuation-induced vertex corrections of the Hubbard type. We show that when the latter are neglected, the many-body enhancement of the spin susceptibility can be cast in a remarkably simple and elegant analytic form.
A simple calculation of the wave-vector- and frequency-dependent paramagnetic spin susceptibility of an interacting electron gas is presented. The equation of motion of the double-time Green's function is solved using a moment-conserving decoupling approximation. For the short-range interaction, our expression for the dynamic spin susceptibility reduces to a previous result of Wolff. In the static and long-wavelength limit, our result for the Stonerenhanced spin susceptibility coincides with that obtained from consideration of the groundstate energy in the Hartree-Fock approximation.
We have measured electron spin resonance line shifts due to collisions in atomic hydrogen gas compressed to densities approximately 10(18) cm(-3) in a strong magnetic field (4.6 T). The shift in a doubly polarized gas is negligible, in contrast with a mixture of two hyperfine states. This difference is explained by properly including effects of quantum statistics in atomic collisions and magnetic dipolar effects. We report on the first direct measurement of the difference between the triplet and singlet s-wave scattering lengths a(t) - a(s) = 60(10) pm, which is in agreement with existing theories.
The energy levels of hydrogen and helium atoms in strong magnetic fields are calculated in this study. The current work contains estimates of the binding energies of the first few low-lying states of these systems that are improvements upon previous estimates. The methodology involves computing the eigenvalues and eigenvectors of the generalized two-dimensional Hartree-Fock partial differential equations for these one- and two-electron systems in a self-consistent manner. The method described herein is applicable to calculations of atomic structure in magnetic fields of arbitrary strength as it exploits the natural symmetries of the problem without assumptions of any basis functions for expressing the wave functions of the electrons or the commonly employed adiabatic approximation. The method is found to be readily extendable to systems with more than two electrons.