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Physica Scripta

Laser preparation of spin-polarized atoms from molecular photodissociation

L. Rubio Lago, Dimitris Sofikitis, Antonis Koubenakis, Theodore Peter Rakitzis

Published Dec 22, 2005• 4 citations
Publisher

Abstract

We discuss how nuclear spin can be highly polarized from the transfer of molecular rotational polarization via the hyperfine interaction, and how large atomic electronic polarization can be produced via molecular photodissociation with polarized light. In combination, these two pulsed-laser techniques can be used to produce highly polarized atoms at densities close to the density of the parent molecules. We compare these methods to existing methods for producing polarized atoms and present specific examples.

DOI
10.1088/0031-8949/73/1/n13

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We describe methods for the production of spin-polarized H and D atoms from the IR-excitation and photodissociation of molecular beams of HBr, HI, and NH3{\rm NH_{3}}NH3​ isotopes, including optical excitation schemes with partial hyperfine resolution. We discuss the extent to which the production rates may approach the IR-laser production rates of 1021 photons s−1{\rm 10^{21}\, photons\, s^{-1}}1021photonss−1, and how the production rates of conventional methods of ∼1017 s−1{\sim}{\rm 10^{17} \, s^{-1}}∼1017s−1 may be surpassed significantly.
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We propose laser-based methods for the production of nuclear spin hyperpolarized molecules. Following pulsed, coherent excitation from ground-state molecules in a molecular beam to specific rotational $|J\phantom{\rule{0.16em}{0ex}}{m}_{J}\ensuremath{\rangle}$ states, the resulting hyperfine polarization beating produces desirable nuclear spin mI{m}_{I}mI​ population distributions and ${m}_{I}\ensuremath{-}{m}_{J}$ correlations at specific later times. At this point, selective dissociation can be used to remove undesired spin states, or a strong magnetic field can be applied, which later can be removed adiabatically to transfer the population-enhanced nuclear spin configurations to the desired nuclear spin state. Finally, the polarization beating is stopped, and the molecules are stored by cryogenic trapping. We show how these methods can be used to produce the long-lived singlet state of 15N2O^{15}\mathrm{N}_{2}\mathrm{O}15N2​O and ortho H2O{\mathrm{H}}_{2}\mathrm{O}H2​O, which have been proposed as magnetic tracers. We discuss how large production rates between 1 and $100 \ensuremath{\mu}\mathrm{mol}$/s with singlet-state populations between 35% and 100% can be achieved.
Nuclear spin polarization has important applications across various fields, including physics andmedicine. It also offers several advantages, such as cross-section enhancement, in the five-nucleonfusion reactions, namely the D–T and D–3^33He reactions. This work presents a theoretical studyof spin dynamics in the hyperfine regime for selected atomic and molecular systems and exploresalternative techniques to generate or enhance nuclear spin polarization in these systems. Particularemphasis is placed on coherent spin manipulation strategies and the role of hyperfine interactions intransferring angular momentum from electronic (in atoms) or rotational (in molecules) to nucleardegrees of freedom.
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