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Physical Review Letters

Orbital Angular Momentum Exchange in the Interaction of Twisted Light with Molecules

M. Babiker, C. R. Bennett, Davıd L. Andrews, Luciana C. Dávila Romero

Published Sep 11, 2002• 278 citations
Publisher

Abstract

In the interaction of molecules with light endowed with orbital angular momentum, an exchange of orbital angular momentum in an electric dipole transition occurs only between the light and the center of mass motion; i.e., internal "electronic-type" motion does not participate in any exchange of orbital angular momentum in a dipole transition. A quadrupole transition is the lowest electric multipolar process in which an exchange of orbital angular momentum can occur between the light, the internal motion, and the center of mass motion. This rules out experiments seeking to observe exchange of orbital angular momentum between light beams and the internal motion in electric dipole transitions.

DOI
10.1103/physrevlett.89.143601

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In the interaction of molecules with light endowed with orbital angular momentum, an exchange of orbital angular momentum in an electric dipole transition occurs only between the light and the center of mass motion; i.e., internal "electronic-type" motion does not participate in any exchange of orbital angular momentum in a dipole transition. A quadrupole transition is the lowest electric multipolar process in which an exchange of orbital angular momentum can occur between the light, the internal motion, and the center of mass motion. This rules out experiments seeking to observe exchange of orbital angular momentum between light beams and the internal motion in electric dipole transitions.
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Recent experiments involving the interaction of optical vortices with atoms in quadrupole transitions have shown it to be accompanied by the exchange of orbital angular momentum (OAM) between the electronic states of the atom and the optical vortex field. Earlier work, both theoretical and experimental, had ruled out the transfer of a vortex OAM to the electronic degrees of freedom in an electric dipole atomic transition and it has been confirmed that the lowest multipolar order involving an OAM transfer to the electronic motion is indeed the electric quadrupole. Hitherto, the quadrupole transition involving optical vortices has not been quantified and we thus set out to evaluate the absorption rate accompanied by an OAM transfer with reference to the $6^{2}S_{1/2}\ensuremath{\rightarrow}5^{2}D_{5/2}$ in Cs when cesium atoms are subject to the field of a linearly polarized optical vortex. Our results assuming typical experimentally accessible parameters indicate that the absorption rate for moderate light intensities is lower than the quadrupole spontaneous emission rate but should still be within the measurement capabilities of modern spectroscopic techniques.
We derive the interaction Hamiltonian between a diatomic molecule and a Laguerre-Gaussian beam under the assumption of a small spread of the center of mass wave function of the molecule in comparison with the beam waist. Considering the dynamical variables of the center of mass, vibrational, rotational, and electronic motion, we show that, within the electronic dipole approximation, the orbital angular momentum of the field couples with the rotational and electronic motion. The changes in the transition probabilities and selection rules induced by the field orbital angular momentum and the applicability of the derived interaction mechanisms for polyatomic molecules are discussed.
Twisted light beams, or optical vortices, have been used to drive the circular motion of microscopic particles in optical tweezers and have been shown to generate vortices in quantum gases. Recent studies have established that electric quadrupole interactions can mediate an orbital angular momentum exchange between twisted light and the electronic degrees of freedom of atoms. Here we consider a quadrupole atomic transition mediated by a circularly-polarized optical vortex. We evaluate the transfer rate of the optical angular momentum to a Ca+ ion involving the 42S1∕2→32D5∕2 quadrupole transition and explain how the polarization state and the topological charge of the vortex beam determine the selection rules.