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arXiv:2203.03742 · Journal of Physics A Mathematical and Theoretical

Optical angular momentum in atomic transitions: a paradox

Stephen Mark Barnett, Fiona C. Speirits, Mohamed Babiker

Published Apr 29, 2022• 12 citations
arXivHTMLPDF

Abstract

Abstract Stated simply the paradox is as follows: it is clear that the orbital angular momentum of a light beam in its direction of propagation is an intrinsic quantity, and therefore has the same value everywhere in the beam. How then can a Gaussian beam, with precisely zero orbital angular momentum, drive a (single-photon) quadrupole transition which requires the transfer of angular momentum 2ℏ to an absorbing atom?

DOI
10.1088/1751-8121/ac6bd1

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Cambridge University Press eBooks•Nov 8, 2012•0 citations
Abstract Stated simply the paradox is as follows: it is clear that the orbital angular momentum of a light beam in its direction of propagation is an intrinsic quantity, and therefore has the same value everywhere in the beam. How then can a Gaussian beam, with precisely zero orbital angular momentum, drive a (single-photon) quadrupole transition which requires the transfer of angular momentum 2ℏ to an absorbing atom?
The exchange of orbital angular momentum between a Laguerre-Gaussian beam of light and the center-of-mass motion of an atom or molecule is well known. We show that the orbital angular momentum of light can also be transferred to the internal electronic or rotational motion of an atom or a molecule provided the internal and center-of-mass motions are coupled. However, this transfer does not happen directly to the internal motion, but via center-of-mass motion. If atoms or molecules are cooled down to the recoil limit, then an exchange of angular momentum between the quantized center-of-mass motion and the internal motion is possible during the interaction of cold atoms or molecules with the Laguerre-Gaussian beam. The orientation of the exchanged angular momentum is determined by the sign of the winding number of the Laguerre-Gaussian beam. We present selective results of numerical calculations for the quadrupole transition rates in the interaction of the Laguerre-Gaussian beam with an atomic Bose-Einstein condensate to illustrate the underlying mechanism of light orbital angular momentum transfer. We discuss how the alignment of diatomic molecules will facilitate exploration of the effects of light orbital angular momentum on the electronic motion of molecules.
We generated orbital angular momentum in atoms with a spin degree of freedom and coherently transferred it to a light field, which resulted in the generation of a Laguerre-Gaussian (LG) beam. In this method, atoms obtain orbital angular momentum through Larmor precession around the quadrupole field. Successive operations of quadrupole and homogeneous magnetic fields lead to a change of sign in the LG beam or even generation of superposition states of the LG beam with different indexes in real time. Possible applications to control orbital angular momentum of arbitrary photons are also discussed.
Photons carry one unit of angular momentum associated with their spin~\cite{Beth1936}. Structured vortex beams carry additional orbital angular momentum which can also be transferred to matter~\cite{Allen1992}. This extra twist has been used for example to drive motion of microscopic particles in optical tweezers as well as to create vortices in degenerate quantum gases~\cite{He1995,Andersen2006}. Here we demonstrate the transfer of optical orbital angular momentum from the transverse spatial structure of the beam to the internal (electronic) degrees of freedom of an atom. Probing a quadrupole transition of a single trapped 40^{40}40Ca+^++ ion localized at the center of the vortex, we observe strongly modified selection rules, accounting for both the photon spin and the vorticity of the field. In particular, we show that an atom can absorb two quanta of angular momentum from a single photon even when rotational symmetry is conserved. In contrast to previous findings~\cite{Araoka2005,Loeffler2011a,Mathevet2013}, our experiment allows for conditions where the vorticity of the laser beam determines the optical excitation, contributing to the long-standing discussion on whether the orbital angular momentum of photons can be transferred to atomic internal degrees of freedom~\cite{VanEnk1994,Babiker2002,Jauregui2004, Schmiegelow2012, Mondal2014, Scholz-Marggraf2014} and paves the way for its use to tailor light-matter interactions.
Photons can carry angular momentum, not only due to their spin, but also due to their spatial structure. This extra twist has been used, for example, to drive circular motion of microscopic particles in optical tweezers as well as to create vortices in quantum gases. Here we excite an atomic transition with a vortex laser beam and demonstrate the transfer of optical orbital angular momentum to the valence electron of a single trapped ion. We observe strongly modified selection rules showing that an atom can absorb two quanta of angular momentum from a single photon: one from the spin and another from the spatial structure of the beam. Furthermore, we show that parasitic ac-Stark shifts from off-resonant transitions are suppressed in the dark centre of vortex beams. These results show how light's spatial structure can determine the characteristics of light-matter interaction and pave the way for its application and observation in other systems.
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.
Introduction Although the orbital angular momentum (OAM) of light is often quantified in terms of ℓℏ per photon, one should recognise that this result can be derived directly from Maxwell's equations and is most certainly not an exclusively quantum property. Following the recognition of optical OAM in 1992 [1], the immediate thrust of experimental work was to observe OAM transfer to microscopic objects. These exciting experiments by Rubinsztein- Dunlop [2, 3] and others established that the predicted angular momentum was truly mechanical, but did not provide insight on OAM at the level of single photons. Laguerre- Gaussian modes were identified as being a natural basis set for describing beams with OAM, where their phase terms describe the helical phasefronts corresponding to an OAM of ℓℏ per photon. The polarisation of light has played an important historical role in the experimental investigation of quantum entanglement, quantum gate operations and quantum cryptography. A potential advantage of OAM is that it resides in a higher-dimensional state space which, as follows from the theory, is infinite-dimensional. One of the experimental challenges is to access a large number of these dimensions. In quantum communication, the most obvious advantage of high n -dimensional systems is the increased bandwidth [4], but qunits also lead to stronger security [5, 6]. An increase in the number of entangled quantum modes has also been shown to improve measures of nonlocality [7], to allow quantum computation with better fault tolerance [8] and to simplify quantum logic structures [9].