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Optics Express

Role of higher-order electric field corrections in the quadrupole interaction of twisted light with matter

Abdullah F. Alharbi, A. Lyras

Published Jan 24, 2025• 1 citation
Publisher

Abstract

Recent studies on twisted-light-matter interactions have highlighted the importance of the longitudinal electric field component, which had previously been overlooked. Together with the transverse component, it corresponds to the lowest-order terms in a perturbative expansion over the paraxial parameter. In this work, we investigate the influence of higher-order correction terms in the perturbative expansion on the quadrupole excitation of a trapped atom. This article begins by resolving discrepancies in the literature regarding the calculation of transverse fields at second and higher even orders using the appropriate gauge. A key finding of our study reveals that including a higher-order term in the perturbative expansion is not always sufficient to enhance accuracy in describing the interaction at a given level; instead, two successive orders may need to be considered together. This is particularly evident in quadrupole transitions involving no change in the magnetic quantum number (Δ m = 0), where longitudinal corrections play a more significant role than their transverse counterparts, despite the latter being lower order. This behavior is attributed to the sensitivity of quadrupole interactions to field gradients and the connection between odd- and even-order fields via transverse gradients.

DOI
10.1364/oe.544711

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We investigate a controlled beyond-electric-dipole extension of the quantum Rabi model in which the leading electric-dipole interaction is supplemented by an electric-quadrupole contribution. A central issue is the parity selection rule: for two exact atomic parity eigenstates of opposite parity, an electric-quadrupole transition matrix element vanishes. We therefore do not interpret the additional longitudinal coupling as an E2 transition between an opposite-parity pair. Instead, we consider an inversion-asymmetric (or parity-mixed) two-level system for which the two retained states may have different diagonal quadrupole moments. Projection of the multipolar interaction then produces a state-dependent term proportional to σz(a + a†), while the ordinary transition dipole produces the transverse term proportional to σx(a + a†). A state-independent quadrupolar contribution is removed by a bosonic displacement, leaving the effective Hamiltonian H =ωa†a+∆σz/2+gσx(a+a†)+gQσz(a+a†). This construction connects the beyond-dipole physical problem to the well-studied class of Rabi models with simultaneous transverse and longitudinal coupling, including asymmetric or biased Rabi models. We make this relation explicit by a constant spin rotation, which maps the model to a biased Rabi Hamiltonian with effective coupling κ = √g2 +g2Q and bias δ = ∆gQ/(2κ). We then derive the corresponding second-order Bargmann differential equation and solve its exceptional polynomial sector using a Zhang-type functional Bethe ansatz. The resulting Bethe equations, root-sum constraint, exceptional energy branches, and the first nontrivial parameter condition are obtained explicitly. In the limit gQ → 0, the construction continuously recovers the ordinary Rabi exceptional sector. From an experimental perspective, the connection with demonstrated quadrupolar light--matter coupling in engineered quantum systems suggests that the present framework may have relevance for spectroscopic studies of beyond-electric-dipole interactions, although a direct experimental realization of the specific effective model considered here remains to be established [20].

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Recent studies on twisted-light-matter interactions have highlighted the importance of the longitudinal electric field component, which had previously been overlooked. Together with the transverse component, it corresponds to the lowest-order terms in a perturbative expansion over the paraxial parameter. In this work, we investigate the influence of higher-order correction terms in the perturbative expansion on the quadrupole excitation of a trapped atom. This article begins by resolving discrepancies in the literature regarding the calculation of transverse fields at second and higher even orders using the appropriate gauge. A key finding of our study reveals that including a higher-order term in the perturbative expansion is not always sufficient to enhance accuracy in describing the interaction at a given level; instead, two successive orders may need to be considered together. This is particularly evident in quadrupole transitions involving no change in the magnetic quantum number (Δ m = 0), where longitudinal corrections play a more significant role than their transverse counterparts, despite the latter being lower order. This behavior is attributed to the sensitivity of quadrupole interactions to field gradients and the connection between odd- and even-order fields via transverse gradients.
The propagation of light beams is well described using the paraxial approximation, where field components along the propagation direction are usually neglected. For strongly inhomogeneous or shaped light fields, however, this approximation may fail, leading to intriguing variations of the light-matter interaction. This is the case of twisted light having opposite orbital and spin angular momenta. We compare experimental data for the excitation of a quadrupole transition in a single trapped ^{40}Ca^{+} ion from Schmiegelow et al. [Nat. Commun. 7, 12998 (2016)NCAOBW2041-172310.1038/ncomms12998] with a complete model where longitudinal components of the electric field are taken into account. Our model matches the experimental data and excludes by 11 standard deviations the approximation of a complete transverse field. This demonstrates the relevance of all field components for the interaction of twisted light with matter.
Electric quadrupole absorption is driven by optical field gradients, not by field amplitudes alone. This distinction is crucial for structured light, where a paraxially small longitudinal field can generate a leading-order longitudinal gradient. For fully vectorial Laguerre-Gaussian modes, Maxwell transversality locks this longitudinal gradient to the transverse structured gradient of the leading paraxial field. This locking is therefore a general electromagnetic constraint, not a focusing-dependent correction that can be removed independently. Decomposing the symmetric-traceless optical field-gradient tensor into spherical components reveals a strongly channel-selective response: the Δm=0Δm=0Δm=0 transition requires the longitudinal gradient at the retained order, the Δm=±1Δm=\pm1Δm=±1 channels receive scalar and vectorial nonparaxial corrections on top of the carrier-scale longitudinal derivative of the transverse field, and the Δm=±2Δm=\pm2Δm=±2 channels remain transverse at the same order. These results show that longitudinal optical structure can enter structured-light quadrupole transitions as an indispensable leading-gradient contribution, even when the longitudinal field amplitude itself is paraxially small.
It is well established that the longitudinal component of paraxial optical vortices has a key role in specific atomic quadrupole transitions near the beam axis when the spin and orbital angular momenta are antiparallel. By deriving analytical expressions for the position-dependent selection rules, this work shows that the significant role of the longitudinal fields is not limited to this case, but rather is a more general feature for any paraxial light including, for example, optical vortices with parallel spin and orbital angular momenta as well as Guassian beams. Numerically, the transition strengths induced by the weaker longitudinal component can be twice as high as those by the stronger transverse component. We also show that there are transitions that can be induced exclusively by the longitudinal component for light carrying two quanta of orbital angular momentum.
Using a method based on the Magnus expansion, the survival of Rydberg atoms in intense laser fields is studied. Usually, for atoms in intense laser fields, effects beyond the electric dipole approximation need to be considered. In the past few years, researchers have primarily paid attention to the nondipole effects induced by the electric quadrupole term of the optical field. The quadrupole term plays a more important role than the electric dipole term in the calculation of the survival probability of Rydberg atoms in intense laser fields even though the magnitude of the former is smaller than that of the latter in terms of the multipole expansion of the optical vector potential. Meanwhile, the effects of higher-order corrections beyond the quadrupole term remain ambiguous. In this paper, we confirm that corrections containing higher-order terms, except for the quadrupole term, can be neglected in the calculation of the transitions of Rydberg atoms in external fields. We then use the second-order time evolution operator containing the quadrupole term to study the scaling law of the transition probability of Rydberg He in laser fields with different parameters.
We investigate a controlled beyond-electric-dipole extension of the quantum Rabi model in which the leading electric-dipole interaction is supplemented by an electric-quadrupole contribution. A central issue is the parity selection rule: for two exact atomic parity eigenstates of opposite parity, an electric-quadrupole transition matrix element vanishes. We therefore do not interpret the additional longitudinal coupling as an E2 transition between an opposite-parity pair. Instead, we consider an inversion-asymmetric (or parity-mixed) two-level system for which the two retained states may have different diagonal quadrupole moments. Projection of the multipolar interaction then produces a state-dependent term proportional to σz(a + a†), while the ordinary transition dipole produces the transverse term proportional to σx(a + a†). A state-independent quadrupolar contribution is removed by a bosonic displacement, leaving the effective Hamiltonian H =ωa†a+∆σz/2+gσx(a+a†)+gQσz(a+a†). This construction connects the beyond-dipole physical problem to the well-studied class of Rabi models with simultaneous transverse and longitudinal coupling, including asymmetric or biased Rabi models. We make this relation explicit by a constant spin rotation, which maps the model to a biased Rabi Hamiltonian with effective coupling κ = √g2 +g2Q and bias δ = ∆gQ/(2κ). We then derive the corresponding second-order Bargmann differential equation and solve its exceptional polynomial sector using a Zhang-type functional Bethe ansatz. The resulting Bethe equations, root-sum constraint, exceptional energy branches, and the first nontrivial parameter condition are obtained explicitly. In the limit gQ → 0, the construction continuously recovers the ordinary Rabi exceptional sector. From an experimental perspective, the connection with demonstrated quadrupolar light--matter coupling in engineered quantum systems suggests that the present framework may have relevance for spectroscopic studies of beyond-electric-dipole interactions, although a direct experimental realization of the specific effective model considered here remains to be established [20].
We investigate a controlled beyond-electric-dipole extension of the quantum Rabi model in which the leading electric-dipole interaction is supplemented by an electric-quadrupole contribution. A central issue is the parity selection rule: for two exact atomic parity eigenstates of opposite parity, an electric-quadrupole transition matrix element vanishes. We therefore do not interpret the additional longitudinal coupling as an E2 transition between an opposite-parity pair. Instead, we consider an inversion-asymmetric (or parity-mixed) two-level system for which the two retained states may have different diagonal quadrupole moments. Projection of the multipolar interaction then produces a state-dependent term proportional to σz(a + a†), while the ordinary transition dipole produces the transverse term proportional to σx(a + a†). A state-independent quadrupolar contribution is removed by a bosonic displacement, leaving the effective Hamiltonian H =ωa†a+∆σz/2+gσx(a+a†)+gQσz(a+a†). This construction connects the beyond-dipole physical problem to the well-studied class of Rabi models with simultaneous transverse and longitudinal coupling, including asymmetric or biased Rabi models. We make this relation explicit by a constant spin rotation, which maps the model to a biased Rabi Hamiltonian with effective coupling κ = √g2 +g2Q and bias δ = ∆gQ/(2κ). We then derive the corresponding second-order Bargmann differential equation and solve its exceptional polynomial sector using a Zhang-type functional Bethe ansatz. The resulting Bethe equations, root-sum constraint, exceptional energy branches, and the first nontrivial parameter condition are obtained explicitly. In the limit gQ → 0, the construction continuously recovers the ordinary Rabi exceptional sector. From an experimental perspective, the connection with demonstrated quadrupolar light--matter coupling in engineered quantum systems suggests that the present framework may have relevance for spectroscopic studies of beyond-electric-dipole interactions, although a direct experimental realization of the specific effective model considered here remains to be established [20].