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arXiv:1901.10598 · Physical Review A

Subradiance-enhanced excitation transfer between dipole-coupled nanorings of quantum emitters

Maria Moreno-Cardoner, David Plankensteiner, Laurin Ostermann, Darrick E. Chang, Helmut Ritsch

Published Aug 7, 2019• 63 citations
arXivHTMLPDF

Abstract

A ring of dipole-coupled quantum emitters positioned at subwavelength distances possesses only a few radiant but many subradiant collective excitations with lifetimes growing exponentially with the atom number. These exhibit a three-dimensionally confined spatial radiation field pattern and form nanoscale high-$Q$ optical resonators. Tailoring size, orientation, and distance between two rings allows for increasing the ratio of coherent ring-to-ring energy transfer versus free-space emission by orders of magnitude. In particular, the more dark and delocalized over several sites are excitons, the higher is their fidelity for transport to a second ring.

DOI
10.1103/physreva.100.023806

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A ring of dipole-coupled quantum emitters positioned at subwavelength distances possesses only a few radiant but many subradiant collective excitations with lifetimes growing exponentially with the atom number. These exhibit a three-dimensionally confined spatial radiation field pattern and form nanoscale high-QQQ optical resonators. Tailoring size, orientation, and distance between two rings allows for increasing the ratio of coherent ring-to-ring energy transfer versus free-space emission by orders of magnitude. In particular, the more dark and delocalized over several sites are excitons, the higher is their fidelity for transport to a second ring.
An array of N closely spaced dipole coupled quantum emitters exhibits super- and subradiance with characteristic tailorable spatial radiation patterns. Optimizing the emitter geometry and distance with respect to the spatial profile of a near resonant optical cavity mode allows us to increase the ratio between light scattering into the cavity mode and free space emission by several orders of magnitude. This leads to distinct scaling of the collective coherent emitter-field coupling vs the free space decay as a function of the emitter number. In particular, for subradiant states, the effective cooperativity increases much faster than the typical linear ∝N scaling for independent emitters. This extraordinary collective enhancement is manifested both in the amplitude and the phase profile of narrow collective antiresonances appearing at the cavity output port in transmission spectroscopy.
Abstract Ring geometries of subwavelength-spaced quantum emitters exhibit outstanding radiation properties and are useful for antennas, excitation transport, and storage. Taking inspiration from the oligomeric geometry, in particular by considering only the position and dipole orientations of the bacteriochlorophylls in biological light-harvesting 2 complexes of (approximately 6 nm in diameter), we propose and predict highly efficient interlayer excitation transfer, achieving a maximum of 100% transfer for certain choices of dipole orientations in a three-dimensional (3D) concentric stacked ring geometry with C 9 symmetry and a diameter of 400 nm, formed by two-level atoms. Utilizing the quantum optical open system Lindblad master equation approach for estimating the collective dipole dynamics, we demonstrate that, depending on the system parameters, our bio-inspired 3D ring of quantum emitters enables efficient asymmetric excitation transfer between two ring layers, in particular from sparse to dense quantum emitter arrangements. The presented nanoscale geometry is expected to be realizable with diverse physical platforms operating at cryogenic temperatures, where the interacting dipole description remains applicable and, importantly, dominant over environmental decoherence.
Decoherence is mostly detrimental in quantum information and quantum optics applications. However, the interplay between environment-induced incoherent dynamics and unitary evolution can give rise to novel quantum many-body phenomena that can be harnessed as a useful resource. As is well known, in dense subwavelength atomic arrays only a single collective eigenmode in the single-excitation manifold couples strongly to free-space radiation, exhibiting superradiant spontaneous emission. Most of the remaining eigenstates form a manifold of weakly radiative modes, giving rise to long-lived subradiant excitations. Here we demonstrate that populating these subradiant modes via additional decoherence mechanisms, such as dephasing or coupling to phonons, can significantly enhance single-photon absorption in a nanoring of quantum emitters. Such nanoring geometry is particularly appealing due to its unique optical properties and its resemblance to natural light-harvesting complexes, which serve as efficient antennas in photosynthesis. Our findings may shed light on fundamental aspects of energy absorption in nature; despite the much greater complexity of biological systems, they may nonetheless operate according to similar underlying optical principles.
Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom. While vibrations are typically considered detrimental to coherent dynamics, we show that molecular dimers or rings can be operated as platforms for the preparation of long-lived dark superposition states aided by vibrational relaxation. In closed ring configurations, we extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence.
Nanoscopic arrays of quantum emitters can feature highly sub-radiant collective excitations with a lifetime exponentially growing with emitter number. Adding an absorptive impurity as an energy dump in the center of a ring shaped polygon allows to exploit this feature to create highly efficient single photon antennas. Here among regular polygons with an identical center absorbing emitter, a nonagon exhibits a distinct optimum of the absorption efficiency. This special enhancement originates from the unique emergence of a subradiant eigenstate with dominant center occupation. Only for nine emitters the sum of coupling strengths of each emitter to all others matches the center to the ring coupling. Analogous to a parabolic mirror the antenna ring then concentrates incoming radiation at its center without being significantly excited itself. Similar large efficiency enhancements, which even prevail for broadband excitation, can also be engineered for other antenna sizes by tailoring the frequency and magnitude of the central absorber. Interestingly, for very small structures a quantum treatment predicts an even stronger enhancement for the single photon absorption enhancement than a classical dipole model. As natural light harvesting structures are often based on ring shaped structures, the underlying principle might be exploited there as well.
Efficient transport and harvesting of excitation energy under low light conditions is an important process in nature and quantum technologies alike. Here we formulate a quantum optics perspective to excitation energy transport in configurations of two-level quantum emitters with a particular emphasis on efficiency and robustness against disorder. We study a periodic geometry of emitter rings with subwavelength spacing, where collective electronic states emerge due to near-field dipole–dipole interactions. The system gives rise to collective subradiant states that are particularly suited to excitation transport and are protected from energy disorder and radiative decoherence. Comparing ring geometries with other configurations shows that the former are more efficient in absorbing, transporting, and trapping incident light. Because our findings are agnostic as to the specific choice of quantum emitters, they indicate general design principles for quantum technologies with superior photon transport properties and may elucidate potential mechanisms resulting in the highly efficient energy transport efficiencies in natural light-harvesting systems.