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arXiv:2410.08940 · Physical Review Letters

Engineering Dipole-Dipole Couplings for Enhanced Cooperative Light-Matter Interactions

Adam Burgess, Madeline C. Waller, Erik M. Gauger, Robert G. Bennett

Published Mar 21, 2025• 8 citations
arXivHTMLPDF

Abstract

Cooperative optical effects are enabled and controlled by interactions between molecular dipoles, meaning that their mutual orientation is of paramount importance to, for example, superabsorbing light-harvesting antennas. Here we show how to move beyond the possibilities of simple geometric tailoring, demonstrating how a metallic sphere placed within a ring of parallel dipoles engineers an effective Hamiltonian that generates "guide-sliding" states within the ring system. This allows steady-state superabsorption in noisy room temperature environments, outperforming previous designs while being significantly simpler to implement. As exemplified by this showcase, our approach represents a powerful design paradigm for tailoring cooperative light-matter effects in molecular structures that extends beyond superabsorbing systems to a huge array of quantum energy transport systems.

DOI
10.1103/physrevlett.134.113602

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Cooperative optical effects are enabled and controlled by interactions between molecular dipoles, meaning that their mutual orientation is of paramount importance to, for example, superabsorbing light-harvesting antennas. Here we show how to move beyond the possibilities of simple geometric tailoring, demonstrating how a metallic sphere placed within a ring of parallel dipoles engineers an effective Hamiltonian that generates "guide-sliding" states within the ring system. This allows steady-state superabsorption in noisy room temperature environments, outperforming previous designs while being significantly simpler to implement. As exemplified by this showcase, our approach represents a powerful design paradigm for tailoring cooperative light-matter effects in molecular structures that extends beyond superabsorbing systems to a huge array of quantum energy transport systems.
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Networks of interacting molecular optical dipoles play an important role in photosynthetic light harvesting, and also hold significant promise for future artificial technologies. This manuscript gives a brief overview of questions addressed by (our) recent theoretical work with a focus on taking inspiration from biological structures and processes to come up with designs for utilising bio-inspired collective quantum optical effects. These could, for instance, enable quantum-enhanced light harvesting, the charging of Dicke quantum batteries through superabsorption of light, and achieving efficient long-range energy transport. Particular attention is given to the role of inter-emitter quantum coherence as an enabler of these effects.
Abstract Efficient devices for light harvesting and photon sensing are fundamental building blocks of basic energy science and many essential technologies. Recent efforts have turned to biomimicry to design the next generation of light-capturing devices, partially fueled by an appreciation of the fantastic efficiency of the initial stages of natural photosynthetic systems at capturing photons. In such systems extended excitonic states are thought to play a fundamental functional role, inducing cooperative coherent effects, such as superabsorption of light and supertransfer of photoexcitations. Inspired by this observation, we design an artificial light-harvesting and photodetection device that maximally harnesses cooperative effects to enhance efficiency. The design relies on separating absorption and transfer processes (energetically and spatially) in order to overcome the fundamental obstacle to exploiting cooperative effects to enhance light capture: the enhanced emission processes that accompany superabsorption. This engineered separation of processes greatly improves the efficiency and the scalability of the system.
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We investigate how laser-driven, cooperative dipole-dipole interactions in weakly trapped atomic arrays give rise to self-organized configurations. Starting from an analytically tractable two-emitter system, we identify the possible steady-state spatial arrangements accessible to the atoms. We then extend this analysis to larger ensembles in both linear and ring geometries. In linear chains, we demonstrate the emergence of topologically nontrivial dimerized configurations across a range of initial interatomic spacings. In ring geometries, we find that the system undergoes self-organized contraction and expansion, enabling access to length scales below those set by the trapping lattice. Our results demonstrate that collective light-matter interactions in free space can spontaneously generate modified ordered geometries, even when the emitters are initially separated by distances larger than their transition wavelength.
Almost 60 years ago Dicke introduced the term superradiance to describe a signature quantum effect: N atoms can collectively emit light at a rate proportional to N(2). Structures that superradiate must also have enhanced absorption, but the former always dominates in natural systems. Here we show that this restriction can be overcome by combining several well-established quantum control techniques. Our analytical and numerical calculations show that superabsorption can then be achieved and sustained in certain simple nanostructures, by trapping the system in a highly excited state through transition rate engineering. This opens the prospect of a new class of quantum nanotechnology with potential applications including photon detection and light-based power transmission. An array of quantum dots or a molecular ring structure could provide a suitable platform for an experimental demonstration.