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arXiv:1504.05849 · The Journal of Physical Chemistry C

Quantum-Enhanced Capture of Photons Using Optical Ratchet States

K. D. B. Higgins, Brendon W. Lovett, Erik M. Gauger

Published Aug 23, 2017• 33 citations
arXivHTMLPDF

Abstract

Abstract Natural and artificial light harvesting systems often operate in a regime where the flux of photons is relatively low. Besides absorbing as many photons as possible, it is paramount to prevent excitons from annihilation via photon re-emission until they have undergone an irreversible energy conversion process. Taking inspiration from photosynthetic antenna structures, we here consider ringlike systems and introduce a class of states we call ratchets: excited states capable of absorbing but not emitting light. This allows our antennae to absorb further photons while retaining the excitations from those that have already been captured. Simulations for a ring of four sites reveal a peak power enhancement by up to a factor of 35 owing to a combination of ratcheting and the prevention of emission through dark-state population. In the slow extraction limit, the achievable power enhancement due to ratcheting alone exceeds 20%.

DOI
10.1021/acs.jpcc.7b07138

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Abstract Natural and artificial light harvesting systems often operate in a regime where the flux of photons is relatively low. Besides absorbing as many photons as possible, it is paramount to prevent excitons from annihilation via photon re-emission until they have undergone an irreversible energy conversion process. Taking inspiration from photosynthetic antenna structures, we here consider ringlike systems and introduce a class of states we call ratchets: excited states capable of absorbing but not emitting light. This allows our antennae to absorb further photons while retaining the excitations from those that have already been captured. Simulations for a ring of four sites reveal a peak power enhancement by up to a factor of 35 owing to a combination of ratcheting and the prevention of emission through dark-state population. In the slow extraction limit, the achievable power enhancement due to ratcheting alone exceeds 20%.
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.
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.
Subwavelength arrays of quantum emitters feature unique and largely design-able nonlinear optical properties. As a generic example we study a sub-wavelength sized ring of identical dipoles with an extra identical absorbing emitter at the center. For a 9-ring one finds the most efficient antenna configuration to direct single incoming photons to the center without re-emission. Interestingly, for very tiny structures sizes below a tenth of a wavelength, a full quantum description predicts an even larger absorption enhancement than a mean field model using a classical dipole approximation. We identify the origin of the enhancement in the appearance of a collective dark state with dominant center occupation. By special design of the center absorber one thus can harness the same efficiency enhancement also at different wavelengths and for other geometric structures. On the one hand this idea could be the basis of a new generation of highly efficient and selective nano antennas, while on the other hand, it could be an important piece towards understanding the surprising efficiency of natural light harvesting molecules. Adding gain via active dipoles in such nano ring systems allows to design minimalist laser like classical light sources. In the nonlinear operating regime at stronger pump fields these systems transform to non-classical light sources with tailor-able spatio-temporal emission upon coherent illumination.
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.
We analytically derive transfer probabilities and efficiencies for an artificial light-harvesting photosynthetic system, which consists of a ring coupled to a central acceptor. For an incident photon pair, we find near-perfect single excitation transfer efficiency with negligible double excitation transfer in the weak-coupling regime. In the strong-coupling regime, single excitation transfer efficiency was greater than 9090%90, while the double excitation efficiency was approximately 5050%50. We have found that the three main factors which determine high transfer efficiencies are large acceptor probabilities, long acceptor decay times, and strong photon-ring coupling. A possible implementation of the theoretical framework to bio-inspired solar energy devices is also discussed.
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.