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arXiv:2307.01375

Quantum theory of single-photon nonlinearities generated by ensembles of emitters

Kurt A. Jacobs, Stefan Krastanov, Mikkel Heuck, Dirk Englund

Published Jul 3, 2023• 0 citations
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Abstract

The achievement of sufficiently fast interactions between two optical fields at the few-photon level would provide a key enabler for a broad range of quantum technologies. One critical hurdle in this endeavor is the lack of a comprehensive quantum theory of the generation of nonlinearities by ensembles of emitters. Distinct approaches applicable to different regimes have yielded important insights: i) a semiclassical approach reveals that, for many-photon coherent fields, the contributions of independent emitters add independently allowing ensembles to produce strong optical nonlinearities via EIT; ii) a quantum analysis has shown that in the few-photon regime collective coupling effects prevent ensembles from inducing these strong nonlinearities. Rather surprisingly, experimental results with around twenty photons are in line with the semi-classical predictions. Theoretical analysis has been fragmented due to the difficulty of treating nonlinear many-body quantum systems. Here we are able to solve this problem by constructing a powerful theory of the generation of optical nonlinearities by single emitters and ensembles. The key to this construction is the application of perturbation theory to perturbations generated by subsystems. This theory reveals critical properties of ensembles that have long been obscure. The most remarkable of these is the discovery that quantum effects prevent ensembles generating single-photon nonlinearities only within the rotating-wave regime; outside this regime single-photon nonlinearities scale as the number of emitters. The theory we present here also provides an efficient way to calculate nonlinearities for arbitrary multi-level driving schemes, and we expect that it will prove a powerful foundation for further advances in this area.

DOI
10.48550/arxiv.2307.01375

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The achievement of sufficiently fast interactions between two optical fields at the few-photon level would provide a key enabler for a broad range of quantum technologies. One critical hurdle in this endeavor is the lack of a comprehensive quantum theory of the generation of nonlinearities by ensembles of emitters. Distinct approaches applicable to different regimes have yielded important insights: i) a semiclassical approach reveals that, for many-photon coherent fields, the contributions of independent emitters add independently allowing ensembles to produce strong optical nonlinearities via EIT; ii) a quantum analysis has shown that in the few-photon regime collective coupling effects prevent ensembles from inducing these strong nonlinearities. Rather surprisingly, experimental results with around twenty photons are in line with the semi-classical predictions. Theoretical analysis has been fragmented due to the difficulty of treating nonlinear many-body quantum systems. Here we are able to solve this problem by constructing a powerful theory of the generation of optical nonlinearities by single emitters and ensembles. The key to this construction is the application of perturbation theory to perturbations generated by subsystems. This theory reveals critical properties of ensembles that have long been obscure. The most remarkable of these is the discovery that quantum effects prevent ensembles generating single-photon nonlinearities only within the rotating-wave regime; outside this regime single-photon nonlinearities scale as the number of emitters. The theory we present here also provides an efficient way to calculate nonlinearities for arbitrary multi-level driving schemes, and we expect that it will prove a powerful foundation for further advances in this area.
Most phenomena around us can be explained by classical optics since photons interact weakly with atoms. When the interaction is strong enough where one photon affects the properties of other photons, we go to the regime of quantum photon-photon nonlinear optics. The work in this thesis explores this regime of physics. This paves the path to exploring strongly interacting many-body physics with photons which is still a largely unexplored domain. The ability to control strongly interacting photons is also of central importance in quantum science and engineering. We use the approach of Electromagnetically Induced Transparency (EIT) in atomic ensembles to create strong interactions and demonstrate coherent control between single photons. Using EIT, we coherently map single photons onto the atoms which travel as coupled excitations of light and matter called dark-state polaritons. When the medium is optically dense, the polariton propagates as a massive particle with a velocity that is much smaller than the speed of light. These polaritons interact with each other via their atomic component. In this thesis, we show robust symmetry-protected collisions between photons that imprint a large phase of π/2 with little loss and extend the nature of photon-photon interactions to the repulsive regime, which are essential for quantum communication and metrology. We use the technique of photon blockade to make a fast optical detector of Rydberg states, directly demonstrating the use of quantum nonlinear optics for quantum computation. We also study the extensions of the attractive and repulsive photons for three particles shedding light into the formation of bound states and crystals of photons and paving the way to studying many-body physics of photons.
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How single-photon nonlinearity is quenched with multiple quantum emitters: Quantum Zeno effect in collective interactions with ΛΛΛ-level atoms
Single-photon nonlinearity, namely the change in the response of the system as the result of the interaction with a single photon, is generally considered an inherent property of a single quantum emitter. Understanding the dependence of the nonlinearity on the number of emitters is important both fundamentally and practically, as strong light-matter coupling is more readily achieved through collective interactions than with a single emitter. Here, we theoretically consider a system that explores the transition from a single to multiple emitters with a ΛΛΛ-level scheme. We show that the single-photon nonlinearity indeed vanishes with the number of emitters. Interestingly, the mechanism behind this behavior is the quantum Zeno effect, manifested in the slowdown of the photon-controlled dynamics.
Coupling light to ensembles of strongly interacting particles has emerged as a promising route toward achieving few photon nonlinearities. One specific way to implement this kind of nonlinearity is to interface light with highly excited atomic Rydberg states by means of electromagnetically induced transparency, an approach which allows freely propagating photons to acquire synthetic interactions of hitherto unprecedented strength. Here, we present an overview of this rapidly developing field, from classical effects to quantum manifestations of the nonlocal nonlinearities emerging in such systems. With an emphasis on underlying theoretical concepts, we describe the many experimental breakthroughs so far demonstrated and discuss potential applications looming on the horizon.
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Quantum nonlinear optics seeks to harness strong photon-photon interactions for scalable quantum technologies, although dissipative losses still pose a major barrier to near-unity conversion efficiency. Here, we bridge non-Hermitian physics with the quantum nonlinear domain by exploiting perfect absorption to identify and optimize few-photon nonlinear processes. We theoretically investigate two circuit QED systems, operating in the light-matter ultrastrong coupling regime. The first (i) enables simultaneous two-atom excitations by single photons, while the second (ii) realizes the strong coupling between a single-photon and a two-photon Fock states. We demonstrate that, since the strong optical nonlinearities cause quantum spectral features to emerge already at the level of linear response theory, the perfect absorption condition in ∣S11∣|S_{11}|∣S11​∣ enables near-deterministic single-photon down-conversion into (i) a qubit-qubit-correlated pair and (ii) a two-photon pair. We show that the conversion efficiency can be systematically optimized through experimentally accessible parameters, both linked to the emergence of Hermitian subspaces within the effective non-Hermitian Hamiltonians. These findings position non-Hermitian engineering as a broadly applicable route to optimizing quantum devices at the single-photon level, even beyond circuit-QED platforms.