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arXiv:1701.05038 · Physical Review A

Deterministic quantum nonlinear optics with single atoms and virtual photons

Anton Frisk Kockum, Adam Miranowicz, Vincenzo Macrí, Salvatore Savasta, Franco Nori

Published Jun 29, 2017• 156 citations
arXivHTMLPDF

Abstract

We show how analogs of a large number of well-known nonlinear-optics phenomena can be realized with one or more two-level atoms coupled to one or more resonator modes. Through higher-order processes, where virtual photons are created and annihilated, an effective deterministic coupling between two states of such a system can be created. In this way, analogs of three-wave mixing, four-wave mixing, higher-harmonic and -subharmonic generation (i.e., up- and down-conversion), multiphoton absorption, parametric amplification, Raman and hyper-Raman scattering, the Kerr effect, and other nonlinear processes can be realized. In contrast to most conventional implementations of nonlinear optics, these analogs can reach unit efficiency, only use a minimal number of photons (they do not require any strong external drive), and do not require more than two atomic levels. The strength of the effective coupling in our proposed setups becomes weaker the more intermediate transition steps are needed. However, given the recent experimental progress in ultrastrong light-matter coupling and improvement of coherence times for engineered quantum systems, especially in the field of circuit quantum electrodynamics, we estimate that many of these nonlinear-optics analogs can be realized with currently available technology.

DOI
10.1103/physreva.95.063849

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We show how analogs of a large number of well-known nonlinear-optics phenomena can be realized with one or more two-level atoms coupled to one or more resonator modes. Through higher-order processes, where virtual photons are created and annihilated, an effective deterministic coupling between two states of such a system can be created. In this way, analogs of three-wave mixing, four-wave mixing, higher-harmonic and -subharmonic generation (i.e., up- and down-conversion), multiphoton absorption, parametric amplification, Raman and hyper-Raman scattering, the Kerr effect, and other nonlinear processes can be realized. In contrast to most conventional implementations of nonlinear optics, these analogs can reach unit efficiency, only use a minimal number of photons (they do not require any strong external drive), and do not require more than two atomic levels. The strength of the effective coupling in our proposed setups becomes weaker the more intermediate transition steps are needed. However, given the recent experimental progress in ultrastrong light-matter coupling and improvement of coherence times for engineered quantum systems, especially in the field of circuit quantum electrodynamics, we estimate that many of these nonlinear-optics analogs can be realized with currently available technology.
Spontaneous parametric down-conversion is a well-known process in quantum nonlinear optics in which a photon incident on a nonlinear crystal spontaneously splits into two photons. Here we propose an analogous physical process where one excited atom directly transfers its excitation to a pair of spatially separated atoms with probability approaching 1. The interaction is mediated by the exchange of virtual rather than real photons. This nonlinear atomic process is coherent and reversible, so the pair of excited atoms can transfer the excitation back to the first one: the atomic analog of sum-frequency generation of light. The parameters used to investigate this process correspond to experimentally demonstrated values in ultrastrong circuit quantum electrodynamics. This approach can be extended to realize other nonlinear interatomic processes, such as four-atom mixing, and is an attractive architecture for the realization of quantum devices on a chip. We show that four-qubit mixing can efficiently implement quantum repetition codes and, thus, can be used for error-correction codes.
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.
Controlling light photon-by-photon is central to quantum optics. At a fundamental level, photon interactions are mediated by their coupling to atoms, and ultimate control requires deterministic light-matter interfacing of single photons to single atoms. Extending this paradigm to radiatively couple multiple individual atoms in a deterministic and scalable manner opens the arena of many-body quantum optics. Here, we realize such a setting by coherently coupling solid-state artificial atoms to a nanophotonic waveguide and demonstrate higher-order photon correlations that are controlled by the number of quantum emitters. We study the scaling of nonlinear photonic transport induced by emitter-photon scattering and demonstrate that adding a quantum emitter generates higher-order photon correlations. Specifically, we experimentally observe genuine three-photon correlations from a pair of collectively coupled emitters, while contributions from lower photon numbers are suppressed. In addition, we scale to three resonant quantum emitters coupled to the waveguide. These advancements demonstrate the onset of many-body quantum optics in waveguide quantum electrodynamics, enabling new photonic quantum simulators, the creation of many-body entangled states, and the exploration of novel quantum phase transitions.
Deterministic single-photon sources are indispensable core devices for quantum information technology, yet high-performance implementation remains a long-standing bottleneck for linear optical quantum computing. We propose a feasible scheme for deterministic single-photon emission based on a △\triangle△-type three-level atom coupled to a single-mode cavity, driven by two classical external fields, which is adaptable to both strong and ultrastrong cavity-atom coupling regimes. Under continuous-wave driving, the system achieves excellent single-photon characteristics: the normalized equal-time second-order correlation function reaches g(2)(0)∼10−6g^{(2)}(0)\sim10^{-6}g(2)(0)∼10−6, with a photon indistinguishability of 98.73%98.73\%98.73% and a state purity of 99.95%99.95\%99.95% in the strong coupling regime, while the ultrastrong coupling regime further suppresses G(2)(0)∼10−8G^{(2)}(0)\sim10^{-8}G(2)(0)∼10−8, yielding an indistinguishability of 99.10%99.10\%99.10% and a purity of 99.99%99.99\%99.99%. For pulsed driving in the ultrastrong coupling regime, the source realizes superior performance, with an emission efficiency, indistinguishability, and purity of 99.96%99.96\%99.96%, 98.98%98.98\%98.98%, and 99.99%99.99\%99.99% under resonant conditions, and 100%100\%100%, 95.91%95.91\%95.91%, and 99.93%99.93\%99.93% under detuned conditions, respectively. The near-ideal optical performance of the proposed scheme provides a viable route for constructing high-quality deterministic single-photon sources, which offers a promising solution to the limitations of conventional single-photon devices and facilitates the further development of quantum information science and fundamental quantum optical research.
This thesis presents a study of photon generation and conversion processes in nonlinear optics. Our results extend beyond the first order perturbative regime, in which only pairs of photons are generated in spontaneous parametric down-conversion or four wave mixing. They also allow us to identify the limiting factors for achieving unit efficiency frequency conversion, and to correctly account for the propagation of bright nonclassical photon states generated in the nonlinear material. This is done using the Magnus expansion, which allows us to incorporate corrections due to time-ordering effects in the time evolution of the state, while also respecting the quantum statistics associated with squeezed states (in photon generation) and single photons or coherent states (in photon conversion). We show more generally that this expansion should be the preferred strategy when dealing with any type of time-dependent Hamiltonian that is a quadratic form in the creation and annihilation operators of the fields involved. Using the Magnus expansion, simple figures of merit to estimate the relevance of these time-ordering corrections are obtained. These quantities depend on the group velocities of the modes involved in the nonlinear process and provide a very simple physical picture of the interactions between the photons at different times. These time-ordering effects are shown to be important only when the photons and pump beam overlap within the nonlinear material for a significant amount of time. We also discuss the possibility of preparing Fock states with many photons using parametric down-conversion sources and realistic photon-number-resolving detectors. After discussing photon generation processes, we study photon conversion processes in which a nonlinear material and a classical strong pump field are used modify the frequency of a second incoming low-intensity field. We show that time-ordering effects limit the efficiency of this conversion process, re-examine strategies to get around this problem, and show that it should be possible to have a clear observation of modified upconversion probabilities due to these effects, and thus have an experimental demonstration of time-ordering effects in nonlinear optics.
The fields of quantum and nonlinear optics have given rise to a variety of nonclassical states of light that have been proven to surpass certain limitations set by classical physics. Namely, certain squeezed and entangled states have been shown to beat the shot-noise limit when making precision phase measurements in interferometry, as well as write lithographic patterns that are smaller than classically allowed by the Rayleigh diffraction limit. Additionally, single-photon sources and entangled photon pairs have given rise to provably secure quantum key distribution for cryptography. Producing these quantum states of light has proven a difficult task. Nonlinear crystals, when pumped by a laser, produce pairs of single photons via the process of spontaneous parametric down conversion (SPDC). This process is mediated by the second order nonlinear susceptibility of the material. When pumped in a high gain regime, these crystals give rise to optical parametric amplification, which is a viable source of squeezed light. The vast majority of research in this area has focused on crystals that are seeded by vacuum in their two modes. This dissertation concerns the field of quantum nonlinear optics. It is an investigation into the processes that occur when nonlinear materials interact with the electromagnetic field on the single photon level. I have focused on seeding nonlinear crystals with quantum states of light, including single photons and entangled states. This process results in various states directly applicable to interferometry, imaging, and cryptography. Another application investigated is an absolute radiance measurement via stimulated parametric down conversion resulting from non-vacuum seeding of a nonlinear crystal. Additionally, other nonlinear processes, including four-wave mixing, nonlinear magneto-optical effects and coherent population trapping in warm atomic vapor involving quantum states of light are investigated. The process of seeding third-order nonlinear interactions, such as in atomic vapors, gives rise to a variety of interesting, nonclassical phenomena such as entangled image transfer and nonlocal imaging. Strong analogies between SPDC and four-wave mixing are drawn. I also experimentally show an all optical pi-only phase shift of one light beam via another in warm Cesium vapor.