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arXiv:1702.00660 · Physical Review A

Quantum nonlinear optics without photons

Roberto Stassi, Vincenzo Macrí, Anton Frisk Kockum, Omar Di Stefano, Adam Miranowicz, Salvatore Savasta, Franco Nori

Published Aug 9, 2017• 80 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreva.96.023818

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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.
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.
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.
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.
Mediated by the interactions with quantum vacuum fields, a probe laser field propagating in a nonlinear optical medium can generate new pair of light fields over a broad spectral range via spontaneous parametric process. Such process is inherently independent of the incident direction of light and reciprocal thus far, due to the direction-independent field-vacuum interactions. In this work, we experimentally demonstrate within sodium atomic vapors that such spontaneous parametric process can be nonreciprocal by unidirectionally coupling it to another pumped four-wave mixing process. Thanks to the broad bandwidth of the spontaneous parametric process, in combination with the Doppler and power-induced broadening of atomic energy levels, we achieve optical isolation with isolation ratio >25 dB over a bandwidth larger than 100 GHz. Considering that both spontaneous parametric processes and the pumped four-wave mixing have been realized in diverse solid photonic platforms, the demonstrated concept can motivate further explorations in the design of integrated magnetic-free broadband optical nonreciprocity via the interactions between nonlinear optical processes.
Pairs of entangled photons are crucial for photonic quantum technologies. The demand for integrability and multi-functionality suggests 'flat' platforms - ultrathin layers and metasurfaces - as sources of photon pairs. With the success in demonstrating spontaneous parametric down-conversion (SPDC) from such sources, an alternative process to generate photon pairs, spontaneous four-wave mixing (SFWM), also starts to attract interest. In materials with nonzero second-order nonlinear susceptibility χ(2)χ^{(2)}χ(2), SFWM can generate photon pairs both directly, through the third-order nonlinear susceptibility χ(3)χ^{(3)}χ(3), and in a cascaded way, through second harmonic generation (SHG) followed by SPDC. Usually, the cascaded process is more efficient. Here, we show that in a thin layer, direct SFWM dominates, because the wavevector mismatch for SFWM is much smaller than for SHG or SPDC. To demonstrate it, we implement the photon pair generation via SFWM in a second-order nonlinear material - a thin layer of lithium niobate (LN). The existence of both second- and third-order nonlinear processes offers broader opportunities for quantum state engineering.
We investigate the nonlinear interaction between two photons in a single-input pulse at an atomic two-level nonlinearity. A one-dimensional model for the propagation of light to and from the atom is used to describe the precise spatiotemporal coherence of the two-photon state. It is shown that the interaction generates spatiotemporal entanglement in the output state similar to the entanglement observed in parametric down-conversion. A method of generating photon pairs from coherent pump light using this quantum-mechanical four-wave mixing process is proposed.