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 $|S_{11}|$ 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.
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∣ 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.
The realization of strong nonlinear coupling between single photons has been a long-standing goal in quantum optics and quantum information science, promising wide impact applications, such as all-optical deterministic quantum logic and single-photon frequency conversion. Here, we report an experimental observation of the strong coupling between a single-photon and a two-photon Fock state in an ultrastrongly-coupled circuit-QED system. This strong nonlinear interaction is realized by introducing a detuned flux qubit working as an effective coupler between two modes of a superconducting coplanar waveguide resonator. The ultrastrong light–matter interaction breaks the excitation number conservation, and an external flux bias breaks the parity conservation. The combined effect of the two enables the strong one–two-photon coupling. Quantum Rabi-like avoided crossing is resolved when tuning the two-photon resonance frequency of the first mode across the single-photon resonance frequency of the second mode. Within this new photonic regime, we observe the thresholdless second harmonic generation for a mean photon number below one. Our results represent a key step towards a new regime of quantum nonlinear optics, where individual photons can deterministically and coherently interact with each other in the absence of any stimulating fields. Systems with strong photon-photon interactions enable advanced quantum optical applications as well as the study of highly correlated light-matter states. Here the authors report strong coupling between single- and two-photon states in a superconducting circuit, enabling a new regime of nonlinear quantum optics.
Photon-based quantum logic gate has substantial advantages over conventional atom-based designs as a result of a longer coherence time and an inherent compatibility with quantum communication protocol of flying qubits, photons. As a vital logic gate for universal quantum computing, the two-photon controlled-phase gate demands a few-photon nonlinearity, which historically suffers from either an indeterministic nature in the linear optics regime, or a weak nonlinearity within naturally-occurring materials in the nonlinear optics regime. It is intriguing yet challenging to deliver a logic gate design by exploiting a genuine fewphoton nonlinearity. In this dissertation, we study a particular one-dimensional quantum nanophotonic system that offers the desired few-photon nonlinearity through light-matter interactions in the quantum limit (i.e., between light quanta of photons and individual material formation of atoms). Towards this end, we study the exotic photonic trimer state generation to frst demonstrate few-photon nonlinearity. Then we report the breakdown of the non-Hermitian Hamiltonian for correlated multi-photon process to unveil the non-trivial effects of few-photon nonlinearity. Finally by exploiting such a nonlinearity, we present a deterministic two-photon controlled-phase gate proposal, and further showcase universal quantum logic gate designs in quantum nanophotonic systems.
The application of quantum states of light such as entangled photons, for example, created by parametric down conversion, has experienced tremendous progress in the almost 40 years since their first experimental realization. Initially, they were employed in the investigation of the foundations of quantum physics, such as the violation of Bell's inequalities and studies of quantum entanglement. They later emerged as basic platforms for quantum communication protocols and, in the recent experiments on single-photon interactions, in photonic quantum computation. These applications aim at the controlled manipulation of the photonic degrees of freedom, and therefore rely on simple models of matter, where the analysis is simpler. Furthermore, quantum imaging with entangled light can achieve enhanced resolution, and quantum metrology can overcome the shot noise limit for classical light. This Account focuses on an entirely different emerging class of applications using quantum light as a powerful spectroscopic tool to reveal novel information about complex molecules. These applications utilize two appealing properties of quantum light: its distinct intensity fluctuations and its nonclassical bandwidth properties. These give rise to new and surprising behavior of nonlinear optical signals. Nonclassical intensity fluctuations can enhance nonlinear optical signals relative to linear absorption. For instance, the two-photon absorption of entangled photon pairs scales linearly (rather than quadratically) in the photon flux, just like a single photon absorption. This enables nonlinear quantum spectroscopy of photosensitive, for example, biological, samples at low light intensities. We will discuss how the two-photon absorption cross section becomes a function of the photonic quantum state, which can be manipulated by properties of the entangled photon pairs. In addition, the quantum correlations in entangled photon states further influence the nonlinear signals in a variety of ways. Apart from affecting the signal's scaling with intensity, they also constitute an entirely new approach to shaping and controlling excitation pathways in molecular aggregates in a way that cannot be achieved with shaped classical pulses. This is because between the two absorption events in entangled two-photon absorption, the light and material system are entangled. Classical constraints for the simultaneous time and frequency resolution can thus be circumvented, since the two are not Fourier conjugates. Here we review the simplest manifestation of quantum light spectroscopy, two-photon absorption spectroscopy with entangled photons. This will allow us to discuss exemplarily the impact of quantum properties of light on a nonlinear optical signal and explore the opportunities for future applications.
Non-Hermitian quantum mechanics has emerged as a powerful framework for describing open quantum systems, particularly in optical platforms where engineered gain and loss can lead to exotic phenomena. This paper theoretically investigates the synthesis of non-Hermitian quantum light within driven photonic crystals. We propose a methodology that leverages the unique dispersion engineering capabilities of photonic crystals, coupled with controlled introduction of gain and loss elements and strong classical driving fields. Our approach aims to generate novel quantum light states characterized by non-Hermitian properties, such as modified photon statistics, entanglement, and the manifestation of exceptional points in quantum correlations. The paper outlines the theoretical foundations, reviews relevant prior work in non-Hermitian optics and quantum light generation in photonic structures, and details a specific methodology involving coupled resonator systems and nonlinear optical processes. We predict that such driven non-Hermitian photonic crystals can offer unprecedented control over quantum light properties, enabling the generation of squeezed states with enhanced sensitivity, robust entangled photon pairs, and potentially new regimes for quantum metrology and information processing. The discussion addresses the implications of these findings for fundamental quantum optics and their potential experimental realizations, highlighting the challenges and promising avenues for future research.
Multiphoton absorption processes have a nonlinear dependence on the amplitude of the incident optical field, i.e., the number of photons. However, multiphoton absorption is generally weak and multiphoton events occur with extremely low probability. Consequently, it is extremely challenging to engineer quantum nonlinear devices that operate at the single photon level and the majority of quantum technologies have to rely on single photon interactions. Here we demonstrate experimentally and theoretically that exploiting coherent absorption of N=2 NOON states makes it possible to enhance the number of two-photon states that are absorbed by at most a factor of 2 with respect to a linear absorption process. An absorbing metasurface placed inside a Sagnac-style interferometer into which we inject an N=2 NOON state, exhibits two-photon absorption with 40.5 efficiency, close to the theoretical maximum. This high probability of simultaneous absorption of two photons holds the promise for applications in fields that require multiphoton upconversion but are hindered by high peak intensities.
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.