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arXiv:2510.19992

Quantum Nonlinear Response of Emitter Lattices

Blas Durá-Azorín, Antonio I. Fernández‐Domínguez, Alejandro Manjavacas

Published Oct 22, 2025• 0 citations
arXivHTMLPDF

Abstract

We theoretically investigate the emergence of quantum nonlinearities in the optical response of lattices of two-level quantum emitters coherently driven by a laser. For subwavelength lattice periods, where the system behaves as a quantum metasurface, we find that a resonant incident plane wave can populate excitonic Bloch states with parallel wavevectors different from the incident field, including those lying outside the light cone. Closely related to resonance fluorescence, the far-field emission from the system in the strong-driving regime is dominated by a broadband background of photons spanning a wide range of frequencies and wavevectors. Moreover, we show that, for periods approaching the driving wavelength, the emitter lattice enters in a bistable regime due to the renormalization of the driving rate, in striking contrast with its classical (bosonic) analog. This bistable behavior enables the selective activation and deactivation of the optical quantum nonlinearities of the system.

DOI
10.48550/arxiv.2510.19992

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We theoretically investigate the emergence of quantum nonlinearities in the optical response of lattices of two-level quantum emitters coherently driven by a laser. For subwavelength lattice periods, where the system behaves as a quantum metasurface, we find that a resonant incident plane wave can populate excitonic Bloch states with parallel wavevectors different from the incident field, including those lying outside the light cone. Closely related to resonance fluorescence, the far-field emission from the system in the strong-driving regime is dominated by a broadband background of photons spanning a wide range of frequencies and wavevectors. Moreover, we show that, for periods approaching the driving wavelength, the emitter lattice enters in a bistable regime due to the renormalization of the driving rate, in striking contrast with its classical (bosonic) analog. This bistable behavior enables the selective activation and deactivation of the optical quantum nonlinearities of the system.
Abstract We study theoretically the nonlinear optical response of a super-lattice of regularly arranged three-level identical quantum emitters with a doublet in the excited state to the action of a monochromatic electromagnetic field quasi-resonant to optical transitions in the emitter, using into account the dephasing of the system. The total retarded dipole-dipole interaction of the emitters is accounted for in the mean-field approximation. This interaction plays the role of positive feedback, which (in combination with the immanent nonlinearity of emitters themselves) leads to multistability of the super-lattice response. The stability of different response branches is analyzed using the Lyapunov exponents’ method. Another important property of the super-lattice is its high reflectance in a certain frequency range; i.e., within this range, the super-lattice operates as a perfect nanometer mirror; moreover, reflection can be switched to transmission changing slightly the incident field amplitude (bistability). The possibility of the application of the above-mentioned super-lattice optical properties in nanophotonics is discussed.
Subwavelength arrays of quantum emitters offer an efficient free-space approach to coherent light-matter interfacing, using ultracold atoms or two-dimensional solid-state quantum materials. The combination of collectively suppressed photon losses and emerging optical nonlinearities due to strong photon coupling to mesoscopic numbers of emitters holds promise for generating nonclassical light and engineering effective interactions between freely propagating photons. While most studies have thus far relied on numerical simulations, we describe here a diagrammatic Green's function approach that permits analytical investigations of nonlinear processes. We illustrate the method by deriving a simple expression for the scattering matrix that describes photon-photon interactions in an extended two-dimensional array of quantum emitters and reproduces the results of numerical simulations of coherently driven arrays. The approach yields intuitive insights into the nonlinear response of the system and offers a promising framework for the systematic development of a theory for interacting photons and many-body effects on collective radiance in two-dimensional arrays of quantum emitters. Published by the American Physical Society 2024
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.
In the strong coupling regime of cavity QED where the characteristic damping rates are orders of magnitude below the coherent coupling, resolved multi-photon resonances can be observed for strong enough driving strength. In a certain frequency range, the external coherent drive field hits multi-photon resonances which correspond to very high order transitions that cannot be excited at the given power of the driving field. We found that in this range the cavity field evolves into a robust semiclassical solution which is the mixture of the vacuum and an excited quasi-classical state. The system is reminiscent of optical bistability, however, here a single atom produces a telegraph signal for the outgoing intensity by switching between two states with large photon number difference. We calculate this behavior also for the Tavis-Cummings model representing three qubits in an existing circuit QED experimental setting.
The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.
Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative aspects such as dipole-dipole interactions and subradiance find applications in the design of nanoscale coherent light sources and highly-reflective quantum metasurfaces made up of hundreds of optically trapped atoms, in the implementation of topological quantum optics on subwavelength arrays of emitters, in quantum metrology and quantum information. The quick bursts of radiation from a collection of quasi-indistiguishable emitters provides an alternative approach to standard lasers by introducing superradiant lasers operating at extremely low intracavity power. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity in light-matter systems by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitters ensembles. These analytical approaches are then also extended to frequency disordered or vibronically coupled quantum emitter ensembles with wide relevance ranging from atoms in optical lattices, quantum dots in solid state environments or molecular quantum systems.