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arXiv:2203.04998 · Physical Review Research

Cooperative subwavelength molecular quantum emitter arrays

R. Holzinger, S. A. Oh, Michael Reitz, Helmut Ritsch, Claudiu Genes

Published Aug 11, 2022• 17 citations
arXivHTMLPDF

Abstract

Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom. While vibrations are typically considered detrimental to coherent dynamics, we show that molecular dimers or rings can be operated as platforms for the preparation of long-lived dark superposition states aided by vibrational relaxation. In closed ring configurations, we extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence.

DOI
10.1103/physrevresearch.4.033116

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Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom. While vibrations are typically considered detrimental to coherent dynamics, we show that molecular dimers or rings can be operated as platforms for the preparation of long-lived dark superposition states aided by vibrational relaxation. In closed ring configurations, we extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence.
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.
A ring of dipole-coupled quantum emitters positioned at subwavelength distances possesses only a few radiant but many subradiant collective excitations with lifetimes growing exponentially with the atom number. These exhibit a three-dimensionally confined spatial radiation field pattern and form nanoscale high-QQQ optical resonators. Tailoring size, orientation, and distance between two rings allows for increasing the ratio of coherent ring-to-ring energy transfer versus free-space emission by orders of magnitude. In particular, the more dark and delocalized over several sites are excitons, the higher is their fidelity for transport to a second ring.
An array of N closely spaced dipole coupled quantum emitters exhibits super- and subradiance with characteristic tailorable spatial radiation patterns. Optimizing the emitter geometry and distance with respect to the spatial profile of a near resonant optical cavity mode allows us to increase the ratio between light scattering into the cavity mode and free space emission by several orders of magnitude. This leads to distinct scaling of the collective coherent emitter-field coupling vs the free space decay as a function of the emitter number. In particular, for subradiant states, the effective cooperativity increases much faster than the typical linear ∝N scaling for independent emitters. This extraordinary collective enhancement is manifested both in the amplitude and the phase profile of narrow collective antiresonances appearing at the cavity output port in transmission spectroscopy.
The interaction between light and matter has captivated physicists for centuries, from early studies of vision and refraction in ancient Greece to the development of quantum mechanics and quantum electrodynamics in the past century. While the response of a single quantum emitter to light is well understood, the radiative properties of an ensemble of closely spaced emitters are far more intricate. Coupling to a shared electromagnetic environment induces coherent and dissipative interactions between emitters, giving rise to a collective response that cannot be captured by treating them independently. In the regime of few excitations, the system hosts delocalized subradiant states, that is, coherent superpositions that are largely decoupled from the electromagnetic field and thus decay at suppressed rates. While this weak coupling makes subradiant states attractive for quantum technologies, it also renders them difficult to manipulate. At higher excitation densities, the intrinsic nonlinearity of emitters and the exponential growth of the Hilbert space make theoretical and numerical descriptions of the system and its dynamics increasingly challenging. This thesis explores two fundamental questions: How can subradiant and dark states be selectively accessed and harnessed for practical applications in quantum technologies? And how can interacting ensembles of quantum emitters be efficiently simulated to uncover their many-body physics? The first part of the thesis develops protocols for controlling and addressing dark states in free-space and waveguide-coupled atomic arrays, demonstrating their utility in quantum storage and the deterministic generation of entangled photonic states. Incorporating atomic motion, we further show that collective subradiant states can enhance cooling in dense atomic arrays, offering new avenues for controlling motional dynamics. In the second part, we introduce cumulant expansions of the equations of motion as a powerful tool to analytically and numerically investigate collective decay in the many-body regime. We first examine the collective decay of fully excited atomic arrays in free space, characterizing the onset and scaling of the superradiant burst across different geometries. In collaboration with experiments on ultracold erbium atoms in optical lattices, we provide the first direct observations of many-body collective effects in free-space ordered arrays, including early-time superradiant bursts, late-time subradiant tails, and the emergence of atomic correlations throughout the dynamics. Finally, we theoretically and numerically explore the transient formation of multi-excitation subradiant states, and demonstrate how the existence of multiple dissipation channels suppresses steady-state superradiance in extended arrays.
The efficient preparation of collective eigenstates of subwavelength-spaced optical dipoles is a prerequisite for observing their signature radiative properties and for their applications in quantum information processing. We theoretically investigate the deterministic preparation of super- and subradiant states of two dipole-coupled two-level quantum emitters at deep-subwavelength separation using the Swing-UP of quantum EmitteR population (SUPER) excitation scheme. Utilizing suitable pulse parameters for two red-detuned, time-overlapping Gaussian pulses, the SUPER scheme enables close-to-unity population inversion in the targeted collective eigenstates. Furthermore, a tunable optical phase in the SUPER scheme enables the simultaneous inversions in both pure super- and subradiant states with finite populations, thereby resulting in the preparation of hybrid collective states. These results are possible to realize with or without an optical cavity. Our approach to populating the collective eigenstates in a cavity environment paves the way for the efficient preparation of these states in the presence of environmental decoherence. Our scheme enables single-photon generation, which is measured using the second-order correlation function. We also discuss in detail possible experimental realizations, in particular using solid-state emitters and molecules.
Photon emission is the hallmark of light-matter interaction and the foundation of photonic quantum science, enabling advanced sources for quantum communication and computing. Although single-emitter radiation can be tailored by the photonic environment, the introduction of multiple emitters extends this picture. A fundamental challenge, however, is that the radiative dipole-dipole coupling rapidly decays with spatial separation, typically within a fraction of the optical wavelength. We realize distant dipole-dipole radiative coupling with pairs of solid-state optical quantum emitters embedded in a nanophotonic waveguide. We dynamically probe the collective response and identify both super- and subradiant emission as well as means to control the dynamics by proper excitation techniques. Our work constitutes a foundational step toward multiemitter applications for scalable quantum-information processing.