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arXiv:2308.08037 · Nature Physics

Superradiant and subradiant states in lifetime-limited organic molecules through laser-induced tuning

Christian Lange, Emma Daggett, Valentin Walther, Libai Huang, Jonathan D. Hood

Published Feb 19, 2024• 43 citations
arXivHTMLPDF

Abstract

Abstract An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning. The molecules are embedded as defects in an organic nanocrystal. The pump light redistributes charges in the nanocrystal and dramatically increases the likelihood of resonant molecules. The frequency spectra, lifetimes, and second-order correlation agree with a simple quantum model. This scalable tuning approach with organic molecules provides a pathway for observing collective quantum phenomena in sub-wavelength arrays of quantum emitters.

DOI
10.1038/s41567-024-02404-4

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Abstract An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning. The molecules are embedded as defects in an organic nanocrystal. The pump light redistributes charges in the nanocrystal and dramatically increases the likelihood of resonant molecules. The frequency spectra, lifetimes, and second-order correlation agree with a simple quantum model. This scalable tuning approach with organic molecules provides a pathway for observing collective quantum phenomena in sub-wavelength arrays of quantum emitters.
We implement permanent spectral tuning to bring lifetime-limited emitters into collective resonance within an integrated photonic cavity. This addresses a fundamental challenge in solid-state cavity QED: combining multiple coherent quantum emitters with scalable nanophotonics. Our hybrid approach decouples emitter synthesis from nanophotonic fabrication using straightforward techniques that make cavity QED broadly accessible. High doping densities allow us to couple several coherent emitters to a single cavity mode, while optically-induced frequency shifting provides long-lived spectral control. By tuning two molecules into resonance, we demonstrate controlled formation of collective quantum states, establishing a scalable platform for many-body cavity QED. This opens pathways toward chemically-designed quantum systems where optical properties are engineered through synthetic chemistry.
Abstract The control and manipulation of quantum-entangled states is crucial for the development of quantum technologies. A promising route is to couple solid-state quantum emitters through their optical dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Here we implement hyperspectral imaging to identify pairs of coupled dibenzanthanthrene molecules, and find distinctive spectral signatures of maximally entangled superradiant and subradiant electronic states by tuning the molecular optical resonances with Stark effect. We demonstrate far-field selective excitation of the long-lived subradiant delocalized state with a laser field tailored in amplitude and phase. Optical nanoscopy of the coupled molecules unveils spatial signatures that result from quantum interferences in their excitation pathways and reveal the location of each emitter. Controlled electronic-states superposition will help deciphering more complex physical or biological mechanisms governed by the coherent coupling and developing quantum information schemes.
Abstract We present numerical calculations of the cooperative photoluminescence spectra of two dipole–dipole–coupled dibenzoterrylene molecules embedded in an anthracene crystal at liquid-helium temperature. Using master-equation formalism for non-identical two-level emitters, we reproduce the excitation spectra recently observed in experiment. The excellent agreement between the simulations, analytical model, and measurements confirms the observation of controllable molecular entanglement and validates the theoretical framework. The approach provides an efficient computational tool for predicting and controlling cooperative photoluminescence in solid-state molecular systems. These results establish a basis for future experiments aimed at achieving optical entanglement of organic molecules and developing quantum photonic devices.
The control and manipulation of quantum-entangled states is crucial for the development of quantum technologies. A promising route is to couple solid-state quantum emitters through their optical dipole-dipole interactions. Entanglement in itself is challenging, as it requires both nanometric distances between emitters and nearly degenerate electronic transitions. Here we implement hyperspectral imaging to identify pairs of coupled dibenzanthanthrene molecules, and find distinctive spectral signatures of maximally entangled superradiant and subradiant electronic states by tuning the molecular optical resonances with Stark effect. We demonstrate far-field selective excitation of the long-lived subradiant delocalized state with a laser field tailored in amplitude and phase. Optical nanoscopy of the coupled molecules unveils spatial signatures that result from quantum interferences in their excitation pathways and reveal the location of each emitter. Controlled electronic-states superposition will help deciphering more complex physical or biological mechanisms governed by the coherent coupling and developing quantum information schemes.
Quantum light-matter interactions form the basis of many quantum technologies and much fundamental research. Organic molecules are an impressive platform for the generation of quantum light, both as single photon emitters and as collective systems. In this work, I investigate quantum light-matter interactions with molecules of dibenzoterrylene in crystals of anthracene. I outline methods to grow dibenzoterrylene-doped anthracene crystals, and I characterize the optical properties of cryogenically cooled molecules. I prepare collective systems composed of pairs of molecules interacting through their free-space electromagnetic fields. I demonstrate a method to tune interacting molecules into resonance to form superradiant and subradiant collective states. Finally, I present a platform for solid-state cavity QED based on molecules of dibenzoterrylene coupled to a nanophotonic cavity. This demonstration establishes a route toward scalable deterministic photon generation with molecules. I also tune pairs of cavity-coupled molecules into resonance to form distributed collective states, opening the door to cavity-mediated many-body interactions.
When an ensemble of quantum emitters interacts with a common radiation field, their emission becomes collective, giving rise to superradiant and subradiant states, characterized by broadened and narrowed linewidths. In this work, we propose to harness subradiant states for quantum metrology; such states naturally arise in subwavelength-spaced atomic arrays in free space and in small ensembles of emitters coupled to one-dimensional waveguides. We demonstrate that their collective optical response yields sharp, narrow features in the transmittance spectrum, which can be used to enhance sensitivity to external perturbations. This improved sensitivity can be applied to atomic clock operation, spatially resolved imaging of emitter positions, and enables precise detection of both global and spatially varying detunings (such as those induced by electromagnetic fields or gravitational gradients).