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arXiv:2602.18517

Vapor Phase Assembly of Molecular Emitter Crystals for Photonic Integrated Circuits

Arya D. Keni, Christian M. Lange, Adhyyan S. Mansukhani, Emma Daggett, Ankit Kundu, Ishita Agarwal, Patrick Bak, Benjamin Cerjan, Jonathan D. Hood

quant-phSubmitted Feb 19, 2026• Announced Feb 23, 2026
arXivHTMLPDF

Abstract

Organic molecules embedded in an organic matrix exhibit lifetime-limited optical coherence and bright emission at cryogenic temperatures below 3 K. Here we present a simple vapor-phase growth method for synthesizing optically thin DBT-doped anthracene crystals that are compatible with integrated nanophotonics. The crystals are ~200 nm thick with sub-nm surface roughness and a tunable lateral dimension of up to 200 $μ$m. The molecular transitions remain narrow and spectrally stable, with inhomogeneous broadening below 100 GHz, comparable to DBT in bulk anthracene. The dopant density is tunable up to several hundred molecules per $μ$m$^2$, ensuring emitters within the near-field of nanophotonic structures. We demonstrate that the crystals can be micropositioned onto integrated photonic devices with the molecular dipole aligned to the optical mode. This approach opens a path toward on-chip single-photon sources and collective many-emitter effects.

Comments
15 pages (7 page main, 7 page supplemental, 1 page references). 5 main figures, 9 supplemental figures

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Organic molecules embedded in an organic matrix exhibit lifetime-limited optical coherence and bright emission at cryogenic temperatures below 3 K. Here we present a simple vapor-phase growth method for synthesizing optically thin DBT-doped anthracene crystals that are compatible with integrated nanophotonics. The crystals are ~200 nm thick with sub-nm surface roughness and a tunable lateral dimension of up to 200 μμμm. The molecular transitions remain narrow and spectrally stable, with inhomogeneous broadening below 100 GHz, comparable to DBT in bulk anthracene. The dopant density is tunable up to several hundred molecules per μμμm2^22, ensuring emitters within the near-field of nanophotonic structures. We demonstrate that the crystals can be micropositioned onto integrated photonic devices with the molecular dipole aligned to the optical mode. This approach opens a path toward on-chip single-photon sources and collective many-emitter effects.
We present a hybrid solid-state cavity quantum electrodynamics (QED) platform that integrates a high density of coherent organic molecules with high-quality-factor nanophotonics. Thin anthracene crystals doped with dibenzoterrylene (DBT) are mechanically transferred onto prefabricated silicon nitride photonic crystal cavities, preserving both the cavity quality and molecular coherence. This approach decouples emitter synthesis from nanofabrication, providing a pathway for integrating other types of emitters. The high density of molecular emitters results in up to ten molecules being coupled to a single cavity. By tuning pairs of molecules into resonance within a single cavity mode, we observe cavity-mediated interactions in both dispersive and dissipative regimes. These results establish an accessible route to deterministic on-chip single- and multiphoton sources.
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The physical realisation of a photonic quantum computer requires a reliable, fast, ondemand source of single indistinguishable photons. A promising candidate for one of these sources is a single dye molecule in a solid state matrix placed within the evanescent field of a photonic waveguide. This thesis explores the possibility of coupling of single dibenzoterrylene (DBT) molecules in an anthracene matrix to a silicon nitride waveguide at room temperature. I first discuss the theory by which photons from a DBT molecule can be evanescently coupled to a ridge waveguide. I present a novel growth method to form DBT-doped anthracene crystals which is very promising for applications to photonic devices. I discuss the methodology and the theory of such growth. I describe the confocal microscope I developed and used to image and characterise the emission of the single DBT molecules embedded in these crystals. My measurements show that the molecules are extremely stable single quantum emitters with a well-de ned polarization relative to the crystal axes. Measurements of the saturation intensity at room temperature allow me to estimate that a single DBT molecule could deliver at least 1012 photons before bleaching. This method of growth was used to deposit DBT molecules on top of a silicon nitride ridge waveguide. The results of the coupling experiment are shown. These include confocal images, saturation and lifetime measurements. The coupling efficiency is calculated and compared to what was simulated. The challenges of such structures are then presented. To tackle these challenges I deposited the molecules on top of lithium niobate and in silicon nitride slots. I conclude with a proposal for constructing the best photonic structure which would guarantee an easy deposition of the molecules and high coupling efficiencies.
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Engineering the photonic environment using lattices of coupled resonators, which we refer to as lattice quantum electrodynamics (QED), provides a route to control both the spontaneous emission of individual quantum emitters and the photon-mediated interactions between them. Here we introduce an optical lattice QED platform based on individual dibenzoterrylene (DBT) molecules embedded in anthracene crystals and coupled to lattices of open optical microcavities. This hybrid architecture benefits from narrow-linewidth molecular emitters, site-resolved optical access, engineered coupled-resonator bands, and compatibility with established molecular frequency-tuning techniques. As a proof-of-principle demonstration, we observe emitter-photon bound states formed when the optical transition of a single molecule is tuned to the band gap of a Su-Schrieffer-Heeger (SSH) cavity lattice. These in-gap states display directional localization and photon emission on a single sublattice, inherited from the vacancy-induced topological edge modes of the underlying SSH lattice. Our results establish open-cavity lattices coupled to DBT molecules as a versatile architecture for engineering many-emitter quantum optical systems with controllable photon-mediated interactions.