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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

On-Chip Stark Tuning of Molecular Resonances in Nanoprinted Crystals

Mohammad Musavinezhad, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

Published Jun 23, 2025• 0 citations
Publisher

Abstract

Organic dye molecules can be used for generating streams of single photons and feature a high level of intrinsic nonlinearity. When embedded in organic crystals, polycyclic aromatic hydrocarbon molecules such as dibenzo-terrylene (DBT) exhibit lifetime-limited electronic transitions at liquid helium temperatures. While recent studies have demonstrated promising functionalities of molecules in quantum photonic devices, deterministic control of their spatial placement and spectral resonances remains challenging.

DOI
10.1109/cleo/europe-eqec65582.2025.11109106

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Conference on Lasers and Electro-Optics•Jun 21, 2015•0 citations
Organic dye molecules can be used for generating streams of single photons and feature a high level of intrinsic nonlinearity. When embedded in organic crystals, polycyclic aromatic hydrocarbon molecules such as dibenzo-terrylene (DBT) exhibit lifetime-limited electronic transitions at liquid helium temperatures. While recent studies have demonstrated promising functionalities of molecules in quantum photonic devices, deterministic control of their spatial placement and spectral resonances remains challenging.
Dibenzoterrylene (DBT) molecules embedded in an anthracene host crystal are promising sources of single photons. They have high photostability and can be readily included in photonic structures [1] . Furthermore, when cooled to cryogenic temperatures they are spectrally stable and display fully coherent, lifetime-limited emission in the zero-phonon line (ZPL) [2] , and have a large branching ratio for this decay compared to incoherent decay involving molecular vibrations [3] . Another key characteristic of DBT-based photon sources is the proximity of their emission wavelength compared to rubidium atoms [4] , which can be exploited for quantum technology applications. However, so far fine-tuning of the emission of DBT has mainly been achieved using Stark tuning with a static electric field.
Single organic molecules hold great promise for generating, manipulating, and storing single photons. Such processes form the basis for new quantum-enhanced technologies such as sensing, communications, and computation. In this talk I will focus on a particularly promising molecule – dibenzoterrylene (DBT). When DBT is introduced into a solid crystal of anthracene it is photostable and emits light between 780 and 795 nm. When cooled to cryogenic temperature, DBT is isolated from phonon-induced dephasing meaning that the photons have a lifetime-limited. I will present recent results in growing DBT-doped anthracene crystals, introducing these to nanophotonic interfaces for enhancing the collection of photons, tuning the DBT emission wavelength to coincide with rubidium atomic absorption, and finally pump-probe spectroscopy experiments to find long-lived triplet states in DBT which will be useful for building a single-molecule quantum memory.
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.
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.
Abstract The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single-molecule scale, how a focused laser beam can locally shift by hundreds of times their natural line width and, in a persistent way, the transition frequency of organic chromophores cooled at liquid helium temperature in different host matrices. Supported by quantum chemistry calculations, the results can be interpreted as effects of a photoionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental observation is then applied to a common challenge in quantum photonics, i.e., the independent tuning and synchronization of close-by quantum emitters, which is desirable for multiphoton experiments. Five molecules that are spatially separated by about 50 μm and originally 20 GHz apart are brought into resonance within twice their line width. This tuning method, which does not require additional fabrication steps, is here independently applied to multiple emitters, with an emission line width that is only limited by the spontaneous decay and an inhomogeneous broadening limited to 1 nm. The system hence shows promise for photonic quantum technologies.
Single photons are very attractive for quantum information processing, given their long coherence time and their ability to carry information in many degrees of freedom. A current challenge is the generation of single photons in a photonic chip in order to scale up the complexity of quantum operations. Solid state emitters could offer this possibility. Quantum dots are one promising approach, but photons produced by different dots are generally distinguishable. Nitrogen-vacancy (N-V) centres in diamond are also promising, however it is challenging to place these in photonic circuits and the emitted photons have many frequencies. By contrast, dibenzoterrylene (DBT) molecules embedded in a thin film of anthracene (AC) at cryogenic temperatures produce a high yield of indistinguishable photons [1, 2]. DBT acts as a two-level system with a narrow 30 MHz near-infrared (785 nm) zero-phonon line [1]. We have proposed that a DBT molecule, deposited in the vicinity of a nanoscale waveguide, could emit these photons efficiently into the waveguide [3]. Conventional spin-coating methods [1] do not offer sufficient control over the surface coverage and the morphology of the AC crystal for deposition on photonic structures, while crystals grown with sublimation are too thick. Another method is needed.