Color centers have attracted significant attention for their applications in quantum technology, making their integration into photonic structures an essential area of research to advance the realization of quantum platforms. In particular, resonant cavities offer a promising platform for enhancing the light-matter interaction of color centers. This work explores the fabrication of microcavities embedded with fluorescent nanodiamonds using two-photon polymerization (2PP). We investigate the trade-off between nanodiamond concentration in the photoresist and the resulting structural quality and cavity Q-factor. Our results demonstrate the successful integration of nanodiamonds into cylindrical cavities doped with 0.002 wt% concentration. These cavities maintain good quality factors on the order of 105 and contain one to three fluorescent color centers. The position of the fluorescent nanodiamonds within the microcavities is confirmed using fluorescence spectroscopy, laser scanning microscopy (LSM), and Raman spectroscopy. Additionally, utilizing Finite-Difference Time-Domain (FDTD) simulations, we explore novel designs for efficient emitter-cavity coupling with color centers in 4H-Silicon Carbide (SiC) nanostructures. We optimized a double nanobeam cavity design supporting high-quality factor resonances and a \"sawfish\" cavity design for improved fabrication and light-matter interaction with color center in SiC. Building upon this knowledge, we discuss future directions for leveraging 2PP fabrication to integrate nanodiamonds with novel Whispering Gallery Modes (WGM) cavities, aiming at achieving low mode volumes to explore the Purcell effect. Therefore, this research paves the way for developing integrated devices containing nanodiamonds and WGM cavities for quantum technology applications.
Color centers have attracted significant attention for their applications in quantum technology, making their integration into photonic structures an essential area of research to advance the realization of quantum platforms. In particular, resonant cavities offer a promising platform for enhancing the light-matter interaction of color centers. This work explores the fabrication of microcavities embedded with fluorescent nanodiamonds using two-photon polymerization (2PP). We investigate the trade-off between nanodiamond concentration in the photoresist and the resulting structural quality and cavity Q-factor. Our results demonstrate the successful integration of nanodiamonds into cylindrical cavities doped with 0.002 wt% concentration. These cavities maintain good quality factors on the order of 105 and contain one to three fluorescent color centers. The position of the fluorescent nanodiamonds within the microcavities is confirmed using fluorescence spectroscopy, laser scanning microscopy (LSM), and Raman spectroscopy. Additionally, utilizing Finite-Difference Time-Domain (FDTD) simulations, we explore novel designs for efficient emitter-cavity coupling with color centers in 4H-Silicon Carbide (SiC) nanostructures. We optimized a double nanobeam cavity design supporting high-quality factor resonances and a "sawfish" cavity design for improved fabrication and light-matter interaction with color center in SiC. Building upon this knowledge, we discuss future directions for leveraging 2PP fabrication to integrate nanodiamonds with novel Whispering Gallery Modes (WGM) cavities, aiming at achieving low mode volumes to explore the Purcell effect. Therefore, this research paves the way for developing integrated devices containing nanodiamonds and WGM cavities for quantum technology applications.
Diamond has emerged as a leading host material for solid-state quantum emitters, quantum memories, and quantum sensors. However, the challenges in fabricating photonic devices in diamond have limited its potential for use in quantum technologies. While various hybrid integration approaches have been developed for coupling diamond color centers with photonic devices defined in a heterogeneous material, these methods suffer from either large insertion loss at the material interface or evanescent light-matter coupling. Here, we present a new technique that enables the deterministic assembly of diamond color centers in a silicon nitride photonic circuit. Using this technique, we observe Purcell enhancement of silicon vacancy centers coupled to a silicon nitride ring resonator. Our hybrid integration approach has the potential for achieving the maximum possible light-matter interaction strength while maintaining low insertion loss and paves the way toward scalable manufacturing of large-scale quantum photonic circuits integrated with high-quality quantum emitters and spins.
Abstract The progress in integration of nanodiamond with photonic devices is analyzed in the light of quantum optical applications. Nanodiamonds host a variety of optically active defects, called color centers, which provide rich ground for photonic engineering. Theoretical introduction describing light and matter interaction between optical modes and a quantum emitter is presented, including the role of the Debye–Waller factor typical of color center emission. The synthesis of diamond nanoparticles is discussed in an overview of methods leading to experimentally realized hybrid platforms of nanodiamond with gallium phosphide, silicon dioxide, and silicon carbide. The trade‐offs in the substrate index of refraction values are reviewed in the context of the achieved strength of light and matter interaction. Thereby, the recent results on the growth of color center‐rich nanodiamond on prefabricated silicon carbide microdisk resonators are presented. These hybrid devices achieve up to fivefold enhancement of the diamond color‐center light emission and can be employed in integrated quantum photonics.
The development of integrated quantum technologies relies on efficient single-photon sources and deterministic quantum operations. Solid-state quantum emitters coupled to nanophotonic structures present a promising solution. This work investigates color centers in nanodiamonds,particularly Germanium Vacancy (GeV) [1], Silicon Vacancy (SiV), and Magnesium Vacancy (MgV) centers, a novel, understudied emitter [2], at both room and cryogenic temperatures. These nanodiamonds are chosen for their stability and superior coherence properties at cryogenic conditions. To collect their emission we have successfully deposited a single GeV- nanodiamond on tapered optical nanofibers by gently contacting a diluted droplet to the nanofiber [3], demonstrating an average coupling of 15% into a conventional optical fiber through the confined evanescent field of the nanofiber mode and single photon emission. Building on this achievement, we aim to study the system at cryogenic temperatures, which should enable the demonstration of efficient and indistinguishable single photons coupling to conventional optical fibers.Current collection efficiencies are intrinsically limited to 30% with the nanofiber[4], and improving light-matter coupling efficiency remains a key goal for high-performance single-photon sources and more advanced applications.To achieve this, we are investigating a newly developed technique [5]: the deterministic fabrication of dielectric and plasmonic nanostructures directly on the nanofiber surface using an “electron beam induced deposition” (EBID). The precision and versatility of this technique openthe way to different applications: Purcell enhancement of the quantum emitter emission using metallic nanoantennas and efficient light-matter coupling using dielectric structures. Our first calculation shown that optimizing the composition, geometry, and placement of these nanostructures a simple pattern of carbon pillars around the emitter should increase coupling efficiency up to 69% while maintaining high transmission in the nanofiber. We also demonstratethe fabrication of those nanostructures on top of the nanofiber.This work advances integrated nanophotonic devices for single-photon sources.[1] M. Nahra et al.,Single germanium vacancy centers in nanodia-monds with bulk-like spectral stability, AVS Quantum Science3(1), (2021).[2] E. Corte et al, Magnesium-Vacancy Optical Centers in Diamond, ACS Photonics, 10(1), p101-110, (2023)[3] Pierini et al. Highly Photostable Perovskite Nanocubes : TowardIntegrated Single Photon Sources Based on Tapered Nanofibers.ACS Photonics, 7(8), p.2265-2272, (2020).[4] Fujiwara et al., Highly efficient coupling of photons from na-noemitters into single-mode optical fibers, Nano Letters, 11(10),4362–4365, (2011).[5] A.Balena et al, Deterministic Bottom-Up Fabrication of Plasmonic Nanostructures on OpticalNanofibers via Blurred Electron Beam Deposition (soon to be published in Advance Material).
Building quantum networks requires efficient coupling of solid-state quantum emitters to photonic devices. Tinvacancy center (SnV) has attracted much interest for having long spin coherence times at temperatures above 1 K. Employing SnV as an optically addressable qubit requires integration with photonic structures to both route the emitted photons and enhance the light-matter interaction. We present incorporation of high-quality SnV centers with narrow linewidths in suspended diamond waveguides. Furthermore, we fabricate photonic crystal cavities in diamond with embedded SnV centers. We observe strong intensity enhancement of the photon emission when the cavity is resonant with the color center. Time-resolved photoluminescence measurements confirm that this effect is due to radiative Purcell enhancement of the spontaneous emission. Finally, we demonstrate Stark tuning of transition frequency of SnV centers, essential for multiemitter applications. These results are a significant step toward color-center-based quantum information processing applications without the need for dilution refrigerators.
For cavity quantum electrodynamics systems (cavity-QED) to play a role in quantum information processing applications and in quantum networks, they must be robust and scalable in addition to having a suitable method for the generation, processing and storage of quantum bits. One solution is to develop a composite system that couples a nitrogen vacancy (NV) center in diamond to a whispering gallery mode supported by a fused silica microsphere. Such a system is motivated by the optical and electron-spin properties of the NV center. The NV center is the leading spin-qubit and exhibits atomic like linewidths at cryogenic temperatures and has spin coherence times greater than milliseconds at room temperature. These long coherence times, coupled with nanosecond scale spin readout and manipulation times, allow for millions of quantum operations to be processed. Silica whispering gallery resonators are the only class of microresonators with quality factor high enough to reach the strong coupling regime, which is necessary for some quantum information processing applications. \n \nIntegrating these two components into a system that could position a diamond nanopillar near the surface of a deformed-double stemmed microsphere system, with nanometer precision, at 10 K was a major achievement of this research. Cavity resonances in deformed microspheres can be excited with a free-space coupling technique which simplifies their integration into cryogenic environments. In these intentionally deformed resonators, an enhanced evanescent field decay length was observed at specific locations along the ray orbit. The double-stem arrangement enables the cavity resonance to be tuned over 450 GHz, with sub-10 MHz resolution, at 10 K. These two features, the enhanced decay length and broad range tuning with high resolution, are indispensible tools for cavity-QED studies with silica microspheres. \n \nDiamond nanopillars were fabricated from single crystal diamond with diameters as small as 140 nm in order to maintain a high quality factor. Studies were conducted on NV centers in nanopillars and bulk diamond to determine their suitability for cavity-QED applications. In an attempt to increase the light-matter interaction between NV centers and whispering gallery modes, diamond substrates were optically characterized that were irradiated with nitrogen ions.
With their ability to process and transfer quantum information, large-scale entanglement-based quantum networks could be at the heart of a new age of quantum information, enabling fundamentally new applications such as distributed quantum computation, quantum communication, and quantum enhanced sensing. Due to their long spin coherence, controllable local qubit registers and optically active spins, color centers in diamond are prime candidates for nodes of such a network, and have enabled some of the most advanced quantum network demonstrations to date. These demonstrations include the distribution of a 3-node GHZ state across a quantum network, entanglement swapping, entanglement distillation, and memory-enhanced quantum communication. To move beyond current proof-of-principle networks, a further increase of entanglement generation rates is crucial. This thesis presents theoretical and experimental work on enhancing the spin-photon interface of color centers in diamond to achieve this goal, making use of the Purcell effect. The discussed work follows two main directions: embedding of color centers in open, tuneable Fabry-Perot micro-cavities, and in all-diamond photonic crystal cavities. First, we describe theoretical and experimental progress towards cavity-enhanced quantum networks based on nitrogen-vacancy (NV) centers in diamond. Due to their first order sensitivity to electric fields, we choose to embed NV centers in microns-thin diamond membranes that can be integrated into open fiber-based micro-cavities. We develop analytical methods to optimize the design of such open cavity systems for maximum Purcell enhancement of embedded color centers. We demonstrate a method to fabricate optically coherent NV centers in microns-thin diamond membranes, and use such structures to demonstrate the resonant excitation and detection of coherent, Purcell enhanced NV emission. A theoretical model in excellent agreement with our results suggests our system can improve entanglement rates between distant NV centers by two orders of magnitude with near-term improvements to the setup. Second, we describe progress towards an efficient spin-photon interface of group-IV color centers in diamond by coupling them to photonic nanostructures, allowing for large-scale integration. Due to their first-order insensitivity to electric fields, group-IV color centers can be brought in close proximity to surfaces (~ 100 nm), allowing for sub-wavelength mode volumes and thus very high Purcell factors. We numerically optimize photonic crystal cavity designs to maximize the Purcell enhancement of embedded emitters, test the robustness of our designs to real-world fabrication imperfections, and devise a method to efficiently interface nanophotonic structures. We then proceed to fabricate all-diamond photonic crystal cavities, making use of a dry etching technique that is selective to different crystallographic directions, and characterize the resulting optical quality factors. Finally, we marry the developed fabrication methods to fabricate microns-sized diamond platelets that can be transferred from a holding frame in a controlled fashion. This capability could be crucial for the realization of hybrid photonic circuits that we expect to be at the heart of future large-scale quantum networks.