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arXiv:2108.03727

Nanofibers coated with Rare-Earth complexes

Ori Ezrah Mor, Tal Ohana, Adrien Borne, Yael Diskin‐Posner, Asher, Maor, Yaffe, Omer, Abraham Shanzer, Dayan, Barak

Published Aug 8, 2021• 0 citations
arXivHTMLPDF

Abstract

Crystals and fibers doped with Rare Earth (RE) ions provide the basis to most of today's solid-state optical systems, from lasers and telecom devices to emerging potential quantum applications such as quantum memories and optical to microwave conversion. The two platforms, doped crystals and doped fibers, seem mutually exclusive, each having its own strengths and limitations- the former providing high homogeneity and coherence, and the latter offering the advantages of robust optical waveguides. Here we present a hybrid platform that does not rely on doping but rather on coating the waveguide - a tapered silica optical fiber - with a monolayer of complexes, each containing a single RE ion. The complexes offer an identical, tailored environment to each ion, thus minimizing inhomogeneity and allowing tuning of their properties to the desired application. Specifically, we use highly luminescent Yb$^{+3}$[Zn(II)$_{MC}$(QXA)] complexes, which isolate the RE ion from the environment and suppress non-radiative decay channels. We demonstrate that the beneficial optical transitions of the Yb$^{+3}$ are retained after deposition on the tapered fiber, and observe an excited-state lifetime of over 0.9 ms, on par with state-of-the-art Yb doped inorganic crystals.

DOI
10.48550/arxiv.2108.03727

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Tapered Optical Fibers Coated with Rare-Earth Complexes for Quantum Applications

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High Resolution Image Download MS PowerPoint Slide Crystals and fibers doped with rare-earth (RE) ions provide the basis for most of today’s solid-state optical systems, from lasers and telecom devices to emerging potential quantum applications such as quantum memories and optical to microwave conversion. The two platforms, doped crystals and doped fibers, seem mutually exclusive, each having its own strengths and limitations, the former providing high homogeneity and coherence and the latter offering the advantages of robust optical waveguides. Here we present a hybrid platform that does not rely on doping but rather on coating the waveguide─a tapered silica optical fiber─with a monolayer of complexes, each containing a single RE ion. The complexes offer an identical, tailored environment to each ion, thus minimizing inhomogeneity and allowing tuning of their properties to the desired application. Specifically, we use highly luminescent Yb 3+ [Zn(II) MC (QXA)] complexes, which isolate the RE ion from the environment and suppress nonradiative decay channels. We demonstrate that the beneficial optical transitions of the Yb 3+ are retained after deposition on the tapered fiber and observe an excited-state lifetime of over 0.9 ms, on par with state-of-the-art Yb-doped inorganic crystals.

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In this thesis, we study the single-photon source using a rare-earth (RE) ion doped in a tapered fiber.Single-photon sources are key components for various optical quantum information technologies, and the development of low-cost single-photon sources has been desired for their implementation.A wide variety of emitters for single-photon sources have been studied.Among these emitters, RE ions have attracted much attention as single-photon emitters due to their high stability of luminescence and the sharpness of the emission spectrum with 4f transitions.In our single-photon source, we obtain spatially isolated single RE ions, which are separated from each other beyond the diffraction limit by tapering a commercially available RE-ion-doped silica fiber.RE ions doped in the silica fiber can be optically activated at room temperature.Therefore, our single-photon source does not need cryogenic systems.In addition, the emission wavelength can be selected based on the type of RE ions doped in the fiber.These features of our single-photon source enable the development of a low-cost and wavelength-selectable source.We performed the autocorrelation measurements using a neodymium (Nd 3+ ) ion in the tapered fiber, and showed the generation of single photons from the ion.In addition, we proposed a method to selectively excite a single RE ion in the tapered fiber, which can directly generate single photons within the tapered fiber, and collect them through the tapered fiber with high collection and channeling efficiencies.Generating single photons with this excitation method is proved by the autocorrelation measurements.We also observed the optical properties of the single photon emitted from the single Nd 3+ ion in the tapered fiber, such as the fluorescence lifetime, saturation intensity and polarization states.The fluorescence lifetime is one of the most important parameters for a single-photon source because this parameter is closely related to the emission rate.We observed the fluorescence lifetime of the single Nd 3+ ion in the tapered silica fiber and an 1 ensemble of the Nd 3+ ion in the unstructured silica fiber.The saturation power of the excitation laser and the saturated fluorescence intensity tell us the appropriate excitation power for generating single photons with high signal-to-noise ratio.Here, we measured the relationship between the fluorescence intensity from the single Nd 3+ ion and the power of the excitation light.In addition, the polarization state of the single photons emitted from the single Nd 3+ ion in the tapered fiber was observed.Our results will lead to the implementation of the low-cost and wavelength-selectable single-photon source to realize various optical quantum information technologies.

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Crystals and fibers doped with Rare Earth (RE) ions provide the basis to most of today's solid-state optical systems, from lasers and telecom devices to emerging potential quantum applications such as quantum memories and optical to microwave conversion. The two platforms, doped crystals and doped fibers, seem mutually exclusive, each having its own strengths and limitations- the former providing high homogeneity and coherence, and the latter offering the advantages of robust optical waveguides. Here we present a hybrid platform that does not rely on doping but rather on coating the waveguide - a tapered silica optical fiber - with a monolayer of complexes, each containing a single RE ion. The complexes offer an identical, tailored environment to each ion, thus minimizing inhomogeneity and allowing tuning of their properties to the desired application. Specifically, we use highly luminescent Yb+3^{+3}+3[Zn(II)MC_{MC}MC​(QXA)] complexes, which isolate the RE ion from the environment and suppress non-radiative decay channels. We demonstrate that the beneficial optical transitions of the Yb+3^{+3}+3 are retained after deposition on the tapered fiber, and observe an excited-state lifetime of over 0.9 ms, on par with state-of-the-art Yb doped inorganic crystals.
High Resolution Image Download MS PowerPoint Slide Crystals and fibers doped with rare-earth (RE) ions provide the basis for most of today’s solid-state optical systems, from lasers and telecom devices to emerging potential quantum applications such as quantum memories and optical to microwave conversion. The two platforms, doped crystals and doped fibers, seem mutually exclusive, each having its own strengths and limitations, the former providing high homogeneity and coherence and the latter offering the advantages of robust optical waveguides. Here we present a hybrid platform that does not rely on doping but rather on coating the waveguide─a tapered silica optical fiber─with a monolayer of complexes, each containing a single RE ion. The complexes offer an identical, tailored environment to each ion, thus minimizing inhomogeneity and allowing tuning of their properties to the desired application. Specifically, we use highly luminescent Yb 3+ [Zn(II) MC (QXA)] complexes, which isolate the RE ion from the environment and suppress nonradiative decay channels. We demonstrate that the beneficial optical transitions of the Yb 3+ are retained after deposition on the tapered fiber and observe an excited-state lifetime of over 0.9 ms, on par with state-of-the-art Yb-doped inorganic crystals.
In this thesis, we study the single-photon source using a rare-earth (RE) ion doped in a tapered fiber.Single-photon sources are key components for various optical quantum information technologies, and the development of low-cost single-photon sources has been desired for their implementation.A wide variety of emitters for single-photon sources have been studied.Among these emitters, RE ions have attracted much attention as single-photon emitters due to their high stability of luminescence and the sharpness of the emission spectrum with 4f transitions.In our single-photon source, we obtain spatially isolated single RE ions, which are separated from each other beyond the diffraction limit by tapering a commercially available RE-ion-doped silica fiber.RE ions doped in the silica fiber can be optically activated at room temperature.Therefore, our single-photon source does not need cryogenic systems.In addition, the emission wavelength can be selected based on the type of RE ions doped in the fiber.These features of our single-photon source enable the development of a low-cost and wavelength-selectable source.We performed the autocorrelation measurements using a neodymium (Nd 3+ ) ion in the tapered fiber, and showed the generation of single photons from the ion.In addition, we proposed a method to selectively excite a single RE ion in the tapered fiber, which can directly generate single photons within the tapered fiber, and collect them through the tapered fiber with high collection and channeling efficiencies.Generating single photons with this excitation method is proved by the autocorrelation measurements.We also observed the optical properties of the single photon emitted from the single Nd 3+ ion in the tapered fiber, such as the fluorescence lifetime, saturation intensity and polarization states.The fluorescence lifetime is one of the most important parameters for a single-photon source because this parameter is closely related to the emission rate.We observed the fluorescence lifetime of the single Nd 3+ ion in the tapered silica fiber and an 1 ensemble of the Nd 3+ ion in the unstructured silica fiber.The saturation power of the excitation laser and the saturated fluorescence intensity tell us the appropriate excitation power for generating single photons with high signal-to-noise ratio.Here, we measured the relationship between the fluorescence intensity from the single Nd 3+ ion and the power of the excitation light.In addition, the polarization state of the single photons emitted from the single Nd 3+ ion in the tapered fiber was observed.Our results will lead to the implementation of the low-cost and wavelength-selectable single-photon source to realize various optical quantum information technologies.
Without using any trapping lasers, rare-earth (RE) ions can be doped into some nanofabricated materials in form of nanocrystals in a solid state matrix, thus rendering a natural trap for potential application as a quantum computing device. In particular, passive nuclear spin states of RE ions can be utilized as (i) optical quantum memory (with huge density as yielded from nanocrystals), (ii) qubits by encoding in ground hyperfine states and operated as (iii) two-qubit gate when transferring them to active magnetized electronic states. A feasible implementation of qubits is realised by using those doped RE ions whose open-shell (for inner highly shielded 4f4 f4f shell electrons) energy levels and statevectors are well described by the crystal field (CF) interaction and hyperfine coupling in which the Hamiltonian is composed of various freeion interactions, the CF potential, electronic and nuclear Zeeman effects as well as the hyperfine interaction. For those qubit encoded in the two ground hyperfine states of RE ions, they can have fairly long lifetimes of days and coherence times (from 1.3s for Er3+\mathrm{Er}^{3+}Er3+ to 6 hours for Eu3+\mathrm{Eu}^{3+}Eu3+) due to the unique spectroscopic properties of RE ions. Because of the recent progress in optical single-ion detection for addressing individual qubits with a specific frequency channel, RE ions could be packed in a solid state 3D matrix at nanometer spacing, hence rendering very high qubit densities for quantum memories. Meanwhile, this configure also leads to strong dipole-dipole interactions (or high connectivity) between qubits which are not nearest neighbors. In this study, Kramers ions like 167Er{ }^{167} \mathbf{E r}167Er and 171Yb{ }^{171} \mathbf{Y b}171Yb doped in yttrium orthosilicate Y2SiO5{Y}_{2} {SiO}_{5}Y2​SiO5​ (YSO) nanocrystals will be investigated as a promising system for quantum computing because of their weak spin bath and possibility for being directly milled in single nanocrystals as nano-resonators. By using the famous Wien2k package to carry out the first-principles calculations, we can obtain the CF parameters and hyperfine constants as well as various electronic properties like energy gap and band structure for those Kramers RE ions doped in YSO. We shall present some essential findings from first-principles calculations to obtain various properties of the ground and excited CF and hyperfine states for those RE ions with an aim to optimize RE ions doping in YSO nanocrystals for quantum memories and qubits, contributing to scalable quantum computing architectures.
Rare-Earth (RE) atoms possess a unique atomic energy level structure, leading to excellent electronic and spin coherence properties [1]. Consequently, RE-ion-doped materials are promising candidates for implementing light-matter interfaces for photonic quantum technologies, such as quantum memories. To exploit these properties in quantum technologies, the REs must be hosted in a solid-state material [1]. RE organic molecular crystals offer advantages over the well-known RE-doped inorganic crystals. In organic molecular crystals, RE ions are integral parts of the molecular structure, unlike in inorganic crystals, in which the RE ions are distributed randomly into the crystal lattice structure. This can potentially lead to narrower inhomogeneous broadening. These crystals provide unmatched flexibility in combining with photonic structures and in material composition, allowing the choice of different ligands and point group symmetries around the RE ion [2], [10], [4]. Our research focuses on crystals formed from a molecular complex hosting erbium ions⌈Er(C5H7O2)3(C12H8N2)⌉\lceil{E}r(C_{5}H_{7}O_{2})_{3}(C_{12}H_{8}N_{2})\rceil⌈Er(C5​H7​O2​)3​(C12​H8​N2​)⌉. As these crystals have not yet been studied for quantum information purposes, we conducted a series of optical spectroscopy measurements to characterize the platform. We performed absorption measurements and obtained the absorption profiles at room and cryogenic temperatures. The results show a narrow inhomogeneous broadening in samples with different relative concentrations, even at 100%, for which all molecules contain an erbium ion. We measured the lifetime of the second lowest crystal field level of the ground state manifold(30 cm−1(\boldsymbol{30}\ cm^{-1}(30 cm−1above ground state) to be 1.759 seconds. Additionally, we measured the inhomogeneous broadening of the lowest crystal field level versus temperature to investigate the effects of phonon processes. Finally, under an external magnetic field, we observed Zeeman splitting and determined the g-factor to be 3.23 for erbium ions in this molecular complex.
A fiber-coupled single-photon source is an essential component for the implementation of optical quantum communication technologies. Using the rare-earth ion doped in an optical fiber as an emitter is a significant method to construct such a photon source at room temperature, as well as achieving high coupling and channeling efficiency. In this study, we experimentally demonstrated the generation of single photons at room temperature by selectively exciting a sole rare-earth ion isolated within a tapered silica fiber. The key advantages of our method are the ability to manipulate a purely single ion and the efficient collection of photons from the guided mode of the fiber, owing to the single ion's emission of photons directly within the fiber. These features make our system a promising building block for realizing all-fiber-integrated optical quantum networks. We have also measured the optical lifetime of a single neodymium ion in the tapered fiber, and the result supports that the single-photon correlation time is practically determined by the absorption time of the ion.
Quantum networks are a rapidly developing field of quantum information processing that have the potential to enable long-range entanglement between future quantum computers as well as the implementation of secure communication through quantum key distribution. Two key components of such networks are quantum memories to store entangled photon pairs for use in the quantum repeater protocol and quantum light-matter interfaces to efficiently interconvert between stationary qubits and flying qubits in the form of photons. Rare-earth ion-doped crystals are a promising solid-state platform that show promise for both of these applications due to their long optical and spin coherence times. Due to their relatively weak optical transitions, rare-earth ions have been coupled with nanophotonic resonators to enhance their transition strengths, with past work in the Faraon group utilizing focused ion beam milled photonic crystal resonators with 45-degree angled couplers to couple light in and out. Such resonators have the disadvantage of requiring manual alignment to fabricate, and the couplers are also relatively inefficient which limits the performance of such devices. It is therefore desirable to move towards silicon photonics, where mature techniques such as electron-beam lithography can allow for scalable fabrication of nanophotonic cavities together with high coupling efficiencies. In this thesis, we demonstrate significant progress towards the usage of acid-etched tapered optical fibers as an efficient interface for coupling light into tapered silicon nanophotonic waveguides. We show comprehensive simulations of the taper geometries required to achieve adiabatic coupling with theoretical efficiencies of more than 99%, and design a silicon photonic crystal mirror to be used in the measurement of the fiber-waveguide coupling efficiency. We then optimize the hydrofluoric acid fiber etching process and demonstrate the ability to make tapered fibers which are 200 microns long with a taper half-angle of 2 degrees and a tip diameter of 50 nm. Using these tapered fibers to couple light into tapered silicon waveguides fabricated using electron-beam lithography shows a moderately high coupling efficiency of 11.4% with the potential for improvement. This method of tapered fiber coupling shows promise to be integrated into silicon nanophotonic resonators on rare-earth ion doped crystals and allow for highly efficient quantum memories and quantum light-matter interfaces in the solid-state.