Dynamic control of Purcell enhanced emission of erbium ions in nanoparticles.

The interaction of single quantum emitters with an optical cavity enables the realization of efficient spin-photon interfaces, an essential resource for quantum networks. The dynamical control of the spontaneous emission rate of quantum emitters in cavities has important implications in quantum technologies, e.g., for shaping the emitted photons' waveform or for driving coherently the optical transition while preventing photon emission. Here we demonstrate the dynamical control of the Purcell enhanced emission of a small ensemble of erbium ions doped into a nanoparticle. By embedding the nanoparticles into a fully tunable high finesse fiber based optical microcavity, we demonstrate a median Purcell factor of 15 for the ensemble of ions. We also show that we can dynamically control the Purcell enhanced emission by tuning the cavity on and out of resonance, by controlling its length with sub-nanometer precision on a time scale more than two orders of magnitude faster than the natural lifetime of the erbium ions. This capability opens prospects for the realization of efficient nanoscale quantum interfaces between solid-state spins and single telecom photons with controllable waveform, for non-destructive detection of photonic qubits, and for the realization of quantum gates between rare-earth ion qubits coupled to an optical cavity.

Fast electrical modulation of strong near-field interactions between erbium emitters and graphene.

Combining the quantum optical properties of single-photon emitters with the strong near-field interactions available in nanophotonic and plasmonic systems is a powerful way of creating quantum manipulation and metrological functionalities. The ability to actively and dynamically modulate emitter-environment interactions is of particular interest in this regard. While thermal, mechanical and optical modulation have been demonstrated, electrical modulation has remained an outstanding challenge. Here we realize fast, all-electrical modulation of the near-field interactions between a nanolayer of erbium emitters and graphene, by in-situ tuning the Fermi energy of graphene. We demonstrate strong interactions with a  >1000-fold increased decay rate for  ~25% of the emitters, and electrically modulate these interactions with frequencies up to 300 kHz - orders of magnitude faster than the emitter's radiative decay (~100 Hz). This constitutes an enabling platform for integrated quantum technologies, opening routes to quantum entanglement generation by collective plasmon emission or photon emission with controlled waveform.

A Frequency-Multiplexed Coherent Electro-optic Memory in Rare Earth Doped Nanoparticles.

Quantum memories for light are essential components in quantum technologies like long-distance quantum communication and distributed quantum computing. Recent studies have shown that long optical and spin coherence lifetimes can be observed in rare earth doped nanoparticles, opening exciting possibilities over bulk materials, e.g., for enhancing coupling to light and other quantum systems, and material design. Here, we report on coherent light storage in Eu3+:Y2O3 nanoparticles using the Stark echo modulation memory (SEMM) quantum protocol. We first measure a nearly constant Stark coefficient of 50 kHz/(V/cm) across a bandwidth of 15 GHz, which is promising for broadband operation. Storage of light is then demonstrated with an effective coherence lifetime of 5 µs. Pulses with two different frequencies are also stored, confirming frequency-multiplexing capability, and are used to demonstrate the memory high phase fidelity. These results open the way to nanoscale optical quantum memories with increased efficiency, bandwidth, and processing capabilities.

Defect Engineering for Quantum Grade Rare-Earth Nanocrystals.

Nanostructured systems that combine optical and spin transitions offer new functionalities for quantum technologies by providing efficient quantum light-matter interfaces. Rare-earth (RE) ion-doped nanoparticles are promising in this field as they show long-lived optical and spin quantum states. However, further development of their use in highly demanding applications, such as scalable single-ion-based quantum processors, requires controlling defects that currently limit coherence lifetimes. In this work, we show that a post-treatment process that includes multistep high-temperature annealing followed by high-power microwave oxygen plasma processing advantageously improves key properties for quantum technologies. We obtain single crystalline Eu3+:Y2O3 nanoparticles (NPs) of 100 nm diameter, presenting bulk-like inhomogeneous line widths (Γinh) and population lifetimes (T1). Furthermore, a significant coherence lifetime (T2) extension, up to a factor of 5, is successfully achieved by modifying the oxygen-related point defects in the NPs by the oxygen plasma treatment. These promising results confirm the potential of engineered RE NPs to integrate devices such as cavity-based single-photon sources, quantum memories, and processors. In addition, our strategy could be applied to a large variety of oxides to obtain outstanding crystalline quality NPs for a broad range of applications.

Time-gated triplet-state optical spectroscopy to decipher organic luminophores embedded in rigid matrices.

Wet-chemically synthesized inorganic materials often exhibit luminescence behavior. We have recently shown that the amorphous yttrium-aluminium-borate (a-YAB) powders obtained by sol-gel and modified Pechini methods exhibit organic impurities, responsible for their intense visible photoluminescence and phosphorescence afterglow. However, the heterogeneity of impurity organic compounds and difficulties in their intact extraction from the solid inorganic host matrix limit the extraction-based chemical analysis for luminophore identification. Here, we propose a photo-physical route based on time-gated triplet-state optical spectroscopy (TGTSS) to construct the electronic structures of the trapped unknown luminophores, which successfully illustrates the luminescence properties of a-YAB powders in more detail and also provides important insights intrinsic to the nature of the luminophores. The experimental results accompanied with TD-DFT calculations of the theoretical electronic structures thus help us to propose the probable luminophore compounds trapped in rigid a-YAB matrices. We anticipate that the present approach will open new opportunities for analyzing similar complex luminescent materials, including carbon dots, graphene oxides, etc., which is vital for their improvement.

Simultaneous coherence enhancement of optical and microwave transitions in solid-state electronic spins.

Solid-state electronic spins are extensively studied in quantum information science, as their large magnetic moments offer fast operations for computing1 and communication2-4, and high sensitivity for sensing5. However, electronic spins are more sensitive to magnetic noise, but engineering of their spectroscopic properties, for example, using clock transitions and isotopic engineering, can yield remarkable spin coherence times, as for electronic spins in GaAs6, donors in silicon7-11 and vacancy centres in diamond12,13. Here we demonstrate simultaneously induced clock transitions for both microwave and optical domains in an isotopically purified 171Yb3+:Y2SiO5 crystal, reaching coherence times of greater than 100 µs and 1 ms in the optical and microwave domains, respectively. This effect is due to the highly anisotropic hyperfine interaction, which makes each electronic-nuclear state an entangled Bell state. Our results underline the potential of 171Yb3+:Y2SiO5 for quantum processing applications relying on both optical and spin manipulation, such as optical quantum memories4,14, microwave-to-optical quantum transducers15,16, and single-spin detection17, while they should also be observable in a range of different materials with anisotropic hyperfine interactions.

Controlled size reduction of rare earth doped nanoparticles for optical quantum technologies.

Rare earth doped nanoparticles with sub-wavelength size can be coupled to optical micro- or nano-cavities to enable efficient single ion readout and control, a key requirement for quantum processors and high-fidelity single-ion quantum memories. However, producing small nanoparticles with good dispersion and exploitable optical coherence properties, another key aspect for these applications, is highly challenging by most synthesis and nano-fabrication methods. We report here on the wet chemical etching of Eu3+:Y2O3 nanoparticles and demonstrate that a controlled size reduction down to 150 nm, well below the wavelength of interest, 580 nm, can be achieved. The etching mechanism is found to proceed by reaction with grain boundaries and isolated grains, based on obtained particles size, morphology and polycrystalline structure. Furthermore, this method allows maintaining long optical coherence lifetimes (T 2): the 12.5 µs and 9.3 µs values obtained for 430 nm initial particles and 150 nm etched particles respectively, revealing a broadening of only 10 kHz after etching. These values are the longest T 2 values reported for any nanoparticles, opening the way to new rare-earth based nanoscale quantum technologies.

Evidence of Organic Luminescent Centers in Sol-Gel-Synthesized Yttrium Aluminum Borate Matrix Leading to Bright Visible Emission.

Yttrium aluminum borate (YAB) powders prepared by sol-gel process have been investigated to understand their photoluminescence (PL) mechanism. The amorphous YAB powders exhibit bright visible PL from blue emission for powders calcined at 450 °C to broad white PL for higher calcination temperature. Thanks to 13 C labelling, NMR and EPR studies show that propionic acid initially used to solubilize the yttrium nitrate is decomposed into aromatic molecules confined within the inorganic matrix. DTA-TG-MS analyses show around 2 wt % of carbogenic species. The PL broadening corresponds to the apparition of a new band at 550 nm, associated with the formation of aromatic species. Furthermore, pulsed ENDOR spectroscopy combined with DFT calculations enables us to ascribe EPR spectra to free radicals derived from small (2 to 3 rings) polycyclic aromatic hydrocarbons (PAH). PAH molecules are thus at the origin of the PL as corroborated by slow afterglow decay and thermoluminescence experiments.

Afterglow Luminescence in Wet-Chemically Synthesized Inorganic Materials: Ultra-Long Room Temperature Phosphorescence Instead of Persistent Luminescence.

Wet-chemically synthesized amorphous yttrium-aluminum-borates (a-YAB) exhibit intense visible photoluminescence (PL). Preliminary investigations revealed a correlation of PL with the presence of carbon-related impurities; however, their exact nature is still under investigation. These powders also exhibit afterglow luminescence that lasts for several seconds at room-temperature (RT). A comparison with persistent phosphors and phosphorescent dye revealed that the afterglow in a-YAB is a phosphorescence phenomenon and not the persistence luminescence, which is more common in inorganic solids. The unusual RT phosphorescence in a-YAB could be achieved due to triplet-state stabilization of trapped luminescent organic moieties in glassy matrix. This is indeed an important step forward in understanding the complex luminescence mechanism in such promising wet-chemically synthesized functional materials. Moreover, phosphorescence is detectable for over 10 s at RT, suggesting rigid glassy inorganic matrix is more efficient in preserving phosphorescence at elevated temperatures, opening the path for several attractive applications including time-resolved bioimaging and thermometry.

Optical Line Width Broadening Mechanisms at the 10 kHz Level in Eu3+:Y2O3 Nanoparticles.

We identify the physical mechanisms responsible for the optical homogeneous broadening in Eu3+:Y2O3 nanoparticles to determine whether rare-earth crystals can be miniaturized to volumes less than λ3 while preserving their appeal for quantum technology hardware. By studying how the homogeneous line width depends on temperature, applied magnetic field, and measurement time scale, the dominant broadening interactions for various temperature ranges above 3 K were characterized. Below 3 K the homogeneous line width is dominated by an interaction not observed in bulk crystal studies. These measurements demonstrate that broadening due to size-dependent phonon interactions is not a significant contributor to the homogeneous line width, which contrasts previous studies in rare-earth ion nanocrystals. Importantly, the results provide strong evidence that for the 400 nm diameter nanoparticles under study the minimum line width achieved (45 ± 1 kHz at 1.3 K) is not fundamentally limited. In addition, we highlight that the expected broadening caused by electric field fluctuations arising from surface charges is comparable to the observed broadening. Under the assumption that such Stark broadening is a significant contribution to the homogeneous line width, several strategies for reducing this line width to below 10 kHz are discussed. Furthermore, it is demonstrated that the Eu3+ hyperfine state lifetime is sufficiently long to preserve spectral features for time scales up to 1 s. These results allow integrated rare-earth ion quantum optics to be pursued at a submicron scale and, hence, open up directions for greater scaling of rare-earth quantum technology.

Coherent Spin Control at the Quantum Level in an Ensemble-Based Optical Memory.

Long-lived quantum memories are essential components of a long-standing goal of remote distribution of entanglement in quantum networks. These can be realized by storing the quantum states of light as single-spin excitations in atomic ensembles. However, spin states are often subjected to different dephasing processes that limit the storage time, which in principle could be overcome using spin-echo techniques. Theoretical studies suggest this to be challenging due to unavoidable spontaneous emission noise in ensemble-based quantum memories. Here, we demonstrate spin-echo manipulation of a mean spin excitation of 1 in a large solid-state ensemble, generated through storage of a weak optical pulse. After a storage time of about 1 ms we optically read-out the spin excitation with a high signal-to-noise ratio. Our results pave the way for long-duration optical quantum storage using spin-echo techniques for any ensemble-based memory.

Coherent storage of microwave excitations in rare-earth nuclear spins.

Interfacing between various elements of a computer--from memory to processors to long range communication--will be as critical for quantum computers as it is for classical computers today. Paramagnetic rare-earth doped crystals, such as Nd(3+):Y2SiO5(YSO), are excellent candidates for such a quantum interface: they are known to exhibit long optical coherence lifetimes (for communication via optical photons), possess a nuclear spin (memory), and have in addition an electron spin that can offer hybrid coupling with superconducting qubits (processing). Here we study two of these three elements, demonstrating coherent storage and retrieval between electron and (145)Nd nuclear spin states in Nd(3+):YSO. We find nuclear spin coherence times can reach 9 ms at ∼5 K, about 2 orders of magnitude longer than the electron spin coherence, while quantum state and process tomography of the storage or retrieval operation between the electron and nuclear spin reveal an average state fidelity of 0.86. The times and fidelities are expected to further improve at lower temperatures and with more homogeneous radio-frequency excitation.

Impact of rare earth element clusters on the excited state lifetime evolution under irradiation in oxide glasses.

Rare earth doped active glasses and fibers can be exposed to ionizing radiations in space and nuclear applications. In this work, we analyze the evolution of (2)F(5/2) excited state lifetime in Yb(3+) ions in irradiated aluminosilicate glasses by electrons and γ rays. It is found that the variation of lifetimes depends on the Yb(3+) clusters content of the glasses for irradiation doses in the 10(2)- 1.5∙10(9) Gy range. In particular, glasses with high clustering show a smaller decrease in lifetime with increasing radiation dose. This behavior is well correlated to the variation in paramagnetic defects concentration determined by electron paramagnetic resonance. This effect is also observed in Yb(3+) doped phosphate and Er(3+) doped aluminosilicate glasses, inferring that clustering plays an important role in irradiation induced quenching.

Faithful solid state optical memory with dynamically decoupled spin wave storage.

We report a high fidelity optical memory in which dynamical decoupling is used to extend the storage time. This is demonstrated in a rare-earth doped crystal in which optical coherences were transferred to nuclear spin coherences and then protected against environmental noise by dynamical decoupling, leading to storage times of up to 4.2 ms. An interference experiment shows that relative phases of input pulses are preserved through the whole storage and retrieval process with a visibility ≈1, demonstrating the usefulness of dynamical decoupling for extending the storage time of quantum memories. We also show that dynamical decoupling sequences insensitive to initial spin coherence increase retrieval efficiency.

Use of NIR light and upconversion phosphors in light-curable polymers.

OBJECTIVE: Light-curable polymers are commonly used in restorative surgery, prosthodontics and surgical procedures. Despite the fact of wide application, there are clinical problems due to limitations of blue light penetration: application is restricted to defects exposed to the light source, layered filling of defect is required. METHODS: Combining photo-activation and up conversion allows efficient polymer hardening by deep penetrating near-infrared (NIR) light. The prerequisite 450 nm blue light to polymerize dental resins could be achieved by filler particles, which absorb the incident NIR irradiation and convert it into visible light. RESULTS: The on spot generated blue light results in uniform polymer hardening. Composite samples of 5mm thickness were cured two times faster than pure polymer cured by blue light (30 and 60 s, respectively). Overall degree of monomer conversion resulted in higher values of more than 40%. The enhanced transmission of NIR light was confirmed by optical analysis of dentin and enamel. The NIR transmittance surge in the 800-1200 nm window could improve sealing of complex and deep caries lesions. SIGNIFICANCE: We demonstrate faster curing and an improved degree of polymerization by using upconversion filler particles as multiple light emission centers. This study represents an alternative approach in curing dental resins by NIR source.