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Philippe Goldner

Publications and source records attributed to Philippe Goldner.

At least 37 records · Page 2Linked to original sources

Rare-earth doped yttrium silicate (Y2SiO5) thin films grown by chemical vapour deposition for quantum technologies

Yttrium orthosilicate (Y2SiO5 - YSO) is one of the most promising crystals to host rare-earth (RE) ions for quantum technologies applications. In this matrix, they indeed exhibit narrow optical and spin linewidths that can be exploited to develop quantum memories or quantum information processing capabilities. In this paper, we propose a new method to grow RE doped silicate thin films on silicon wafers based on direct liquid injection chemical vapour deposition (DLI-CVD). We optimize the deposition and annealing conditions to achieve formation of the high temperature X2-YSO phase. The phase purity and crystalline quality of the films are assessed by evaluating the optical properties of Eu3+ ions embedded in this oxide matrix. In view of the results, we discuss the possible phase formation mechanisms, and the potential of this new wafer-compatible form of YSO for quantum technologies applications.

physics.optics↗

Optical coherence and spin population dynamics in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$ single crystals

$^{171}$Yb$^{3+}$-doped Y$_2$SiO$_5$ crystals are a promising platform for optical quantum memories in long-distance quantum communications. The relevance of this material lies in $^{171}$Yb long optical and spin coherence times, along with a large hyperfine splitting, enabling long quantum storage over large bandwidths. Mechanisms affecting the optical decoherence are however not precisely known, especially since low-temperature measurements have so far focused on the 2 to 4 K range. In this work, we performed two- and three-pulse photon echoes and spectral hole burning to determine optical homogeneous linewidths in two 171 Yb:YSO crystals doped at 2 and 10 ppm. Experiments were performed in the 40 mK to 18 K temperature range, leading to linewidths between 320 Hz, among the narrowest reported for rare-earth ions, and several MHz. Our results show that above 6 K the homogeneous linewidth is mainly due to an elastic two-phonon process which results in a slow broadening with temperature, the homogeneous linewidth reaching only 25 kHz at 10 K. At lower temperatures, interactions with $^{89}$Yb nuclear spin-flips, paramagnetic defects or impurities, and also Yb-Yb interactions for the higher concentrated crystal, are likely the main limiting factor to the homogeneous linewidth. In particular, we conclude that the direct effect of spin and optical excited state lifetime is a minor contribution to optical decoherence in the whole temperature range studied. Our results indicate possible paths and regimes for further decreasing the homogeneous linewidths or maintaining narrow lines at higher $^{171}$Yb concentration.

quant-ph↗

Single electron-spin-resonance detection by microwave photon counting

Electron spin resonance (ESR) spectroscopy is the method of choice for characterizing paramagnetic impurities, with applications ranging from chemistry to quantum computing, but it gives access only to ensemble-averaged quantities due to its limited signal-to-noise ratio. Single-electron-spin sensitivity has however been reached using spin-dependent photoluminescence, transport measurements, and scanning-probe techniques. These methods are system-specific or sensitive only in a small detection volume, so that practical single spin detection remains an open challenge. Here, we demonstrate single electron magnetic resonance by spin fluorescence detection, using a microwave photon counter at cryogenic temperatures. We detect individual paramagnetic erbium ions in a scheelite crystal coupled to a high-quality factor planar superconducting resonator to enhance their radiative decay rate, with a signal-to-noise ratio of 1.9 in one second integration time. The fluorescence signal shows anti-bunching, proving that it comes from individual emitters. Coherence times up to 3 ms are measured, limited by the spin radiative lifetime. The method has the potential to apply to arbitrary paramagnetic species with long enough non-radiative relaxation time, and allows single-spin detection in a volume as large as the resonator magnetic mode volume ( 10 um^3 in the present experiment), orders of magnitude larger than other single-spin detection techniques. As such, it may find applications in magnetic resonance and quantum computing.

quant-ph↗

Hot ion implantation to create dense NV centre ensembles in diamond

Creating dense and shallow nitrogen vacancy (NV) ensembles with good spin properties, is a prerequisite for developing diamond-based quantum sensors exhibiting better performance. Ion implantation is a key enabling tool for precisely controlling spatial localisation and density of NV colour centres in diamond. However, it suffers from a low creation yield, while higher ion fluences significantly damage the crystal lattice. In this work, we realize N2 ion implantation in the 30 to 40 keV range at high temperatures. At 800 C, NV ensemble photoluminescence emission is three to four times higher than room temperature implanted films, while narrow electron spin resonance linewidths of 1.5 MHz, comparable to well established implantation techniques are obtained. In addition, we found that ion fluences above 2E14 ions per cm2 can be used without graphitization of the diamond film, in contrast to room temperature implantation. This study opens promising perspectives in optimizing diamond films with implanted NV ensembles that could be integrated into quantum sensing devices.

physics.app-ph↗

Optical coherence properties of Kramers' rare-earth ions at the nanoscale for quantum applications

Rare-earth (RE) ion doped nano-materials are promising candidates for a range of quantum technology applications. Among RE ions, the so-called Kramers' ions possess spin transitions in the GHz range at low magnetic fields, which allows for high-bandwidth multimode quantum storage, fast qubit operations as well as interfacing with superconducting circuits. They also present relevant optical transitions in the infrared. In particular, Er$^{3+}$ has an optical transition in the telecom band, while Nd$^{3+}$ presents a high-emission-rate transition close to 890 nm. In this paper, we measure spectroscopic properties that are of relevance to using these materials in quantum technology applications. We find the inhomogeneous linewidth to be 10.7 GHz for Er$^{3+}$ and 8.2 GHz for Nd$^{3+}$, and the excited state lifetime T$_1$ to be 13.68 ms for Er$^{3+}$ and 540 $μ$s for Nd$^{3+}$. We study the dependence of homogeneous linewidth on temperature for both samples, with the narrowest linewidth being 379 kHz (T$_2$ = 839 ns) for Er$^{3+}$ measured at 3 K, and 62 kHz (T$_2$ = 5.14 $μ$s) for Nd$^{3+}$ measured at 1.6 K. Further, we investigate time-dependent homogeneous linewidth broadening due to spectral diffusion and the dependence of homogeneous linewidth on magnetic field, in order to get additional clarity of mechanisms that can influence the coherence time. In light of our results, we discuss two applications: single qubit-state readout and a Fourier-limited single photon source.

quant-ph↗

Detection of single ions in a nanoparticle coupled to a fiber cavity

Many quantum information protocols require the storage and manipulation of information over long times, and its exchange between nodes of a quantum network across long distances. Implementing these protocols requires an advanced quantum hardware, featuring, for example, a register of long-lived and interacting qubits with an efficient optical interface in the telecommunication band. Here we present the Purcell-enhanced detection of single solid-state ions in erbium-doped nanoparticles placed in a fiber cavity, emitting photons at 1536 nm. The open-access design of the cavity allows for complete tunability both in space and frequency, selecting individual particles and ions. The ions are confined in a volume two orders of magnitude smaller than in previous realizations, increasing the probability of finding ions separated only by a few nanometers which could then interact. We report the detection of individual spectral features presenting saturation of the emission count rate and linewidth, as expected for two-level systems. We also report an uncorrected $g^{(2)} \left ( 0 \right )$ of 0.24(5) for the emitted field, confirming the presence of a single emitter. Our fully fiber-integrated system is an important step towards the realization of the initially envisioned quantum hardware.

quant-ph↗

Coherent optical-microwave interface for manipulation of low-field electronic clock transitions in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$

The coherent interaction of solid-state spins with both optical and microwave fields provides a platform for a range of quantum technologies, such as quantum sensing, microwave-to-optical quantum transduction and optical quantum memories. Rare-earth ions with electronic spins are interesting in this context, but it is challenging to simultaneously and efficiently drive both optical and microwave transitions over a long crystal. In this work, we use a loop-gap microwave resonator to coherently drive optical and microwave clock transitions in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$, at close to zero external magnetic field. The low magnetic field regime is particularly interesting for interfacing these spin transitions with superconducting circuits. We achieve a Rabi frequency of 0.56 MHz at 2.497 GHz, over a 1-cm long crystal. Furthermore, we provide new insights into the spin dephasing mechanism at very low fields, showing that superhyperfine-induced collapse of the Hahn echo signal plays an important role at low fields. Our calculations and measurements reveal that the effective magnetic moment can be manipulated in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$, allowing to suppress the superhyperfine interaction at the clock transition. At a doping concentration of 2 ppm and a temperature of $3.4$ K, we achieve the longest spin coherence time of $10.0 \pm 0.4 ~\text{ms}$ reported in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$.

quant-ph↗

Microwave fluorescence detection of spin echoes

Counting the microwave photons emitted by an ensemble of electron spins when they relax radiatively has recently been proposed as a sensitive method for electron paramagnetic resonance (EPR) spectroscopy, enabled by the development of operational Single Microwave Photon Detectors (SMPD) at millikelvin temperature. Here, we report the detection of spin echoes in the spin fluorescence signal. The echo manifests itself as a coherent modulation of the number of photons spontaneously emitted after a $π/2_X - τ- π_Y - τ- π/2_Φ$ sequence, dependent on the relative phase $Φ$. We demonstrate experimentally this detection method using an ensemble of $\mathrm{Er}^{3+}$ ion spins in a scheelite crystal of $\mathrm{CaWO}_4$. We use fluorescence-detected echoes to measure the erbium spin coherence time, as well as the echo envelope modulation due to the coupling to the $^{183}\mathrm{W}$ nuclear spins surrounding each ion. We finally compare the signal-to-noise ratio of inductively-detected and fluorescence-detected echoes, and show that it is larger with the fluorescence method.

quant-ph↗

Coherent spin dynamics of rare-earth doped crystals in the high-cooperativity regime

Rare-earth doped crystals have long coherence times and the potential to provide quantum interfaces between microwave and optical photons. Such applications benefit from a high cooperativity between the spin ensemble and a microwave cavity -- this motivates an increase in the rare earth ion concentration which in turn impacts the spin coherence lifetime. We measure spin dynamics of two rare-earth spin species, $^{145}$Nd and Yb doped into Y$_{2}$SiO$_{5}$, coupled to a planar microwave resonator in the high cooperativity regime, in the temperature range 1.2 K to 14 mK. We identify relevant decoherence mechanisms including instantaneous diffusion arising from resonant spins and temperature-dependent spectral diffusion from impurity electron and nuclear spins in the environment. We explore two methods to mitigate the effects of spectral diffusion in the Yb system in the low-temperature limit, first, using magnetic fields of up to 1 T to suppress impurity spin dynamics and, second, using transitions with low effective g-factors to reduce sensitivity to such dynamics. Finally, we demonstrate how the `clock transition' present in the $^{171}$Yb system at zero field can be used to increase coherence times up to $T_{2} = 6(1)$ ms.

quant-ph↗

Remote distribution of non-classical correlations over 1250 modes between a telecom photon and a $^{171}$Yb$^{3+}$:Y$_2$SiO$_{5}$ crystal

Quantum repeaters based on heralded entanglement require quantum nodes that are able to generate multimode quantum correlations between memories and telecommunication photons. The communication rate scales linearly with the number of modes, yet highly multimode quantum storage remains challenging. In this work, we demonstrate an atomic frequency comb quantum memory with a time-domain mode capacity of 1250 modes and a bandwidth of 100 MHz, to our knowledge the largest number of modes stored in the quantum regime. The memory is based on a $Y_{2}SiO_{5}$ crystal doped with $^{171}Yb^{3+}$ ions, with a memory wavelength of 979 nm. The memory is interfaced with a source of non-degenerate photon pairs at 979 and 1550 nm, bandwidth-matched to the quantum memory. We obtain strong non-classical second-order cross correlations over all modes, for storage times of up to $25$ $μs$. The telecommunication photons propagated through 5 km of fiber before the release of the memory photons, a key capability for quantum repeaters based on heralded entanglement and feed-forward operations. Building on this experiment should allow distribution of entanglement between remote quantum nodes, with enhanced rates owing to the high multimode capacity.

quant-ph↗

Electron-spin spectral diffusion in an erbium doped crystal at millikelvin temperatures

Erbium-doped crystals offer a versatile platform for hybrid quantum devices because they combine magnetically-sensitive electron-spin transitions with telecom-wavelength optical transitions. At the high doping concentrations necessary for many quantum applications, however, strong magnetic interactions of the electron-spin bath lead to excess spectral diffusion and rapid decoherence. Here we lithographically fabricate a 4.4 GHz superconducting planar micro-resonator on a $\text{CaWO}_{4}$ crystal doped with Er ions at a concentration of twenty parts per million relative to Ca. Using the microwave resonator, we characterize the spectral diffusion processes that limit the electron-spin coherence of Er ions at millikelvin temperatures by applying 2- and 3-pulse echo sequences. The coherence time shows a strong temperature dependence, reaching 1.3 ms at 23 mK for an electron-spin transition of $^{167}\text{Er}$.

quant-ph↗

2022 Roadmap for Materials for Quantum Technologies

Quantum technologies are poised to move the foundational principles of quantum physics to the forefront of applications. This roadmap identifies some of the key challenges and provides insights on materials innovations underlying a range of exciting quantum technology frontiers. Over the past decades, hardware platforms enabling different quantum technologies have reached varying levels of maturity. This has allowed for first proof-of-principle demonstrations of quantum supremacy, for example quantum computers surpassing their classical counterparts, quantum communication with reliable security guaranteed by laws of quantum mechanics, and quantum sensors uniting the advantages of high sensitivity, high spatial resolution, and small footprints. In all cases, however, advancing these technologies to the next level of applications in relevant environments requires further development and innovations in the underlying materials. From a wealth of hardware platforms, we select representative and promising material systems in currently investigated quantum technologies. These include both the inherent quantum bit systems as well as materials playing supportive or enabling roles, and cover trapped ions, neutral atom arrays, rare earth ion systems, donors in silicon, color centers and defects in wide-band gap materials, two-dimensional materials and superconducting materials for single-photon detectors. Advancing these materials frontiers will require innovations from a diverse community of scientific expertise, and hence this roadmap will be of interest to a broad spectrum of disciplines.

quant-ph↗

Erbium-Implanted Materials for Quantum Communication Applications

Erbium-doped materials can serve as spin-photon interfaces with optical transitions in the telecom C-band, making them an exciting class of materials for long-distance quantum communication. However, the spin and optical coherence times of Er3+ ions are limited by currently available host materials, motivating the development of new Er3+-containing materials. Here, we demonstrate the use of ion implantation to efficiently screen prospective host candidates, and show that disorder introduced by ion implantation can be mitigated through post-implantation thermal processing to achieve inhomogeneous linewidths comparable to bulk linewidths in as-grown samples. We present optical spectroscopy data for each host material, which allows us to determine the level structure of each site, allowing us to compare the environments of Er3+ introduced via implantation and via doping during growth. We demonstrate that implantation can generate a range of local environments for Er3+, including those observed in bulk-doped materials, and that the populations of these sites can be controlled with thermal processing.

cond-mat.mtrl-sci↗

Twenty-three millisecond electron spin coherence of erbium ions in a natural-abundance crystal

Erbium ions doped into crystals have unique properties for quantum information processing, because of their optical transition at 1.5 $μ$m and of the large magnetic moment of their effective spin-1/2 electronic ground state. Most applications of erbium require however long electron spin coherence times, and this has so far been missing. Here, by selecting a host matrix with a low nuclear-spin density (CaWO$_4$) and by quenching the spectral diffusion due to residual paramagnetic impurities at millikelvin temperatures, we obtain an Er$^{3+}$ electron spin coherence time of 23 ms. This is the longest electron spin coherence time measured in a material with a natural abundance of nuclear spins and on a magnetically-sensitive transition. Our results establish Er$^{3+}$:CaWO$_4$ as a leading platform for quantum networks.

quant-ph↗

Rare-Earth Molecular Crystals with Ultra-narrow Optical Linewidths for Photonic Quantum Technologies

Rare-earth ions are promising solid state systems to build light-matter interfaces at the quantum level. This relies on their potential to show narrow optical homogeneous linewidths or, equivalently, long-lived optical quantum states. In this letter, we report on europium molecular crystals that exhibit linewidths in the 10s of kHz range, orders of magnitude narrower than other molecular centers. We harness this property to demonstrate efficient optical spin initialization, coherent storage of light using an atomic frequency comb, and optical control of ion-ion interactions towards implementation of quantum gates. These results illustrate the utility of rare-earth molecular crystals as a new platform for photonic quantum technologies that combines highly coherent emitters with the unmatched versatility in composition, structure, and integration capability of molecular materials.

physics.optics↗

Roadmap for Rare-earth Quantum Computing

Several platforms are being considered as hardware for quantum technologies. For quantum computing (QC), superconducting qubits and artificially trapped ions are among the leading platforms, but many others also show promise, e.g. photons, cold atoms, defect centers including Rare-Earth (RE) ions. So far, results are limited to the regime of noisy intermediate scale qubits (NISQ), with a small number of qubits and a limited connectivity, and it is likely that future QC hardware will utilize several existing platforms in different ways. Thus, it currently makes sense to invest resources broadly and explore the full range of promising routes to quantum technology. Rare-earth ions in solids constitute one of the most versatile platforms for future quantum technology. One advantage is good coherence properties even when confined in strong natural traps inside a solid-state matrix. This confinement allows very high qubit densities and correspondingly strong ion-ion couplings. In addition, although their fluorescence is generally weak, cavity integration can enhance the emission greatly and enable very good connections to photonic circuits, including at the telecom wavelengths, making them promising systems for long-term scalability. The primary aim of this roadmap is to provide a complete picture of what components a RE quantum computer would consist of, to describe the details of all parts required to achieve a scalable system, and to discuss the most promising paths to reach it. In brief, we find that clusters of 50-100 single RE ions can act as high fidelity qubits in small processors, occupying only about (10 nm)^3. Due to the high capacity for integration of the RE systems, they be optically read out and connected to other such clusters for larger scalability. We make suggestions for future improvements, which could allow the REQC platform to be a leading one.

quant-ph↗

Electron-Nuclear Interactions as a Test of Crystal-Field Parameters for Low Symmetry Systems: Zeeman-Hyperfine Spectroscopy of Ho$^{3+}$ Doped Y$_2$SiO$_5$

High-resolution Zeeman spectroscopy of electronic-nuclear hyperfine levels of ${^5\mathrm{I}_8}\rightarrow{^5\mathrm{I}_7}$ transitions in Ho$^{3+}$:Y$_2$SiO$_5$ is reported. Crystal-field parameters determined for the two $C_1$ symmetry sites in Er$^{3+}$:Y$_2$SiO$_5$ are successfully used to model the Zeeman-hyperfine data, including the prediction of avoided crossings between hyperfine levels under the influence of an external magnetic field. The two six- and seven-coordinate substitutional sites may be distinguished by comparing the spectra with crystal-field calculations.

cond-mat.mtrl-sci↗

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 >1,000-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 emitters 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.

cond-mat.mes-hall↗