arXiv subjects

Alexandre Tallaire

Publications and source records attributed to Alexandre Tallaire.

17 recordsLinked to original sources

arXiv2026

Oxygen in diamond: thermal stability of ST1 spin centres and creation of oxygen-pair complexes

Little is known about oxygen-related defects in diamond. Recently, the promising room-temperature spin centre named ST1 was identified as an oxygen centre, but of still unknown atomic structure and thermal stability. In this work, we report on the optically active oxygen-related centres and the conditions for their formation, using ion implantation of oxygen in various conditions of depth and fluence. More specifically, we establish the temperature formation/stability range of the ST1 centre, which has a maximum at about 1100{\deg}C and is narrower than for NV centres. In these conditions, optically detected magnetic resonance (ODMR) on small ST1 ensembles was measured with a spin readout contrast of > 20% at 300K. In cathodoluminescence, the 535 nm ST1 peak is not observed. Besides, a broad peak centred at 460 nm is measured for implantation of O$_2$ molecular ions. For an annealing temperature of 1500{\deg}C, a different centre is formed (with ZPL at 584.5 nm) with an intensity increasing with a power law 1.5 < p < 1.9 dependence from the implantation fluence. This suggests that this centre contains two oxygen atoms. Besides, a new spectral feature associated to an intrinsic defect was also observed, with four prominent lines (especially at 594nm). Finally, the thermal formation and stability of oxygen centres in diamond presented here are important for the identification of the atomic structure of defects such as the ST1 and possible O$_2$V$_x$ complex by means of ab initio calculations. Indeed, the formation energies and charge states of defect centres are easier to compute than the full energy level scheme, which to date still remains unsuccessful regarding the ST1 centre.

cond-mat.mtrl-sci↗

arXiv2025

Enhanced magnetic field sensitivity of shallow NV$^-$ ensembles via high-temperature implantation

Dense and shallow ensembles of negatively charged nitrogen-vacancy centers (NV$^-$) with good optical and spin properties play a key role in the performance enhancement of diamond-based quantum sensors. Ion implantation enables precise control of NV$^-$ depth and density. However, at high ion fluence, this method is limited by low NV$^-$ creation yields and sample amorphization. Additionally, shallow NV$^-$ spin properties deteriorate due to surface proximity. In this paper, we study N$_2^+$ ion implantation at energies between 10 and 15 keV with fluences as high as 1e15 ions/cm2 at temperatures of 20, 400 and 800{\deg}C to investigate the influence of implantation temperature on lattice damage, NV$^-$ creation yield and NV$^-$ spin properties. Our results show that diamond maintains structural integrity at 800{\deg}C with fluences up to 1e15 ions/cm2 without amorphization. Furthermore, high-temperature implantation improves NV$^-$ creation yields up to five times without compromising T2$^*$, T2 and T1, making it a promising approach to enhance the magnetic field sensitivity of NV$^-$ ensembles.

quant-ph↗

arXiv2025

Interactions in Rare Earth Doped Nanoparticles: A Multi-Transition, Concentration, and Excitation Path Analysis

Understanding and modeling energy transfer mechanisms in rare-earth-doped nanomaterials is essential for advancing luminescent technologies used in bioimaging, optical thermometry, and solid-state lasers. In this work, we investigate the photoluminescence dynamics of Yb3+ and Er3+ ions in Y2O3 nanoparticles over a wide concentration range (0.5-17%), using both direct and upconversion excitation. Luminescence decays of green, red, and near-infrared transitions were measured and analyzed using a rate-equation model incorporating radiative and non-radiative processes, energy transfer mechanisms, and defect-related quenching. The model successfully reproduces experimental trends across most concentrations and excitation paths. This work provides a reliable and predictive framework for modeling energy transfer in rare-earth doped materials and offers valuable insights for optimizing photoluminescent properties in nanostructured systems.

cond-mat.mtrl-sci↗

arXiv2025

Nitrogen-Vacancy Centers in Epitaxial Laterally Overgrown Diamond: Towards Up-scaling of Color Center-based Quantum Technologies

Providing high-quality, single-crystal diamond (SCD) with a large area is desirable for up-scaling quantum technology applications that rely on color centers in diamond. Growth methods aiming to increase the area of SCD are an active research area. Native color centers offer a sensitive probe for local crystal quality in such novel materials e.g., via their reaction to stress. In this work, we investigate individual native nitrogen-vacancy (NV) centers in SCD layers manufactured via laterally overgrowing hole arrays in a heteroepitaxially grown large-scale substrate. Heteroepitaxy has become a common tool for growing large SCDs; however, achieving the high crystal quality needed for quantum applications remains a challenge. In the overgrown layer, we identify NV centers with spin-decoherence times in the order of hundreds of microseconds, comparable to high-purity homoepitaxial SCD. We quantify the effective crystal strain in different regions of the overgrown layer, indicating a low stress overall and a stress reduction in the diamond layer above the holes.

cond-mat.mtrl-sci↗

arXiv2024

Erbium doped yttrium oxide thin films grown by chemical vapour deposition for quantum technologies

The obtention of quantum-grade rare-earth doped oxide thin films that can be integrated with optical cavities and microwave resonators is of great interest for the development of scalable quantum devices. Among the different growth methods, Chemical Vapour Deposition (CVD) offers high flexibility and has demonstrated the ability to produce oxide films hosting rare-earth ions with narrow linewidths. However, growing epitaxial films directly on silicon is challenging by CVD due to a native amorphous oxide layer formation at the interface. In this manuscript, we investigate the CVD growth of erbium-doped yttrium oxide (Er:Y2O3) thin films on different substrates, including silicon, sapphire, quartz or yttria stabilized zirconia (YSZ). Alternatively, growth was also attempted on an epitaxial Y2O3 template layer on Si (111) prepared by molecular beam epitaxy (MBE) in order to circumvent the issue of the amorphous interlayer. We found that the substrate impacts the film morphology and the crystalline orientations, with different textures observed for the CVD film on the MBE-oxide/Si template (111) and epitaxial growth on YSZ (001). In terms of optical properties, Er3+ ions exhibit visible and IR emission features that are comparable for all samples, indicating a high-quality local crystalline environment regardless of the substrate. Our approach opens interesting prospects to integrate such films into scalable devices for optical quantum technologies.

cond-mat.mtrl-sci↗

arXiv2024

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↗

arXiv2023

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↗

arXiv2023

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 $\mu$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 $\mu$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↗

arXiv2022

All-Optical Nuclear Quantum Sensing using Nitrogen-Vacancy Centers in Diamond

Solid state spins have demonstrated significant potential in quantum sensing with applications including fundamental science, medical diagnostics and navigation. The quantum sensing schemes showing best performance under ambient conditions all utilize microwave or radio-frequency driving, which poses a significant limitation for miniaturization, energy-efficiency and non-invasiveness of quantum sensors. We overcome this limitation by demonstrating a purely optical approach to coherent quantum sensing. Our scheme involves the $^{15}$N nuclear spin of the Nitrogen-Vacancy (NV) center in diamond as a sensing resource, and exploits NV spin dynamics in oblique magnetic fields near the NV's excited state level anti-crossing to optically pump the nuclear spin into a quantum superposition state. We demonstrate all-optical free-induction decay measurements - the key protocol for low-frequency quantum sensing - both on single spins and spin ensembles. Our results pave the way for highly compact quantum sensors to be employed for magnetometry or gyroscopy applications in challenging environments.

cond-mat.mes-hall↗

arXiv2022

Optical properties of SiV and GeV color centers in nanodiamonds under hydrostatic pressures up to 180 GPa

We investigate the optical properties of silicon-vacancy (SiV) and germanium-vacancy (GeV) color centers in nanodiamonds under hydrostatic pressure up to 180 GPa. The nanodiamonds were synthetized by Si or Ge-doped plasma assisted chemical vapor deposition and, for our experiment, pressurized in a diamond anvil cell. Under hydrostatic pressure we observe blue-shifts of the SiV and GeV zero-phonon lines by 17 THz (70 meV) and 78 THz (320 meV), respectively. These measured pressure induced shifts are in good agreement with ab initio calculations that take into account the lattice compression based on the equation of state of diamond and that are extended to the case of the tin-vacancy (SnV) center. This work provides guidance on the use of group-IV-vacancy centers as quantum sensors under extreme pressures that will exploit their specific optical and spin properties induced by their intrinsic inversion-symmetric structure.

quant-ph↗

arXiv2021

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↗

arXiv2020

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↗

arXiv2020

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 Eu$^{3+}$:Y$_2$O$_3$ 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 using SEMM is then demonstrated for times up to 40 $μ$s. Pulses with two different frequencies are also stored, confirming frequency-multiplexing capability, and are used to demonstrate the memory high phase fidelity.

quant-ph↗

arXiv2019

Initialization and Readout of Nuclear Spins via negatively charged Silicon-Vacancy Center in Diamond

In this work, we demonstrate initialization and readout of nuclear spins via a negatively charged silicon-vacancy (SiV) electron spin qubit. Under Hartmann-Hahn conditions the electron spin polarization is coherently transferred to the nuclear spin. The readout of the nuclear polarization is observed via the fluorescence of the SiV. We also show that the coherence time of the nuclear spin (6 ms) is limited by the electron spin-lattice relaxation due to the hyperfine coupling to the electron spin. This work paves the way towards realization of building blocks of quantum hardware with an efficient spin-photon interface based on the SiV color center coupled to a long lasting nuclear memory.

quant-ph↗

arXiv2018

Microwave device characterisation using a widefield diamond microscope

Devices relying on microwave circuitry form a cornerstone of many classical and emerging quantum technologies. A capability to provide in-situ, noninvasive and direct imaging of the microwave fields above such devices would be a powerful tool for their function and failure analysis. In this work, we build on recent achievements in magnetometry using ensembles of nitrogen vacancy centres in diamond, to present a widefield microwave microscope with few-micron resolution over a millimeter-scale field of view, 130nT/sqrt-Hz microwave amplitude sensitivity, a dynamic range of 48 dB, and sub-ms temporal resolution. We use our microscope to image the microwave field a few microns above a range of microwave circuitry components, and to characterise a novel atom chip design. Our results open the way to high-throughput characterisation and debugging of complex, multi-component microwave devices, including real-time exploration of device operation.

quant-ph↗

arXiv2014

Photonic nano-structures on (111) oriented diamond

We demonstrate the fabrication of single-crystalline diamond nanopillars on a (111)-oriented chemical vapor deposited diamond substrate. This crystal orientation offers optimal coupling of nitrogen-vacancy (NV) center emission to the nanopillar mode and is thus advantageous over previous approaches. We characterize single native NV centers in these nanopillars and find one of the highest reported saturated fluorescence count rates in single crystalline diamond in excess of 10${}^6$ counts per second. We show that our nano-fabrication procedure conserves the preferential alignment as well as the spin coherence of the NVs in our structures. Our results will enable a new generation of highly sensitive probes for NV magnetometry and pave the way toward photonic crystals with optimal orientation of the NV center's emission dipole.

cond-mat.mtrl-sci↗

arXiv2013

Maskless and targeted creation of arrays of colour centres in diamond using focused ion beam technology

The creation of nitrogen-vacancy centres in diamond is nowadays well controlled using nitrogen implantation and annealing. Although the high-resolution placement of NV centres has been demonstrated using either collimation through pierced AFM tips or masks with apertures made by electron beam lithography, a targeted implantation into pre-defined structures in diamond may not be achieved using these techniques. We show that a beam of nitrogen ions can be focused to approximately 100 nm using focused ion beam (FIB) technology. The nitrogen ion beam is produced using an electron cyclotron resonance (ECR) plasma source. Combined with a scanning electron microscope, the nitrogen-FIB offers new possibilities for the targeted creation of single defects in diamond. This maskless technology is suitable for example for the creation of optical centres in the cavities of photonic crystals or in diamond tips for scanning magnetometry. Finally, we further show that by changing the gas source from nitrogen to xenon, standard FIB milling capabilities are also available within the same tool.

cond-mat.mes-hall↗