arXiv subjects

Diana Serrano

Publications and source records attributed to Diana Serrano.

At least 19 recordsLinked to original sources

arXiv2025

Optical investigation of ultra-slow spin relaxation in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$ single crystals

We present a comprehensive study of spin relaxation dynamics at cryogenic temperatures in a rare-earth-doped crystal used for quantum memory applications: $^{171}$Yb:Y$_2$SiO$_5$. Spin relaxation is indeed a major limiting factor for both the efficiency and storage time of quantum memory protocols based on atomic frequency combs in rare-earth materials. The relaxation dynamics among the four ground-state hyperfine levels were simultaneously investigated by optically perturbing the spin population distribution and monitoring its return to thermal equilibrium through optical absorption spectroscopy. By applying different types of perturbations, we were also able to distinguish between two types of relaxation processes, induced by spin-phonon and spin-spin interactions. Below 1 K, we observed that the re-thermalization of the Yb$^{3+}$ ion population takes several hours, driven solely by direct phonon absorption or emission. However, the effective lifetime of individual spin states is much shorter - on the order of several seconds in low-doped (2 ppm) samples and of milliseconds in 10 ppm samples - due to spin-spin interactions. These findings provide valuable guidelines for optimizing doping levels and operating temperatures in rare-earth-doped crystals for quantum applications. Notably, they suggest that atomic frequency combs with lifetimes of several hours could be realized using $^{171}$Yb:Y$_2$SiO$_5$ crystals with slightly less than 2 ppm doping and operating near 1 K.

physics.atom-ph↗

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

Optically detected nuclear magnetic resonance of coherent spins in a molecular complex

Nuclear magnetic resonance (NMR) is a powerful tool for applications ranging from chemical analysis to quantum information processing. Achieving optical initialization and detection of molecular nuclear spins promises new opportunities - including improved NMR signals at low magnetic field, sensitivity down to the single-molecule level, and full access to atomically precise molecular architectures for quantum technologies. In this study, we report optical readout of coherently controlled nuclear spins in a europium-based molecular crystal. By harnessing ultra-narrow optical transitions, we achieve optical initialization and detection of nuclear spin states. Through radio-frequency driving, we address two nuclear quadrupole resonances, characterized by narrow inhomogeneous linewidths and a distinct correlation with the optical transition frequency. We implement Rabi oscillations, spin echo and dynamical decoupling techniques, achieving nuclear spin quantum coherence with a lifetime of up to 2 ms. These results highlight the capabilities of optically detected NMR (ODNMR) and underscore the potential of molecular nuclear spins for quantum information processing.

quant-ph↗

arXiv2025

Sub-second spin and lifetime-limited optical coherences in $^{171}$Yb$^{3+}$:CaWO$_4$

Optically addressable solid-state spins have been extensively studied for quantum technologies, offering unique advantages for quantum computing, communication, and sensing. Advancing these applications is generally limited by finding materials that simultaneously provide lifetime-limited optical and long spin coherences. Here, we introduce $^{171}$Yb$^{3+}$ ions doped into a CaWO$_4$ crystal. We perform high-resolution spectroscopy of the excited state, and demonstrate all-optical coherent control of the electron-nuclear spin ensemble. We find narrow inhomogeneous broadening of the optical transitions of 185 MHz and radiative-lifetime-limited coherence time up to 0.75~ms. Next to this, we measure a spin-transition ensemble line width of 5 kHz and electron-nuclear spin coherence time reaching 0.15~seconds at zero magnetic field between 50~mK and 1~K temperatures. These results demonstrate the potential of $^{171}$Yb$^{3+}$:CaWO$_4$ as a low-noise platform for building quantum technologies with ensemble-based memories, microwave-to-optical transducers, and optically addressable single-ion spin qubits.

quant-ph↗

arXiv2025

Ultralong-lived Coherent States in Eu$^{3+}$:Y$_2$O$_3$ Optical Ceramics for Quantum Memories

Rare earth ions (REI) in solid materials are among the leading systems for quantum technology applications. However, developing practical REI quantum devices with long-lived coherent states remains challenging due to great growth difficulties of high-quality REI materials and a lack of comprehensive understanding of REI's decoherence mechanisms. Here we realize a record optical coherence time of 421.5 $\pm$ 10.5 $\mu$s for the $^7$F$_0\rightarrow^5$D$_0$ transition and more than 30 hours lifetime for the $^7$F$_0$ hyperfine spin states in Eu$^{3+}$:Y$_2$O$_3$ optical ceramics. We report the elimination of two-level-system induced optical decoherence in short-range ordered crystals. Meanwhile, a new decoherence mechanism caused by new kinds of perturbing magnetic centers is identified below 1.5 K. We further demonstrate the coherent light storage over 5 $\mu$s by using the atomic frequency comb protocol. These results open up prospects for the realization of practical quantum memories and large scale quantum communications with REI optical ceramics.

quant-ph↗

arXiv2025

Multimodal Purcell enhancement and optical coherence of Eu$^{\text{3+}}$ ions in a single nanoparticle coupled to a microcavity

Europium-doped nanocrystals constitute a promising material for a scalable future quantum computing platform. Long-lived nuclear spin states could serve as qubits addressed via coherent optical transitions. In order to realize an efficient spin-photon interface, we couple the emission from a single nanoparticle to a fiber-based microcavity under cryogenic conditions. The spatial and spectral tunability of the cavity permits us to place individual nanoparticles in the cavity, to measure the inhomogeneous linewidth of the ions, and to show a multi-modal Purcell-enhancement of two transition in Eu$^{\text{3+}}$. A halving of the free-space lifetime to 1.0 ms is observed, corresponding to a 140-fold enhancement of the respective transition. Furthermore, we observe a narrow optical linewidth of 3.3 MHz for a few-ion ensemble in the center of the inhomogeneous line. The results represent an important step towards the efficient readout of single Eu$^{\text{3+}}$ ions, a key requirement for the realization of single-ion-level quantum processing nodes in the solid state.

quant-ph↗

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

Incoherent Measurement of Sub-10 kHz Optical Linewidths

Quantum state lifetimes $T_2$, or equivalently homogeneous linewidths $\Gamma_h = 1/\pi T_2$, are a key parameter for understanding decoherence processes in quantum systems and assessing their potential for applications in quantum technologies. The most common tool for measuring narrow optical homogeneous linewidths, i.e. long $T_2$, is the measurement of coherent photon echo emissions, which however gives very weak signal when the number of emitters is small. This strongly hampers the development of nano-materials, such as those based on rare earth ions, for quantum communication and processing. In this work we propose, and demonstrate in an erbium doped crystal, a measurement of photon echoes based on incoherent fluorescence detection and its variance analysis. It gives access to $T_2$ through a much larger signal than direct photon echo detection, and, importantly, without the need for a highly coherent laser. Our results thus open the way to efficiently assess the properties of a broad range of emitters and materials for applications in quantum nano-photonics.

quant-ph↗

arXiv2024

Opto-RF transduction in Er$^{3+}$:CaWO$_4$

We use an erbium doped CaWO$_4$ crystal as a resonant transducer between the RF and optical domains at 12 GHz and 1532 nm respectively. We employ a RF resonator to enhance the spin coupling but keep a single-pass (non-resonant) optical setup. The overall efficiency is low but we carefully characterize the transduction process and show that the performance can be described by two different metrics that we define and distinguish: the electro-optics and the quantum efficiencies. We reach an electro-optics efficiency of -84 dB for 15.7 dBm RF power. The corresponding quantum efficiency is -142 dB for 0.4 dBm optical power. We develop the Schrödinger-Maxwell formalism, well-known to describe light-matter interactions in atomic systems, in order to model the conversion process. We explicitly make the connection with the cavity quantum electrodynamics (cavity QED) approach that are generally used to describe quantum transduction.

quant-ph↗

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

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↗

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 $μ$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↗

arXiv2023

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↗

arXiv2022

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↗

arXiv2021

High connectivity quantum processor nodes using single-ion-qubits in rare-earth-ion-doped crystals

We present two protocols for constructing quantum processor nodes in randomly doped rare-earth-ion crystals and analyze their properties. By varying the doping concentration and the accessible laser tunability, the processor nodes can contain anywhere from only a few tens to almost $1000$ qubits. Furthermore, the average number of qubits each qubit can interact with, denoted by the connectivity, can be partly tailored to lie between just a few and roughly one hundred. We also study how a limited tunability of the laser affects the results, and conclude that a tuning range of $100$ GHz limits the results to roughly $100$ qubits with around $50$ connections per qubit on average. In order to construct an even larger processor, the vision is that several of these quantum processor nodes should be connected to each other in a multi-node architecture via, e.g., optical interfaces or flying qubits in the form of light. Our results are encouraging for establishing the rare-earth-ion-based systems as a quantum computing platform with strong potential and can serve to focus the efforts within the field.

quant-ph↗

arXiv2021

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↗

arXiv2020

Molecule-based coherent light-spin interfaces for quantum information processing -- optical spin state polarization in a binuclear Europium complex

The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ions (REIs) are suitable candidates for QIP protocols due to their extraordinary photo-physical and magnetic quantum properties such as long optical and spin coherence lifetimes ($T_2$). However, molecules incorporating REIs, despite having advantageous properties such as atomically exact quantum tunability, inherent scalability, and large portability, have not yet been studied for QIP applications. As a first testimony of the usefulness of REI molecules for optical QIP applications, we demonstrate in this study that narrow spectral holes can be burned in the inhomogeneously broadened $^5$D$_0\to^7$F$_0$ optical transition of a binuclear Eu(III) complex, rendering a homogeneous linewidth ($Γ_h$) = 22 $\pm$ 1 MHz, which translates as $T_2 = 14.5$ $\pm$ 0.7 ns at 1.4 K. Moreover, long-lived spectral holes are observed, demonstrating efficient polarization of Eu(III) ground state nuclear spins, a fundamental requirement for all-optical spin initialization and addressing. These results elucidate the usefulness of REI-based molecular complexes as versatile coherent light-spin interfaces for applications in quantum communications and processing.

quant-ph↗