arXiv subjects

David D. Awschalom

Publications and source records attributed to David D. Awschalom.

At least 37 records · Page 2Linked to original sources

arXiv2024

Quantifying the limits of controllability for the nitrogen-vacancy electron spin defect

Solid-state electron spin qubits, like the nitrogen-vacancy center in diamond, rely on control sequences of population inversion to enhance sensitivity and improve device coherence. But even for this paradigmatic system, the fundamental limits of population inversion and potential impacts on applications like quantum sensing have not been assessed quantitatively. Here, we perform high accuracy simulations beyond the rotating wave approximation, including explicit unitary simulation of neighboring nuclear spins. Using quantum optimal control, we identify analytical pulses for the control of a qubit subspace within the spin-1 ground state and quantify the relationship between pulse complexity, control duration, and fidelity. We find exponentially increasing amplitude and bandwidth requirements with reduced control duration and further quantify the emergence of non-Markovian effects for multipulse sequences using sub-nanosecond population inversion. From this, we determine that the reduced fidelity and non-Markovianity is due to coherent interactions of the electron spin with the nuclear spin environment. Ultimately, we identify a potentially realizable regime of nanosecond control duration for high-fidelity multipulse sequences. These results provide key insights into the fundamental limits of quantum information processing using electron spin defects in diamond.

quant-ph↗

arXiv2024

Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl$_3$

Two dimensional (2D) semiconductors present unique opportunities to intertwine optical and magnetic functionalities and to tune these performances through defects and dopants. Here, we integrate exciton pumping into a quantum sensing protocol on nitrogen-vacancy centers in diamond to image the optically-induced transient stray fields in few-layer, antiferromagnetic CrCl$_3$. We discover that exciton recombination enhances the in-plane magnetization of the CrCl$_3$ layers, with a predominant effect in the surface monolayers. Concomitantly, time-resolved photoluminescence measurements reveal that nonradiative exciton recombination intensifies in atomically thin CrCl$_3$ with tightly localized, nearly dipole-forbidden excitons and amplified surface-to-volume ratio. Supported by experiments under controlled surface exposure and density functional theory calculations, we interpret the magnetically enhanced state to result from a defect-assisted Auger recombination that optically activates electron transfer between water vapor related surface impurities and the spin-polarized conduction band. Our work validates defect engineering as a route to enhance intrinsic magnetism in single magnetic layers and opens a novel experimental platform for studying optically-induced, transient magnetism in condensed matter systems.

cond-mat.mtrl-sci↗

arXiv2024

Direct-bonded diamond membranes for heterogeneous quantum and electronic technologies

Diamond has superlative material properties for a broad range of quantum and electronic technologies. However, heteroepitaxial growth of single crystal diamond remains limited, impeding integration and evolution of diamond-based technologies. Here, we directly bond single-crystal diamond membranes to a wide variety of materials including silicon, fused silica, sapphire, thermal oxide, and lithium niobate. Our bonding process combines customized membrane synthesis, transfer, and dry surface functionalization, allowing for minimal contamination while providing pathways for near unity yield and scalability. We generate bonded crystalline membranes with thickness as low as 10 nm, sub-nm interfacial regions, and nanometer-scale thickness variability over 200 by 200 $μm^2$ areas. We measure spin coherence times $T_2$ for nitrogen-vacancy centers in bonded membranes of up to 623(21) $μ$s, suitable for advanced quantum applications. We demonstrate multiple methods for integrating high quality factor nanophotonic cavities with the diamond heterostructures, highlighting the platform versatility in quantum photonic applications. Furthermore, we show that our ultra-thin diamond membranes are compatible with total internal reflection fluorescence (TIRF) microscopy, which enables interfacing coherent diamond quantum sensors with living cells while rejecting unwanted background luminescence. The processes demonstrated herein provide a full toolkit to synthesize heterogeneous diamond-based hybrid systems for quantum and electronic technologies.

physics.app-ph↗

arXiv2024

Coherent Erbium Spin Defects in Colloidal Nanocrystal Hosts

We demonstrate nearly a microsecond of spin coherence in Er3+ ions doped in cerium dioxide nanocrystal hosts, despite a large gyromagnetic ratio and nanometric proximity of the spin defect to the nanocrystal surface. The long spin coherence is enabled by reducing the dopant density below the instantaneous diffusion limit in a nuclear spin-free host material, reaching the limit of a single erbium spin defect per nanocrystal. We observe a large Orbach energy in a highly symmetric cubic site, further protecting the coherence in a qubit that would otherwise rapidly decohere. Spatially correlated electron spectroscopy measurements reveal the presence of Ce3+ at the nanocrystal surface that likely acts as extraneous paramagnetic spin noise. Even with these factors, defect-embedded nanocrystal hosts show tremendous promise for quantum sensing and quantum communication applications, with multiple avenues, including core-shell fabrication, redox tuning of oxygen vacancies, and organic surfactant modification, available to further enhance their spin coherence and functionality in the future.

cond-mat.mes-hall↗

arXiv2024

Extended spin relaxation times of optically addressed telecom defects in silicon carbide

Optically interfaced solid-state defects are promising candidates for quantum communication technologies. The ideal defect system would feature bright telecom emission, long-lived spin states, and a scalable material platform, simultaneously. Here, we employ one such system, vanadium (V4+) in silicon carbide (SiC), to establish a potential telecom spin-photon interface within a mature semiconductor host. This demonstration of efficient optical spin polarization and readout facilitates all optical measurements of temperature-dependent spin relaxation times (T1). With this technique, we lower the temperature from about 2K to 100 mK to observe a remarkable four-orders-of-magnitude increase in spin T1 from all measured sites, with site-specific values ranging from 57 ms to above 27 s. Furthermore, we identify the underlying relaxation mechanisms, which involve a two-phonon Orbach process, indicating the opportunity for strain-tuning to enable qubit operation at higher temperatures. These results position V4+ in SiC as a prime candidate for scalable quantum nodes in future quantum networks.

quant-ph↗

arXiv2024

Anomalous Purcell decay of strongly driven inhomogeneous emitters coupled to a cavity

We perform resonant fluorescence lifetime measurements on a nanocavity-coupled erbium ensemble as a function of cavity-laser detuning and pump power. Our measurements reveal an anomalous three-fold suppression of the ensemble Purcell factor at zero cavity detuning and high pump fluence. We capture qualitative aspects of this decay rate suppression using a Tavis-Cummings model of non-interacting spins coupled to a common cavity.

quant-ph↗

arXiv2024

High-Q Cavity Interface for Color Centers in Thin Film Diamond

Quantum information technology offers the potential to realize unprecedented computational resources via secure channels capable of distributing entanglement between quantum computers. Diamond, as a host to atom-like defects with optically-accessible spin qubits, is a leading platform to realize quantum memory nodes needed to extend the reach of quantum links. Photonic crystal (PhC) cavities enhance light-matter interaction and are essential ingredients of an efficient interface between spins and photons that are used to store and communicate quantum information respectively. Despite great effort, however, the realization of visible PhC cavities with high quality factor (Q) and design flexibility is challenging in diamond. Here, we demonstrate one- and two-dimensional PhC cavities fabricated in recently developed thin-film diamonds, featuring Q-factors of 1.8x10$^5$ and 1.6x10$^5$, respectively, the highest Qs for visible PhC cavities realized in any material. Importantly, our fabrication process is simple and high-yield, based on conventional planar fabrication techniques, in contrast to previous approaches that rely on complex undercut methods. We also demonstrate fiber-coupled 1D PhC cavities with high photon extraction efficiency, and optical coupling between a single SiV center and such a cavity at 4K achieving a Purcell factor of 13. The demonstrated diamond thin-film photonic platform will improve the performance and scalability of quantum nodes and expand the range of quantum technologies.

quant-ph↗

arXiv2023

Quantum spin probe of single charge dynamics

Electronic defects in semiconductors form the basis for many emerging quantum technologies. Understanding defect spin and charge dynamics in solid state platforms is crucial to developing these building blocks, but many defect centers are difficult to access at the single-particle level due to the lack of sensitive readout techniques. A method for probing optically inactive spin defects would reveal semiconductor physics at the atomic scale and advance the study of new quantum systems. We exploit the intrinsic correlation between the charge and spin states of defect centers to measure defect charge populations and dynamics through the steady-state spin population, read-out at the single-defect level with a nearby optically active qubit. We directly measure ionization and charge relaxation of single dark defects in diamond, effects we do not have access to with traditional coherence-based quantum sensing. These spin resonance-based methods generalize to other solid state defect systems in relevant materials.

quant-ph↗

arXiv2023

Microwave-based quantum control and coherence protection of tin-vacancy spin qubits in a strain-tuned diamond membrane heterostructure

Robust spin-photon interfaces in solids are essential components in quantum networking and sensing technologies. Ideally, these interfaces combine a long-lived spin memory, coherent optical transitions, fast and high-fidelity spin manipulation, and straightforward device integration and scaling. The tin-vacancy center (SnV) in diamond is a promising spin-photon interface with desirable optical and spin properties at 1.7 K. However, the SnV spin lacks efficient microwave control and its spin coherence degrades with higher temperature. In this work, we introduce a new platform that overcomes these challenges - SnV centers in uniformly strained thin diamond membranes. The controlled generation of crystal strain introduces orbital mixing that allows microwave control of the spin state with 99.36(9) % gate fidelity and spin coherence protection beyond a millisecond. Moreover, the presence of crystal strain suppresses temperature dependent dephasing processes, leading to a considerable improvement of the coherence time up to 223(10) $μ$s at 4 K, a widely accessible temperature in common cryogenic systems. Critically, the coherence of optical transitions is unaffected by the elevated temperature, exhibiting nearly lifetime-limited optical linewidths. Combined with the compatibility of diamond membranes with device integration, the demonstrated platform is an ideal spin-photon interface for future quantum technologies.

cond-mat.mes-hall↗

arXiv2023

Optical and microstructural characterization of Er$^{3+}$ doped epitaxial cerium oxide on silicon

Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies such as quantum memory, due to the intrinsic spin-photon interface of the rare-earth ion combined with the integration methods available in the solid-state. Erbium-doped cerium oxide (Er:CeO$_2$) is a particularly promising platform for such a quantum memory, as it combines the telecom-wavelength (~1.5 $μ$m) 4f-4f transition of erbium, a predicted long electron spin coherence time supported by CeO$_2$, and is also near lattice-matched to silicon for heteroepitaxial growth. In this work, we report on the epitaxial growth of Er:CeO$_2$ thin films on silicon using molecular beam epitaxy (MBE), with controlled erbium concentration down to 2 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO$_2$ host structure, and characterize the spin and optical properties of the embedded Er$^{3+}$ ions. In the 2-3 ppm Er regime, we identify EPR linewidths of 245(1) MHz, optical inhomogeneous linewidths of 9.5(2) GHz, optical excited state lifetimes of 3.5(1) ms, and spectral diffusion-limited homogenoeus linewidths as narrow as 4.8(3) MHz in the as-grown material. We test annealing of the Er:CeO$_2$ films up to 900 deg C, which yields modest narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%. We have also studied the variation of the optical properties as a function of Er doping and find that the results are consistent with the trends expected from inter-dopant charge interactions.

cond-mat.mtrl-sci↗

arXiv2023

Optical and spin coherence of Er$^{3+}$ in epitaxial CeO$_2$ on silicon

Solid-state atomic defects with optical transitions in the telecommunication bands, potentially in a nuclear spin free environment, are important for applications in fiber-based quantum networks. Erbium ions doped in CeO$_2$ offer such a desired combination. Here we report on the optical homogeneous linewidth and electron spin coherence of Er$^{3+}$ ions doped in CeO$_2$ epitaxial film grown on a Si(111) substrate. The long-lived optical transition near 1530 nm in the environmentally-protected 4f shell of Er$^{3+}$ shows a narrow homogeneous linewidth of 440 kHz with an optical coherence time of 0.72 $μ$s at 3.6 K. The reduced nuclear spin noise in the host allows for Er$^{3+}$ electron spin polarization at 3.6 K, yielding an electron spin coherence of 0.66 $μ$s (in the isolated ion limit) and a spin relaxation of 2.5 ms. These findings indicate the potential of Er$^{3+}$:CeO$_2$ film as a valuable platform for quantum networks and communication applications.

quant-ph↗

arXiv2023

Nanocavity-mediated Purcell enhancement of Er in TiO$_2$ thin films grown via atomic layer deposition

The use of trivalent erbium (Er$^{3+}$), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunications devices and shows promise as a spin-based quantum memory for quantum communication. In particular, its natural telecom C-band optical transition and spin-photon interface makes it an ideal candidate for integration into existing optical fiber networks without the need for quantum frequency conversion. However, successful scaling requires a host material with few intrinsic nuclear spins, compatibility with semiconductor foundry processes, and straightforward integration with silicon photonics. Here, we present Er-doped titanium dioxide (TiO$_2$) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping control over the Er concentration. Even though the as-grown films are amorphous, after oxygen annealing they exhibit relatively large crystalline grains, and the embedded Er ions exhibit the characteristic optical emission spectrum from anatase TiO$_2$. Critically, this growth and annealing process maintains the low surface roughness required for nanophotonic integration. Finally, we interface Er ensembles with high quality factor Si nanophotonic cavities via evanescent coupling and demonstrate a large Purcell enhancement (300) of their optical lifetime. Our findings demonstrate a low-temperature, non-destructive, and substrate-independent process for integrating Er-doped materials with silicon photonics. At high doping densities this platform can enable integrated photonic components such as on-chip amplifiers and lasers, while dilute concentrations can realize single ion quantum memories.

cond-mat.mtrl-sci↗

arXiv2023

Magnon-mediated qubit coupling determined via dissipation measurements

Controlled interaction between localized and delocalized solid-state spin systems offers a compelling platform for on-chip quantum information processing with quantum spintronics. Hybrid quantum systems (HQSs) of localized nitrogen-vacancy (NV) centers in diamond and delocalized magnon modes in ferrimagnets-systems with naturally commensurate energies-have recently attracted significant attention, especially for interconnecting isolated spin qubits at length-scales far beyond those set by the dipolar coupling. However, despite extensive theoretical efforts, there is a lack of experimental characterization of the magnon-mediated interaction between NV centers, which is necessary to develop such hybrid quantum architectures. Here, we experimentally determine the magnon-mediated NV-NV coupling from the magnon-induced self-energy of NV centers. Our results are quantitatively consistent with a model in which the NV center is coupled to magnons by dipolar interactions. This work provides a versatile tool to characterize HQSs in the absence of strong coupling, informing future efforts to engineer entangled solid-state systems.

quant-ph↗

arXiv2023

Guiding Diamond Spin Qubit Growth with Computational Methods

The nitrogen vacancy (NV) center in diamond, a well-studied, optically active spin defect, is the prototypical system in many state of the art quantum sensing and communication applications. In addition to the enticing properties intrinsic to the NV center, its diamond host's nuclear and electronic spin baths can be leveraged as resources for quantum information, rather than considered solely as sources of decoherence. However, current synthesis approaches result in stochastic defect spin positions, reducing the technology's potential for deterministic control and yield of NV-spin bath systems, as well as scalability and integration with other technologies. Here, we demonstrate the use of theoretical calculations of electronic central spin decoherence as an integral part of an NV-spin bath synthesis workflow, providing a path forward for the quantitative design of NV center-based quantum sensing systems. We use computationally generated coherence data to characterize the properties of single NV center qubits across relevant growth parameters to find general trends in coherence time distributions dependent on spin bath dimensionality and density. We then build a maximum likelihood estimator with our theoretical model, enabling the characterization of a test sample through NV T2* measurements. Finally, we explore the impact of dimensionality on the yield of strongly coupled electron spin systems. The methods presented herein are general and applicable to other qubit platforms that can be appropriately simulated.

quant-ph↗

arXiv2023

Detecting spin bath polarization with quantum quench phase shifts of single spins in diamond

Single-qubit sensing protocols can be used to measure qubit-bath coupling parameters. However, for sufficiently large coupling, the sensing protocol itself perturbs the bath, which is predicted to result in a characteristic response in the sensing measurements. Here, we observe this bath perturbation, also known as a quantum quench, by preparing the nuclear spin bath of a nitrogen-vacancy (NV) center in polarized initial states and performing phase-resolved spin echo measurements on the NV electron spin. These measurements reveal a time-dependent phase determined by the initial state of the bath. We derive the relationship between sensor phase and Gaussian spin bath polarization, and apply it to reconstruct both the axial and transverse polarization components. Using this insight, we optimize the transfer efficiency of our dynamic nuclear polarization sequence. This technique for directly measuring bath polarization may assist in preparing high-fidelity quantum memory states, improving nanoscale NMR methods, and investigating non-Gaussian quantum baths.

quant-ph↗

arXiv2022

Purcell enhancement of erbium ions in TiO$_{2}$ on silicon nanocavities

Isolated solid-state atomic defects with telecom optical transitions are ideal quantum photon emitters and spin qubits for applications in long-distance quantum communication networks. Prototypical telecom defects such as erbium suffer from poor photon emission rates, requiring photonic enhancement using resonant optical cavities. Many of the traditional hosts for erbium ions are not amenable to direct incorporation with existing integrated photonics platforms, limiting scalable fabrication of qubit-based devices. Here we present a scalable approach towards CMOS-compatible telecom qubits by using erbium-doped titanium dioxide thin films grown atop silicon-on-insulator substrates. From this heterostructure, we have fabricated one-dimensional photonic crystal cavities demonstrating quality factors in excess of $5\times10^{4}$ and corresponding Purcell-enhanced optical emission rates of the erbium ensembles in excess of 200. This easily fabricated materials platform represents an important step towards realizing telecom quantum memories in a scalable qubit architecture compatible with mature silicon technologies.

cond-mat.mtrl-sci↗

arXiv2022

Development of a Scalable Quantum Memory Platform -- Materials Science of Erbium-Doped TiO$_2$ Thin Films on Silicon

Rare-earth ions (REI) have emerged as an attractive candidate for solid-state qubits, particularly as a quantum memory. Their 4f-4f transitions are shielded by filled 5s and 5p orbitals, offering a degree of protection from external electric fields. Embedded within a thin film oxide host, REIs could enable a qubit platform with significant memory capabilities. Furthermore, a silicon-compatible thin film form factor would enable the use of standard semiconductor fabrication processes to achieve chip-based integrability and scalability for functional quantum networks. Towards this goal, we have carried out optical and microstructural studies of erbium-doped polycrystalline and epitaxial TiO$_2$ thin films on Si (100), r-sapphire, and SrTiO$_3$ (100). We observe that the inhomogeneous optical linewidth of the Er photoluminescence is comparable or better for polycrystalline Er:TiO$_2$(grown on Si) in comparison to single crystal epitaxial films on sapphire or SrTiO$_3$, implying a relative insensitivity to extended defects. We investigated the effect of the film/substrate and film/air interface and found that the inhomogeneous linewidth and spectral diffusion can be significantly improved via bottom buffer and top capping layers of undoped TiO$_2$. Using such approaches, we obtain inhomogeneous linewidths of 5.2 GHz and spectral diffusion of 180 MHz in Er:TiO$_2$ /Si(100) films and have demonstrated the engineerability of quantum-relevant properties in these thin films.

cond-mat.mtrl-sci↗

arXiv2021

Five-second coherence of a single spin with single-shot readout in silicon carbide

An outstanding hurdle for defect spin qubits in silicon carbide (SiC) is single-shot readout - a deterministic measurement of the quantum state. Here, we demonstrate single-shot readout of single defects in SiC via spin-to-charge conversion, whereby the defect's spin state is mapped onto a long-lived charge state. With this technique, we achieve over 80% readout fidelity without pre- or post-selection, resulting in a high signal-to-noise ratio (SNR) that enables us to measure long spin coherence times. Combined with pulsed dynamical decoupling sequences in an isotopically purified host material, we report single spin T2 > 5s, over two orders of magnitude greater than previously reported in this system. The mapping of these coherent spin states onto single charges unlocks both single-shot readout for scalable quantum nodes and opportunities for electrical readout via integration with semiconductor devices.

quant-ph↗