Diamond surface functionalization via visible light-driven C-H activation for nanoscale quantum sensing.

Nitrogen-vacancy (NV) centers in diamond are a promising platform for nanoscale NMR sensing. Despite significant progress toward using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. Such sensing requires that target molecules are immobilized within nanometers of NV centers with long spin coherence. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C-H bonds on single-crystal diamond surfaces under ambient conditions using visible light, forming C-F, C-Cl, C-S, and C-N bonds at the surface. This method is compatible with NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof-of-principle demonstration, we use shallow ensembles of NV centers to detect nuclear spins from surface-bound functional groups. Our approach to surface functionalization opens the door to deploying NV centers as a tool for chemical sensing and single-molecule spectroscopy.

Indistinguishable telecom band photons from a single Er ion in the solid state.

Atomic defects in the solid state are a key component of quantum repeater networks for long-distance quantum communication1. Recently, there has been significant interest in rare earth ions2-4, in particular Er3+ for its telecom band optical transition5-7 that allows long-distance transmission in optical fibres. However, the development of repeater nodes based on rare earth ions has been hampered by optical spectral diffusion, precluding indistinguishable single-photon generation. Here, we implant Er3+ into CaWO4, a material that combines a non-polar site symmetry, low decoherence from nuclear spins8 and is free of background rare earth ions, to realize significantly reduced optical spectral diffusion. For shallow implanted ions coupled to nanophotonic cavities with large Purcell factor, we observe single-scan optical linewidths of 150 kHz and long-term spectral diffusion of 63 kHz, both close to the Purcell-enhanced radiative linewidth of 21 kHz. This enables the observation of Hong-Ou-Mandel interference9 between successively emitted photons with a visibility of V = 80(4)%, measured after a 36 km delay line. We also observe spin relaxation times T1,s = 3.7 s and T2,s > 200 µs, with the latter limited by paramagnetic impurities in the crystal instead of nuclear spins. This represents a notable step towards the construction of telecom band quantum repeater networks with single Er3+ ions.

Chemical Profiles of the Oxides on Tantalum in State of the Art Superconducting Circuits.

Over the past decades, superconducting qubits have emerged as one of the leading hardware platforms for realizing a quantum processor. Consequently, researchers have made significant effort to understand the loss channels that limit the coherence times of superconducting qubits. A major source of loss has been attributed to two level systems that are present at the material interfaces. It is recently shown that replacing the metal in the capacitor of a transmon with tantalum yields record relaxation and coherence times for superconducting qubits, motivating a detailed study of the tantalum surface. In this work, the chemical profile of the surface of tantalum films grown on c-plane sapphire using variable energy X-ray photoelectron spectroscopy (VEXPS) is studied. The different oxidation states of tantalum that are present in the native oxide resulting from exposure to air are identified, and their distribution through the depth of the film is measured. Furthermore, it is shown how the volume and depth distribution of these tantalum oxidation states can be altered by various chemical treatments. Correlating these measurements with detailed measurements of quantum devices may elucidate the underlying microscopic sources of loss.

Neutral Silicon Vacancy Centers in Undoped Diamond via Surface Control.

Neutral silicon vacancy centers (SiV^{0}) in diamond are promising candidates for quantum applications; however, stabilizing SiV^{0} requires high-purity, boron-doped diamond, which is not a readily available material. Here, we demonstrate an alternative approach via chemical control of the diamond surface. We use low-damage chemical processing and annealing in a hydrogen environment to realize reversible and highly stable charge state tuning in undoped diamond. The resulting SiV^{0} centers display optically detected magnetic resonance and bulklike optical properties. Controlling the charge state tuning via surface termination offers a route for scalable technologies based on SiV^{0} centers, as well as charge state engineering of other defects.

Hybrid Integration of GaP Photonic Crystal Cavities with Silicon-Vacancy Centers in Diamond by Stamp-Transfer.

Optically addressable solid-state defects are emerging as some of the most promising qubit platforms for quantum networks. Maximizing photon-defect interaction by nanophotonic cavity coupling is key to network efficiency. We demonstrate fabrication of gallium phosphide 1-D photonic crystal waveguide cavities on a silicon oxide carrier and subsequent integration with implanted silicon-vacancy (SiV) centers in diamond using a stamp-transfer technique. The stamping process avoids diamond etching and allows fine-tuning of the cavities prior to integration. After transfer to diamond, we measure cavity quality factors (Q) of up to 8900 and perform resonant excitation of single SiV centers coupled to these cavities. For a cavity with a Q of 4100, we observe a 3-fold lifetime reduction on-resonance, corresponding to a maximum potential cooperativity of C = 2. These results indicate promise for high photon-defect interaction in a platform which avoids fabrication of the quantum defect host crystal.

A Telecom O-Band Emitter in Diamond.

Color centers in diamond are promising platforms for quantum technologies. Most color centers in diamond discovered thus far emit in the visible or near-infrared wavelength range, which are incompatible with long-distance fiber communication and unfavorable for imaging in biological tissues. Here, we report the experimental observation of a new color center that emits in the telecom O-band, which we observe in silicon-doped bulk single crystal diamonds and microdiamonds. Combining absorption and photoluminescence measurements, we identify a zero-phonon line at 1221 nm and phonon replicas separated by 42 meV. Using transient absorption spectroscopy, we measure an excited state lifetime of around 270 ps and observe a long-lived baseline that may arise from intersystem crossing to another spin manifold.

Room-Temperature Photochromism of Silicon Vacancy Centers in CVD Diamond.

The silicon vacancy (SiV) center in diamond is typically found in three stable charge states, SiV0, SiV-, and SiV2-, but studying the processes leading to their formation is challenging, especially at room temperature, due to their starkly different photoluminescence rates. Here, we use confocal fluorescence microscopy to activate and probe charge interconversion between all three charge states under ambient conditions. In particular, we witness the formation of SiV0 via the two-step capture of diffusing, photogenerated holes, a process we expose both through direct SiV0 fluorescence measurements at low temperatures and confocal microscopy observations in the presence of externally applied electric fields. In addition, we show that continuous red illumination induces the converse process, first transforming SiV0 into SiV- and then into SiV2-. Our results shed light on the charge dynamics of SiV and promise opportunities for nanoscale sensing and quantum information processing.

Nanoscale covariance magnetometry with diamond quantum sensors.

Nitrogen vacancy (NV) centers in diamond are atom-scale defects that can be used to sense magnetic fields with high sensitivity and spatial resolution. Typically, the magnetic field is measured by averaging sequential measurements of single NV centers, or by spatial averaging over ensembles of many NV centers, which provides mean values that contain no nonlocal information about the relationship between two points separated in space or time. Here, we propose and implement a sensing modality whereby two or more NV centers are measured simultaneously, and we extract temporal and spatial correlations in their signals that would otherwise be inaccessible. We demonstrate measurements of correlated applied noise using spin-to-charge readout of two NV centers and implement a spectral reconstruction protocol for disentangling local and nonlocal noise sources.

Biocompatible surface functionalization architecture for a diamond quantum sensor.

Quantum metrology enables some of the most precise measurements. In the life sciences, diamond-based quantum sensing has led to a new class of biophysical sensors and diagnostic devices that are being investigated as a platform for cancer screening and ultrasensitive immunoassays. However, a broader application in the life sciences based on nanoscale NMR spectroscopy has been hampered by the need to interface highly sensitive quantum bit (qubit) sensors with their biological targets. Here, we demonstrate an approach that combines quantum engineering with single-molecule biophysics to immobilize individual proteins and DNA molecules on the surface of a bulk diamond crystal that hosts coherent nitrogen vacancy qubit sensors. Our thin (sub-5 nm) functionalization architecture provides precise control over the biomolecule adsorption density and results in near-surface qubit coherence approaching 100 µs. The developed architecture remains chemically stable under physiological conditions for over 5 d, making our technique compatible with most biophysical and biomedical applications.

Materials challenges and opportunities for quantum computing hardware.

Quantum computing hardware technologies have advanced during the past two decades, with the goal of building systems that can solve problems that are intractable on classical computers. The ability to realize large-scale systems depends on major advances in materials science, materials engineering, and new fabrication techniques. We identify key materials challenges that currently limit progress in five quantum computing hardware platforms, propose how to tackle these problems, and discuss some new areas for exploration. Addressing these materials challenges will require scientists and engineers to work together to create new, interdisciplinary approaches beyond the current boundaries of the quantum computing field.

Hybrid III-V diamond photonic platform for quantum nodes based on neutral silicon vacancy centers in diamond.

Integrating atomic quantum memories based on color centers in diamond with on-chip photonic devices would enable entanglement distribution over long distances. However, efforts towards integration have been challenging because color centers can be highly sensitive to their environment, and their properties degrade in nanofabricated structures. Here, we describe a heterogeneously integrated, on-chip, III-V diamond platform designed for neutral silicon vacancy (SiV0) centers in diamond that circumvents the need for etching the diamond substrate. Through evanescent coupling to SiV0 centers near the surface of diamond, the platform will enable Purcell enhancement of SiV0 emission and efficient frequency conversion to the telecommunication C-band. The proposed structures can be realized with readily available fabrication techniques.

New material platform for superconducting transmon qubits with coherence times exceeding 0.3 milliseconds.

The superconducting transmon qubit is a leading platform for quantum computing and quantum science. Building large, useful quantum systems based on transmon qubits will require significant improvements in qubit relaxation and coherence times, which are orders of magnitude shorter than limits imposed by bulk properties of the constituent materials. This indicates that relaxation likely originates from uncontrolled surfaces, interfaces, and contaminants. Previous efforts to improve qubit lifetimes have focused primarily on designs that minimize contributions from surfaces. However, significant improvements in the lifetime of two-dimensional transmon qubits have remained elusive for several years. Here, we fabricate two-dimensional transmon qubits that have both lifetimes and coherence times with dynamical decoupling exceeding 0.3 milliseconds by replacing niobium with tantalum in the device. We have observed increased lifetimes for seventeen devices, indicating that these material improvements are robust, paving the way for higher gate fidelities in multi-qubit processors.

Optically Detected Magnetic Resonance in Neutral Silicon Vacancy Centers in Diamond via Bound Exciton States.

Neutral silicon vacancy (SiV^{0}) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive due to poor understanding of the excited state fine structure and limited off-resonant spin polarization. Here we report the realization of optically detected magnetic resonance and coherent control of SiV^{0} centers at cryogenic temperatures, enabled by efficient optical spin polarization via previously unreported higher-lying excited states. We assign these states as bound exciton states using group theory and density functional theory. These bound exciton states enable new control schemes for SiV^{0} as well as other emerging defect systems.

Narrow Optical Line Widths in Erbium Implanted in TiO2.

Atomic and atomlike defects in the solid state are widely explored for quantum computers, networks, and sensors. Rare earth ions are an attractive class of atomic defects that feature narrow spin and optical transitions that are isolated from the host crystal, allowing incorporation into a wide range of materials. However, the realization of long electronic spin coherence times is hampered by magnetic noise from abundant nuclear spins in the most widely studied host crystals. Here, we demonstrate that Er3+ ions can be introduced via ion implantation into TiO2, a host crystal that has not been studied extensively for rare earth ions and has a low natural abundance of nuclear spins. We observe efficient incorporation of the implanted Er3+ into the Ti4+ site (>50% yield) and measure narrow inhomogeneous spin and optical line widths (20 and 460 MHz, respectively) that are comparable to bulk-doped crystalline hosts for Er3+. This work demonstrates that ion implantation is a viable path to studying rare earth ions in new hosts and is a significant step toward realizing individually addressed rare earth ions with long spin coherence times for quantum technologies.

Observation of an environmentally insensitive solid-state spin defect in diamond.

Engineering coherent systems is a central goal of quantum science. Color centers in diamond are a promising approach, with the potential to combine the coherence of atoms with the scalability of a solid-state platform. We report a color center that shows insensitivity to environmental decoherence caused by phonons and electric field noise: the neutral charge state of silicon vacancy (SiV0). Through careful materials engineering, we achieved >80% conversion of implanted silicon to SiV0 SiV0 exhibits spin-lattice relaxation times approaching 1 minute and coherence times approaching 1 second. Its optical properties are very favorable, with ~90% of its emission into the zero-phonon line and near-transform-limited optical linewidths. These combined properties make SiV0 a promising defect for quantum network applications.

Improving Defect-Based Quantum Emitters in Silicon Carbide via Inorganic Passivation.

Defect-based color centers in wide-bandgap crystalline solids are actively being explored for quantum information science, sensing, and imaging. Unfortunately, the luminescent properties of these emitters are frequently degraded by blinking and photobleaching that arise from poorly passivated host crystal surfaces. Here, a new method for stabilizing the photoluminescence and charge state of color centers based on epitaxial growth of an inorganic passivation layer is presented. Specifically, carbon antisite-vacancy pairs (CAV centers) in 4H-SiC, which serve as single-photon emitters at visible wavelengths, are used as a model system to demonstrate the power of this inorganic passivation scheme. Analysis of CAV centers with scanning confocal microscopy indicates a dramatic improvement in photostability and an enhancement in emission after growth of an epitaxial AlN passivation layer. Permanent, spatially selective control of the defect charge state can also be achieved by exploiting the mismatch in spontaneous polarization at the AlN/SiC interface. These results demonstrate that epitaxial inorganic passivation of defect-based quantum emitters provides a new method for enhancing photostability, emission, and charge state stability of these color centers.

Visible-frequency hyperbolic metasurface.

Metamaterials are artificial optical media composed of sub-wavelength metallic and dielectric building blocks that feature optical phenomena not present in naturally occurring materials. Although they can serve as the basis for unique optical devices that mould the flow of light in unconventional ways, three-dimensional metamaterials suffer from extreme propagation losses. Two-dimensional metamaterials (metasurfaces) such as hyperbolic metasurfaces for propagating surface plasmon polaritons have the potential to alleviate this problem. Because the surface plasmon polaritons are guided at a metal-dielectric interface (rather than passing through metallic components), these hyperbolic metasurfaces have been predicted to suffer much lower propagation loss while still exhibiting optical phenomena akin to those in three-dimensional metamaterials. Moreover, because of their planar nature, these devices enable the construction of integrated metamaterial circuits as well as easy coupling with other optoelectronic elements. Here we report the experimental realization of a visible-frequency hyperbolic metasurface using single-crystal silver nanostructures defined by lithographic and etching techniques. The resulting devices display the characteristic properties of metamaterials, such as negative refraction and diffraction-free propagation, with device performance greatly exceeding those of previous demonstrations. Moreover, hyperbolic metasurfaces exhibit strong, dispersion-dependent spin-orbit coupling, enabling polarization- and wavelength-dependent routeing of surface plasmon polaritons and two-dimensional chiral optical components. These results open the door to realizing integrated optical meta-circuits, with wide-ranging applications in areas from imaging and sensing to quantum optics and quantum information science.

Free-standing mechanical and photonic nanostructures in single-crystal diamond.

A variety of nanoscale photonic, mechanical, electronic, and optoelectronic devices require scalable thin film fabrication. Typically, the device layer is defined by thin film deposition on a substrate of a different material, and optical or electrical isolation is provided by the material properties of the substrate or by removal of the substrate. For a number of materials this planar approach is not feasible, and new fabrication techniques are required to realize complex nanoscale devices. Here, we report a three-dimensional fabrication technique based on anisotropic plasma etching at an oblique angle to the sample surface. As a proof of concept, this angled-etching methodology is used to fabricate free-standing nanoscale components in bulk single-crystal diamond, including nanobeam mechanical resonators, optical waveguides, and photonic crystal and microdisk cavities. Potential applications of the fabricated prototypes range from classical and quantum photonic devices to nanomechanical-based sensors and actuators.

Tailoring light-matter interaction with a nanoscale plasmon resonator.

We propose and demonstrate a new approach for achieving enhanced light-matter interactions with quantum emitters. Our approach makes use of a plasmon resonator composed of defect-free, highly crystalline silver nanowires surrounded by patterned dielectric distributed Bragg reflectors. These resonators have an effective mode volume (V(eff)) 2 orders of magnitude below the diffraction limit and a quality factor (Q) approaching 100, enabling enhancement of spontaneous emission rates by a factor exceeding 75 at the cavity resonance. We also show that these resonators can be used to convert a broadband quantum emitter to a narrow-band single-photon source with color-selective emission enhancement.

Vibrational excitation in single-molecule transistors: deviation from the simple franck-condon prediction.

We investigated the inner-sphere reorganization of ferrocene ((Cp) 2Fe ( n+ )) and tris(2,2'-bipyridine) iron ((bpy) 3Fe ( n+ )) in a single-molecule-transistor geometry. In (Cp) 2Fe ( n+ ) ( n = 0 and 1), almost no vibrations were excited during single-electron transport, whereas in (bpy) 3Fe ( n+ ) ( n = 1, 2, and 3), many distinct vibrations appeared, consistent with its larger reorganization energy. The observed excitation intensities varied significantly across devices, however, and could not be accounted for by "Franck-Condon" factors. This observation indicates that a quantitative account of electron-vibration coupling in single-electron tunneling requires further investigation.