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.

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.

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.

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.