Role of Oxygen in Laser Induced Contamination at Diamond-Vacuum Interfaces

Many modern-day quantum science experiments rely on high-fidelity measurement of fluorescent signals emitted by the quantum system under study. A pernicious issue encountered when such experiments are conducted near a material interface in vacuum is "laser-induced contamination" (LIC): the gradual accretion of fluorescent contaminants on the surface where a laser is focused. Fluorescence from these contaminants can entirely drown out any signal from e.g. optically-probed color centers in the solid-state. Crucially, while LIC appears often in this context, it has not been systematically studied. In this work, we probe the onset and growth rate of LIC for a diamond nitrogen-vacancy center experiment in vacuum, and we correlate the contamination-induced fluorescence intensities to micron-scale physical build-up of contaminant on the diamond surface. Drawing upon similar phenomena previously studied in the space optics community, we use photo-catalyzed oxidation of contaminants as a mitigation strategy. We vary the residual oxygen pressure over 9 orders of magnitude and find that LIC growth is inhibited at near-atmospheric oxygen partial pressures, but the growth rate at lower oxygen pressure is non-monotonic. Finally, we discuss a model for the observed dependence of LIC growth rate on oxygen content and propose methods to extend in situ mitigation of LIC to a wider range of operating pressures.Comment: 22 pages, 10 figure

Two-dimensional spin systems in PECVD-grown diamond with tunable density and long coherence for enhanced quantum sensing and simulation

Systems of spins engineered with tunable density and reduced dimensionality enable a number of advancements in quantum sensing and simulation. Defects in diamond, such as nitrogen-vacancy (NV) centers and substitutional nitrogen (P1 centers), are particularly promising solid-state platforms to explore. However, the ability to controllably create coherent, two-dimensional spin systems and characterize their properties, such as density, depth confinement, and coherence is an outstanding materials challenge. We present a refined approach to engineer dense ($\gtrsim$1 ppm$\cdot$nm), 2D nitrogen and NV layers in diamond using delta-doping during plasma-enhanced chemical vapor deposition (PECVD) epitaxial growth. We employ both traditional materials techniques, e.g. secondary ion mass spectrometry (SIMS), alongside NV spin decoherence-based measurements to characterize the density and dimensionality of the P1 and NV layers. We find P1 densities of 5-10 ppm$\cdot$nm, NV densities between 1 and 3.5 ppm$\cdot$nm tuned via electron irradiation dosage, and depth confinement of the spin layer down to 1.6 nm. We also observe high (up to 42$\%$) conversion of P1 to NV centers and reproducibly long NV coherence times, dominated by dipolar interactions with the engineered P1 and NV spin baths

Probing many-body noise in a strongly interacting two-dimensional dipolar spin system

The most direct approach for characterizing the quantum dynamics of a strongly-interacting system is to measure the time-evolution of its full many-body state. Despite the conceptual simplicity of this approach, it quickly becomes intractable as the system size grows. An alternate framework is to think of the many-body dynamics as generating noise, which can be measured by the decoherence of a probe qubit. Our work centers on the following question: What can the decoherence dynamics of such a probe tell us about the many-body system? In particular, we utilize optically addressable probe spins to experimentally characterize both static and dynamical properties of strongly-interacting magnetic dipoles. Our experimental platform consists of two types of spin defects in diamond: nitrogen-vacancy (NV) color centers (probe spins) and substitutional nitrogen impurities (many-body system). We demonstrate that signatures of the many-body system's dimensionality, dynamics, and disorder are naturally encoded in the functional form of the NV's decoherence profile. Leveraging these insights, we directly characterize the two-dimensional nature of a nitrogen delta-doped diamond sample. In addition, we explore two distinct facets of the many-body dynamics: First, we address a persistent debate about the microscopic nature of spin dynamics in strongly-interacting dipolar systems. Second, we demonstrate direct control over the spectral properties of the many-body system, including its correlation time. Our work opens the door to new directions in both quantum sensing and simulation.Comment: 10 + 8 + 5 pages; 3 + 5 figure

Diamond Surface Functionalization via Visible Light-Driven C-H Activation for Nanoscale Quantum Sensing

Nitrogen-vacancy centers in diamond are a promising platform for nanoscale nuclear magnetic resonance sensing. Despite significant progress towards 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. NV molecular sensing requires that target molecules are immobilized within a few nanometers of NV centers with long spin coherence time. 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 more 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 to be compatible 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. This functionalization method is compatible with charge stable NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof of principle, we use shallow ensembles of NV centers to detect nuclear spins from functional groups attached to the surface. Our approach to surface functionalization based on visible light-driven C-H bond activation opens the door to deploying NV centers as a broad tool for chemical sensing and single-molecule spectroscopy

Colour centre generation in diamond for quantum technologies

Effective methods to generate colour centres in diamond and other wide band-gap materials are essential to the realisation of solid state quantum technologies based on such systems. Such methods have been the subject of intensive research effort in recent years. In this review, we bring together the various techniques used in the generation and positioning of colour centres in diamond: ion implantation, delta-doping, electron irradiation, laser writing and thermal annealing. We assess the roles and merits of each of these techniques in the formation of colour centres for different quantum technologies and consider future combinations of the techniques to meet the requirements of the most demanding applications