Diamond Surface Research Articles

Theoretical insights into CO2 electroreduction on single and dual heteroatom-doped diamonds

We employed Periodic Density Functional Theory (DFT) to investigate the catalytic activity of single and double dopant of boron (B), nitrogen (N), and phosphorous (P) anchored on diamond surfaces for the CO2 reduction reaction (CO2RR) by analyzing reaction energy profiles. Our findings show that the double-doped catalyst exhibits lower energy barriers in CO2RR compared to the single dopants. Specifically, when considering BB and NN configurations, there is a thermodynamic preference towards the formation of formic acid (HCOOH) with overpotentials of 0.40 and 0.09 V, respectively. The co-doped catalyst comprising B and N (BN) demonstrates a tendency towards the formation of HCOOH without requiring any applied overpotentials. Notably, BN outperforms other catalysts, occupying the top position on the volcano plot, indicating the lowest limiting potential (UL), remarkable thermal stability, and the ability to suppress the competing hydrogen evolution reaction (HER). This research provides valuable insights into the product differentiation in the electroreduction of CO2.

Modulation of spin and charge currents through functionalized 2D diamond devices

In this study, we explore the potential of functionalized two-dimensional (2D) diamond for spin-dependent electronic devices using first-principles calculations. Specifically, we investigate functionalizations with either hydroxyl (−OH) or fluorine (−F) groups. In the case of an isolated layer, we observe that the quantity and distribution of (−OH) or (−F) on the 2D diamond surface significantly influence the sp 2/sp 3 ratio of the carbon atoms in the layer. As the coverage is reduced, both the band gap and magnetic moment decrease. When the 2D diamond is placed between gold contacts and functionalized with (−OH), it results in a device with lower resistance compared to the (−F) functionalization. We predict that the maximum current achieved in the device increases with decreasing (−OH) surface coverage, while the opposite behavior occurs for (−F). Additionally, the surface coverage alone can alter the direction of current rectification in (−F) functionalized 2D diamonds. For all studied systems, a single spin component contributes to the total current for certain values of applied bias, indicating a spin filter behavior.

Charge Stability and Charge-State-Based Spin Readout of Shallow Nitrogen-Vacancy Centers in Diamond.

Spin-based applications of the negatively charged nitrogen-vacancy (NV) center in diamonds require an efficient spin readout. One approach is the spin-to-charge conversion (SCC), relying on mapping the spin states onto the neutral (NV0) and negative (NV-) charge states followed by a subsequent charge readout. With high charge-state stability, SCC enables extended measurement times, increasing precision and minimizing noise in the readout compared to the commonly used fluorescence detection. Nanoscale sensing applications, however, require shallow NV centers within a few nanometers distance from the surface where surface related effects might degrade the NV charge state. In this article, we investigate the charge state initialization and stability of single NV centers implanted ≈5 nm below the surface of a flat diamond plate. We demonstrate the SCC protocol on four shallow NV centers suitable for nanoscale sensing, obtaining a reduced readout noise of 5-6 times the spin-projection noise limit. We investigate the general applicability of the SCC for shallow NV centers and observe a correlation between the NV charge-state stability and readout noise. Coating the diamond with glycerol improves both the charge initialization and stability. Our results reveal the influence of the surface-related charge environment on the NV charge properties and motivate further investigations to functionalize the diamond surface with glycerol or other materials for charge-state stabilization and efficient spin-state readout of shallow NV centers suitable for nanoscale sensing.

Low-temperature characteristics of an AlN/Diamond surface acoustic wave resonator

Phonons confined in mechanical resonators can be coupled to a variety of quantum systems and are expected to be applied to hybrid quantum systems. Diamond surface acoustic wave (SAW) devices are capable of high efficiency in phonon interaction with color centers in diamond. The temperature dependence of the quality factor is crucial for inferring the governing mechanism of coupling efficiency between phonons and color centers in diamond. In this paper, we report on the temperature dependence of the quality factor of an AlN/diamond SAW device from room temperature to 5 K. The temperature dependence of the quality factor and resonant frequency suggests that the mechanism of SAW dissipation in the AlN/diamond SAW resonator at 5 GHz is the phonon–phonon scattering in the Akheiser regime and that further cooling can be expected to improve the quality factor. This result provides a crucial guideline for the future design of AlN/diamond SAW devices.

Direct growth of few-layered graphene on boron doped diamond surface with varying boron doping concentration

The diamond-graphene heterostructure is a promising all‑carbon composite structure, which can take advantages of excellent properties of these two materials. At present, the diamond-graphene heterojunction were mostly synthesized by chemical vapor deposition (CVD) method with intrinsic diamond substrate. In this study, the few-layered graphene is synthesized on boron-doped-diamond (BDD) surface through a simple thermal treatment method with Ni catalyst. The effects of boron doping concentration of substrate on the synthesis of diamond-graphene heterojunctions is studied. It demonstrates that the surface morphology and roughness are improved with the increasing of substrate doping concentration. Compared with the light doped and un-doped diamond, the number of graphene layers and quality decreases and increases, respectively.

Optimizing composition and application conditions of agents for modifying spectral characteristics of diamonds in X-ray luminescence separation

One of the research areas focused on improving the efficiency of diamond-bearing kimberlite beneficiation processes involves the utilization of technology aimed at enhancing the recovery of weakly and anomalously luminescent diamonds during the X-ray luminescence separation process using luminophore-containing chemical agents. The objective of this research was to select the optimal composition of agents that modify the spectral characteristics of minerals and the conditions for their application. A crucial factor for process efficiency is the effective attachment of modifying agents to diamond crystals while avoiding similar attachment to kimberlite mineral surfaces. This is achieved through the use of organic collectors with an optimal composition, characterized by their ability to both adhere to the diamond surface and retain inorganic luminophore grains. The evaluation of luminophore attachment efficiency was performed using visiometric analysis in the UV range. The capability of diamonds to retain luminophore collector droplets or films on their surfaces was evaluated using a technique to measure the three-phase limiting wetting angle. The spectral and kinetic characteristics of diamonds and their recovery during the X-ray luminescence separation process were determined using a POLYUS-M separator. The feasibility of purposefully modifying the spectral characteristics of weakly and anomalously luminescent diamonds through luminophore-containing compositions based on zinc sulfides and zinc orthosilicate has been confirmed through the conducted studies. By considering the criterion of selectivity in the attachment of luminophore emulsion to diamonds and kimberlite minerals, calculated based on the measured surface concentrations of luminophores on the minerals, the optimal ratios between the masses of inorganic luminophore, organic collector, and the aqueous phase of the emulsion were determined. Dispersing agents that offer selective binding of luminophores to diamond crystals were identified, and rational parameters for the composition of the organic collector were established. The temperature range for treating diamond-containing material was defined. As a result of bench testing the modifying agents with the selected composition and conditions for their application in the diamond-containing material treatment cycle before XRF separation, it was confirmed that the recovery of anomalously and weakly luminescent diamonds could exceed 90%, while keeping the yield of kimberlite minerals in the concentrate below 1%.

Interface regulation of diamond-doped GaInSn composites

Diamond-doped GaInSn thermal interface materials have broad application prospects in the field of electronic thermal management. However, the poor wettability of diamond and liquid metal makes the fabrication of composites through simple mechanical agitation difficult. In this study, the wettability between GaInSn and diamond was improved by reducing the surface tension of liquid metal and improving the anisotropy of the diamond surface. The diamond/liquid metal (Dia/LM) interface structure was regulated by controlling the gallium oxide content. Ga2O3 was enriched in the GaInSn and diamond contact surface, which can reduce the surface tension of the liquid metal, improve the wettability of GaInSn to diamond, produce a mechanical locking force with the diamond surface, strengthen the bonding between the liquid metal and the diamond, and reduce the thermal resistance of the liquid metal/diamond interface. The Dia/LM interface structure was controlled by using crushed diamond. Result shows that the wettability of the surface (111) of the diamond was the best. The (100) and (110) planes with poor wettability were cut by the crushed diamond cleavage step, and the area of the crystal plane with poor wettability was reduced, thus improving the wettability of the liquid metal. The improvement of the crushed diamonds' wettability was verified by molecular dynamics calculation. The composite preparation technology of diamond and the GaInSn liquid metal was optimized, and the high-performance Dia/LM thermal interface material was prepared by ultrasonic-assisted and micro-oxidation methods.

Covalent graphene-diamond heterostructure coating on tool surface with enhanced lubricity and anti-wear performance

Graphene possesses extraordinary mechanical strength while it is difficult to integrate graphene layers on macroscale mechanical components due to the weak adhesion strength. In this work, we integrated a top layer of graphene sheets on the diamond-coated tool through in-situ growth of graphene on the diamond grains. With the aid of liquid metal catalyst, ultrastrong C–C covalent bonds are formed in the graphene-diamond interface, which can radically eliminate the peeling off of graphene sheets due to the insufficient adhesion strength. Cutting tests revealed that this top-layer graphene can substantially reduce cutting force and tool flank wear when cutting high-silicon aluminum alloy, with the reduction respectively reaching 40 % and 20 %. During the machining process, the graphene sheets are flattened and they gradually form a compact layer covering on the diamond surface, which can not only lubricate the tool surface but also protect the diamond from wear with the ultrahigh intrinsic strength. Further cutting experiments demonstrated that the effectiveness of the graphene sheets can sustain over 3600 m of cutting distance. The achievement in this work provides a novel insight into the integration of covalent graphene-diamond heterostructures in mechanical systems/devices with outstanding macroscale lubricity and anti-wear performance.

Enhanced holding ability between resin and silanization modified diamonds through sintering Si[sbnd]N bond formation at low temperature

Resin-bonded diamond tools often suffer from poor durability and short lifespan due to the agglomeration of abrasive diamonds and the poor holding ability between diamonds and resin, resulting in diamond detachment during the working process. Modifying the diamond surface is necessary to improve the dispersion of diamonds and the holding ability between diamond and resin. However, common metallic modification methods can cause fine-grained diamonds (FGDs) to agglomerate, and metal plating cannot form a chemical bond with resin at low temperatures for preparing resin-bonded diamond tools. A practical non-metallic method for modifying diamond surfaces was proposed to address these issues, utilizing a silane coupling agent to enhance the binding forces between diamonds and binding agents. A uniform amorphous SiO2 film, with a thickness of 30–40 nm, was developed on FGDs with the hydrolysis and condensation reactions of tetraethylorthosilicate in a water and alcohol mixed solution. The SiO2 layer formed with the CO, CO, and C-O-Si chemical bonds can increase electrostatic repulsion between diamonds, overcoming diamond agglomeration. FGDs modified with SiO2 were combined with phenolic resin and pressed at 170 °C, forming SiN bonds between the resin and SiO2 film and improving the bonding force. Moreover, the SiN bonds can be produced at low temperatures, reducing the risk of diamond detachment during their operation. Hence, the lifespan of modified diamond wheel increase by 22 % than that of pristine diamond wheel. This study provides valuable guidance for developing high-performance, long-lasting, resin-bonded diamond tools.

Widefield Diamond Quantum Sensing with Neuromorphic Vision Sensors.

Despite increasing interest in developing ultrasensitive widefield diamond magnetometry for various applications, achieving high temporal resolution and sensitivity simultaneously remains a key challenge. This is largely due to the transfer and processing of massive amounts of data from the frame-based sensor to capture the widefield fluorescence intensity of spin defects in diamonds. In this study, a neuromorphic vision sensor to encode the changes of fluorescence intensity into spikes in the optically detected magnetic resonance (ODMR) measurements is adopted, closely resembling the operation of the human vision system, which leads to highly compressed data volume and reduced latency. It also results in a vast dynamic range, high temporal resolution, and exceptional signal-to-background ratio. After a thorough theoretical evaluation, the experiment with an off-the-shelf event camera demonstrated a 13× improvement in temporal resolution with comparable precision of detecting ODMR resonance frequencies compared with the state-of-the-art highly specialized frame-based approach. It is successfully deploy this technology in monitoring dynamically modulated laser heating of gold nanoparticles coated on a diamond surface, a recognizably difficult task using existing approaches. The current development provides new insights for high-precision and low-latency widefield quantum sensing, with possibilities for integration with emerging memory devices to realize more intelligent quantum sensors.

Creation of shallow nitrogen vacancy centers in HPHT diamond surface via catalytic etching of transition metal

The nitrogen vacancy (NV) color centers are a solid-state quantum system with the ability to maintain long coherence times at room temperatures. NV centers have potential applications in quantum detection, which necessitates their positioning at minimal distances from surfaces. However, the existing methods for fabricating NV centers are cumbersome, expensive, and difficult to control. This study investigates the etching mechanism of transition metals on diamond under plasma conditions and develops a method for producing shallow NV centers on the surface of high pressure and high temperature diamond. Our proposed method enables the production of shallow NV centers below the surface in the longitudinal direction, while simultaneously allowing precise control over the lateral distribution. Moreover, the operating costs associated with our technique are significantly lower than those of ion implantation and electron irradiation. This research contributes to the advancement of iron-etching diamond processing technology, and the proposed method facilitates the more portable preparation of shallow color centers in specific regions, enabling the realization of locally controllable and scalable coupled quantum systems.

Deposition and Characterisation of a Diamond/Ti/Diamond Multilayer Structure

In this work, a diamond/Ti/diamond multilayer structure has been fabricated by successively following thin-film CVD and PVD routes. It has been found that a combined pre-treatment of the silicon base substrate, via argon plasma etching for creating surface roughness and, thereafter, detonation nanodiamond (DND) seeding, helps in the nucleation and growth of well-adherent CVD diamond films with a well-defined Raman signal at 1332 cm−1, showing the crystalline nature of the film. Ti sputtering on such a CVD-grown diamond surface leads to an imprinted bead-like microstructure of the titanium film, generated from the underlying diamond layer. The cross-sectional thickness of the titanium layer can be found to vary by as much as 0.5 µm across the length of the surface, which was caused by a subsequent hydrogen plasma etching process step of the composite film conducted after Ti sputtering. The hydrogen plasma etching of the Ti–diamond composite film was found to be essential for smoothening the uneven as-grown texture of the films, which was developed due to the unequal growth of the microcrystalline diamond columns. Such hydrogen plasma surface treatment helped further the nucleation and growth of a nanocrystalline diamond film as the top layer, which was deposited following a similar CVD route to that used in depositing the bottom diamond layer, albeit with different process parameters. For the latter, a hydrogen gas diluted with PH3 precursor recipe produced smaller nanocrystalline diamond crystals for the top layer. The titanium layer in between the two diamond layers possesses a very-fine-grained microstructure. Transmission electron microscopy (TEM) results show evidence of intermixing between the titanium and diamond layers at their respective interfaces. The thin films in the composite multilayer follow the contour of the plasma-etched silicon substrate and are thus useful in producing continuous protective coatings on 3D objects—a requirement for many engineering applications.

Theoretical prediction of hafnium-terminated diamond (100) surface with promising negative electron affinity for electron emission applications

Controlling the chemical termination of diamond surface shows great promise in achieving negative electron affinity (NEA). In this work, we explore the feasibility of obtaining stable NEA properties by hafnium (Hf) termination on bare and oxidized diamond (100) surfaces based on swarm-intelligence structural search and first-principles calculations. The negative adsorption energies demonstrate that Hf-terminated diamond surfaces are energetically favorable. Remarkably, the lowest-energy structure at 0.25 monolayer Hf coverage on an oxidized surface has an extremely large adsorption energy of −11.15 eV, which is consistent with the largest bonding orbital population of 7.28 eV. The most negative NEA values of bare and oxidized surfaces are −3.50 and −3.19 eV at 0.25 monolayer Hf coverage, respectively. Both structures have dynamic stability, and the oxidized surface exhibits excellent thermal stability even up to 1200 K. Owing to their super stability and outstanding NEA properties, Hf-terminated diamond surfaces are suggested as promising candidate materials for electron emission applications.

Highly conductive diamond skeleton reinforced Cu-matrix composites for high-efficiency thermal management

The weak interfacial bonding strength between diamond and copper intrinsically restricts the enhancement of the thermal conductivity of diamond particles/copper composites (abbreviated as DP/Cu). This work first proposed the diamond skeleton (DS) as the reinforcement element rather than dispersed diamond particles. The tungsten (W) transition layer (c.a. ∼300 nm thick) having adequate thermal expansion coefficient was sputtered onto the surface of DS via vacuum evaporation technology, aiming to improve the wettability between diamond and copper and accordingly increase the thermal conductivity of DS/copper composites extruded by gas pressure infiltration technique. The experimental results show that the coated W layer can effectively improve the wettability of the diamond surface and reduce the wettability angle from 108.6° to 13.2°. Raman and XRD spectra show that the W layer can, to a great extent, prevent the graphitization of the diamond surface. SEM and EDX evidence a continuous heat transfer path of DS inside the composites. The thermal conductivity of the DS/Cu composite with low diamond loading of 18.4 vol% reaches 575 W/mK, 43.3% higher than that of pure Cu. Finite element simulations show that DS exhibits excellent heat transfer characteristics, agreeing well with the thermal conductivity simulation results.

Coherent manipulation of nuclear spins in the strong driving regime

Spin-based quantum information processing makes extensive use of spin-state manipulation. This ranges from dynamical decoupling of nuclear spins in quantum sensing experiments to applying logical gates on qubits in a quantum processor. Fast manipulation of spin states is highly desirable for accelerating experiments, enhancing sensitivity, and applying elaborate pulse sequences. Strong driving using intense radio-frequency (RF) fields can, therefore, facilitate fast manipulation and enable broadband excitation of spin species. In this work, we present an antenna for strong driving in quantum sensing experiments and theoretically address challenges of the strong driving regime. First, we designed and implemented a micron-scale planar spiral RF antenna capable of delivering intense fields to a sample. The planar antenna is tailored for quantum sensing experiments using the diamond’s nitrogen-vacancy (NV) center and should be applicable to other solid-state defects. The antenna has a broad bandwidth of 22 MHz, is compatible with scanning probes, and is suitable for cryogenic and ultrahigh vacuum conditions. We measure the magnetic field induced by the antenna and estimate a field-to-current ratio of G/A, representing a six-fold increase in efficiency compared to the state-of-the-art, crucial for cryogenic experiments. We demonstrate the antenna by driving Rabi oscillations in 1H spins of an organic sample on the diamond surface and measure 1H Rabi frequencies of over 500 kHz, i.e. -pulses shorter than 1 —an order of magnitude faster than previously reported in NV-based nuclear magnetic resonance (NMR). Finally, we discuss the implications of driving spins with a field tilted from the transverse plane in a regime where the driving amplitude is comparable to the spin-state splitting, such that the rotating wave approximation does not describe the dynamics well. We present a simple recipe to optimize pulse fidelity in this regime based on a phase and offset-shifted sine drive, which may be optimized in situ without numerical optimization procedures or precise modeling of the experiment. We consider this approach in a range of driving amplitudes and show that it is particularly efficient in the case of a tilted driving field. The results presented here constitute a foundation for implementing fast nuclear spin control in various systems.

Instantaneous formation of covalently bonded diamond–graphite–graphene with synergistic properties

Diamond and graphene are the most widely used carbon allotropes and offer great potential for developing mechanical, electronic, energy-storage, and sensor applications. Their combination, especially interfacial covalent bonding, can impart excellent properties. However, achieving interfacial covalent bonding with superior performance using flexible and low-power strategies remains challenging. This study developed a novel instantaneous transformation method from diamond to graphene to prepare a new covalent structure of diamond–nano-graphite–graphene (CDGG). That is, a nanosecond-pulse laser induces sp3-to-sp2 instantaneous transformations from diamond to graphite in air, and the subsequent mechanical cleavage overcomes the weak van der Waals forces to achieve the final transformation of graphite to graphene. First, the key factors influencing laser-induced graphitization and mechanical cleavage were investigated, and a covalent carbon structure with multidirectional graphene was obtained. Furthermore, the mechanisms encompassing the lattice transformation, interface relationships, transformation time, and interface bonding were elucidated. The obtained new structure synergized the excellent properties of diamond, nano-graphite, and graphene, exhibiting superior lubrication, mechanochemical wear resistance, durability, and load-capacity. Compared to polished diamond, the obtained structure exhibited a significant decrease in the stable coefficient of friction by 49–59 % and a reduction of more than one order of magnitude in the relative wear rate under high friction against ferrous metals with a normal load of 1–9 N. Even under a heavy load of 100 N, it still exhibited superior lubrication and mechanochemical wear resistance. Finally, the preparation and patterning of covalent carbon structures were achieved on various diamond surfaces with high efficiency, environmental friendliness, and low power. This study is expected to broaden the scope of developing and applying diamond, diamond films, and graphene devices.

X-ray quantification of oxygen groups on diamond surfaces for quantum applications

Identifying the surface chemistry of diamond materials is increasingly important for device applications, especially quantum sensors. Oxygen-related termination species are widely used because they are naturally abundant, chemically stable, and compatible with stable nitrogen vacancy centres near the diamond surface. Diamond surfaces host a mixture of oxygen-related species, and the precise chemistry and relative coverage of different species can lead to dramatically different electronic properties, with direct consequences for near-surface quantum sensors. However, it is challenging to unambiguously identify the different groups or quantify the relative surface coverage. Here we show that a combination of x-ray absorption and photoelectron spectroscopies can be used to quantitatively identify the coverage of carbonyl functional groups on the diamond surface. Using this method we reveal an unexpectedly high fraction of carbonyl groups (9%) on a wide range of sample surfaces. Furthermore, through a combination of ab initio calculations and spectroscopic studies of engineered surfaces, we reveal unexpected complexities in the x-ray spectroscopy of oxygen terminated diamond surfaces. Of particular note, we find the binding energies of carbonyl-related groups on diamond differs significantly from other organic systems, likely resulting in previous misestimation of carbonyl fractions on diamond surfaces.

Mechanistic insights into the formation of dislocation-related pits on diamond surface under plasma etching treatment: A combined simulation and experimental approach

Reactive ion etching (RIE) is a widely applied technique for high-precision machining of demanding diamond devices. However, the persistent challenge of widely distributed dislocation-related etch pits on processed surfaces remains poorly understood. In this study, the material removal and pit formation during the etching of the dislocation region by hydrogen and oxygen were investigated by reactive force-field (ReaxFF) molecular dynamics simulation combined with experimental verification. The results unveiled the pivotal role of crystal structure disruption and symmetrically distributed stress, induced by dislocations, in promoting bond-breaking processes and triggering the formation of etch pits. The etching parameter optimized simulations revealed that once the impact effect of oxygen atoms counterbalances the promotion of dislocation to the bond breaking, the formation of dislocation pits can be effectively avoided, which is convincingly validated by experimental results. Besides, our research further verified that pure hydrogen etching is an inefficient surface post-treatment process with a more significant pit-forming problem, and exists two distinct pit-forming mechanisms dependent on the incident energy. Additionally, substrate temperature variation has global but negligible influences on pits formation within the 400 K range. These findings carry significant implications for the optimization of processing parameters and the large-scale implementation of RIE in diamond processing, demonstrating the potential to address pit-forming issues with commonly used gases.

Electrochemical Properties and Structure of Membranes from Perfluorinated Copolymers Modified with Nanodiamonds.

In this study, we aimed to design and research proton-conducting membranes based on Aquivion®-type material that had been modified with detonation nanodiamonds (particle size 4-5 nm, 0.25-5.0 wt. %). These nanodiamonds carried different functional groups (H, OH, COOH, F) that provided the hydrophilicity of the diamond surface with positive or negative potential, or that strengthened the hydrophobicity of the diamonds. These variations in diamond properties allowed us to find ways to improve the composite structure so as to achieve better ion conductivity. For this purpose, we prepared three series of membrane films by first casting solutions of perfluorinated Aquivion®-type copolymers with short side chains mixed with diamonds dispersed on solid substrates. Then, we removed the solvent and the membranes were structurally stabilized during thermal treatment and transformed into their final form with -SO3H ionic groups. We found that the diamonds with a hydrogen-saturated surface, with a positive charge in aqueous media, contributed to the increase in proton conductivity of membranes to a greater rate. Meanwhile, a more developed conducting diamond-copolymer interface was formed due to electrostatic attraction to the sulfonic acid groups of the copolymer than in the case of diamonds grafted with negatively charged carboxyls, similar to sulfonic groups of the copolymer. The modification of membranes with fluorinated diamonds led to a 5-fold decrease in the conductivity of the composite, even when only a fraction of diamonds of 1 wt. % were used, which was explained by the disruption in the connectivity of ion channels during the interaction of such diamonds mainly with fluorocarbon chains of the copolymer. We discussed the specifics of the mechanism of conductivity in composites with various diamonds in connection with structural data obtained in neutron scattering experiments on dry membranes, as well as ideas about the formation of cylindrical micelles with central ion channels and shells composed of hydrophobic copolymer chains. Finally, the characteristics of the network of ion channels in the composites were found depending on the type and amount of introduced diamonds, and correlations between the structure and conductivity of the membranes were established.

Hydrogen and oxygen mixed-termination for nitrogen-vacancy quantum sensors in hexagonal diamond

Controlling the chemical termination of hexagonal diamond surface opens up new possibilities for shallow nitrogen-vacancy (NV) centers in quantum sensing applications. In this work, the H/O/OH mixed terminations on hexagonal diamond (100) surfaces to host NV centers are investigated by first-principles calculations. Results indicate that H–O, O–OH, and H–O–OH mixed surfaces produce positive electron affinity with neither spin noise nor surface-related state. It is concluded that the surface-connected ether bonds should be maintained, and unconnected ether bonds should be avoided, preserving the shallow NV centers unaffected. Based on the surface stability analysis, we further confirm that the H–O surface has a higher possibility to be fabricated. Moreover, we make an intensive study by placing an NV center ∼12 Å from the hexagonal (100) surface, and the results elucidate that the H–O surface has no obvious effect on the defect states of the NV center. Therefore, we identify a combination of surface terminators that is a prospective candidate for NV-based quantum sensors.