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This study focuses on the self-assembly and subsequent diamond growth on SiO$_2$ buffered lithium niobate (LiNbO$_3$) and lithium tantalate (LiTaO$_3$) single crystals. The zeta-potential of LNO and LTO single crystal were measured as a function of pH. They were found to be negative in the pH range 3.5-9.5. The isoelectric point for LNO was found to be at pH $\sim$ 2.91 and that of LTO to be at pH $\sim$ 3.20. X-ray photoelectron spectroscopy performed on the surfaces show presence of oxygen groups which may be responsible for the negative zeta potential of the crystals. Self-assembly of nanodiamond particles on LTO and LNO, using nanodiamond colloid, were studied. As expected, high nanodiamond density was seen when self-assembly was done using a positively charged nanodiamond particles. Diamond growth was attempted on the nanodiamond coated substrates but they were found to be unsuitable for direct growth due to disintegration of substrates in diamond growth conditions.. A $\sim$100nm thick silicon dioxide layer was deposited on the crystals, followed by nanodiamond self assembly and diamond growth. Thin diamond films were successfully grown on both coated crystals. The diamond quality was analysed by Raman spectroscopy and atomic force microscopy.

The negatively charged nitrogen-vacancy centre (NV$^-$) in diamond has been utilized in a wide variety of sensing applications. The centre's long spin coherence and relaxation times ($T_2^*$, $T_2$ and $T_1$) at room temperature are crucial to this, as they often limit sensitivity. Using NV$^-$ centres in nanodiamonds allows for operations in environments inaccessible to bulk diamond, such as intracellular sensing. We report long spin coherence and relaxation times at room temperature for single NV$^-$ centres in isotopically-purified polycrystalline ball-milled nanodiamonds. Using a spin-locking pulse sequence, we observe spin coherence times, $T_2$, up 786 $\pm$ 200 $\mu$s. We also measure $T_2^*$ times up to 2.06 $\pm$ 0.24 $\mu$s and $T_1$ times up to 4.32 $\pm$ 0.60 ms. Scanning electron microscopy and atomic force microscopy measurements show that the diamond containing the NV$^{-}$ centre with the longest $T_1$ time is smaller than 100 nm. EPR measurements give an N$_{s}$$^{0}$ concentration of 0.15 $\pm$ 0.02 ppm for the nanodiamond sample., Comment: 13 pages, 3 figures

A superconducting boron doped nanocrystalline diamond (B-NCD) coplanar waveguide resonator (CPR) is presented for kinetic inductance ($L_k$) and penetration depth ($\lambda_{\rm{L}}$) measurements at microwave frequencies of 0.4 to 1.2 GHz and at temperatures below 3 K. Using a simplified effective medium CPR approach, this work demonstrates that thin granular B-NCD films ($t\approx $ 500 nm) on Si have a large penetration depth ($\lambda_{\rm{L}}\approx 4.3$ to 4.4 $\mu$m), and therefore an associated high kinetic inductance ($L_{k,\square} \approx $ 670 to 690 pH/$\square$). These values are much larger than those typically obtained for films on single crystal diamond which is likely due to the significant granularity of the nanocrystalline films. Based on the measured Q factors of the structure, the calculated surface resistance in this frequency range is found to be as low as $\approx$ 2 to 4 $\mu\Omega$ at $T<2$ K, demonstrating the potential for granular B-NCD for high quality factor superconducting microwave resonators and highly sensitive kinetic inductance detectors., Comment: First draft

A microwave plasma model of a chemical vapour deposition (CVD) reactor is presented for understanding spatial heteroepitaxial growth of polycrystalline diamond on Si. This work is based on the TM0(n>1)p clamshell style reactor (Seki Diamond/ASTEX SDS 6K, Carat CTS6U, ARDIS-100 style) whereby a simplified H_2 plasma model is used to show the radial variation in growth rate over small samples with different sample holders. The model uses several steps: an electromagnetic (EM) eigenfrequency solution, a frequency-transient EM/plasma fluid solution and transient a heat transfer solution at low and high microwave power density. Experimental growths provide model validation with characterisation using Raman spectroscopy and scanning electron microscopy. This work demonstrates that shallow holders result in non-uniform diamond films, with a radial variation akin to the electron density and temperature distribution at the wafer surface. For the same process conditions, greater homogeneity is observed for taller holders, however, if the height is too extreme, the diamond quality reduces. From a modelling perspective, EM solutions are limited but useful for examining electric field focusing at the sample edges, resulting in accelerated diamond growth. For better accuracy, plasma fluid and heat transfer solutions are imperative for modelling spatial growth variation., Comment: EDIT1: Title changed

Diamond is a material that offers potential in numerous device applications. In particular, highly boron doped diamond is attractive due to its superconductivity and high Young's Modulus. The fabrication of stable, low resistance, ohmic contacts is essential to ensure proper device function. Previous work has established the efficacy of several methods of forming suitable contacts to diamond at room temperature and above, including carbide forming and carbon soluble metallisation schemes. Herein, the stability of several contact schemes (Ti, Cr, Mo, Ta and Pd) to highly boron doped nanocrystalline diamond was verified down to the cryogenic temperatures with modified Transmission Line Model (TLM) measurements. While all contact schemes remained ohmic, a significant temperature dependency is noted at Tc and at the lowest temperatures the contact resistances ranged from Ti/Pt/Au with ${(8.83 \pm 0.10)\times 10^{-4} \:{\Omega}.cm}$ to Ta/Pt/Au with ${(8.07 \pm 0.62) \times 10^{-6} \:{\Omega}.cm}$., Comment: 14 pages, 5 figures

In this work a strategy to grow diamond on $\beta$-Ga$_2$O$_3$ has been presented. The $\zeta$-potential of the $\beta$-Ga$_2$O$_3$ substrate was measured and it was found to be negative with an isoelectric point at pH $\sim$ 4.6. The substrates were seeded with mono-dispersed diamond solution for growth of diamond. The seeded substrates were etched when exposed to diamond growth plasma and globules of gallium could be seen on the surface. To overcome the problem $\sim$100 nm of SiO$_2$ and Al$_2$O$_3$ were deposited using atomic layer deposition. The nanodiamond seeded SiO$_2$ layer was effective in protecting the $\beta$-Ga$_2$O$_3$ substrate and thin diamond layers could be grown. In contrast Al$_2$O$_3$ layers were damaged when exposed to diamond growth plasma. The thin diamond layers were characterised with scanning electron microscopy and Raman spectroscopy. Raman spectroscopy revealed the diamond layer to be under compressive stress of 1.3 -- 2.8GPa.

Diamond heat-spreaders for gallium nitride (GaN) devices currently depend upon a robust wafer bonding process. Bonding-free membrane methods demonstrate potential, however, chemical vapour deposition (CVD) of diamond directly onto a III-nitride (III-N) heterostructure membrane induces significant thermal stresses. In this work, these thermal stresses are investigated using an analytical approach, a numerical model and experimental validation. The thermal stresses are caused by the mismatch in the coefficient of thermal expansion (CTE) between the GaN/III-N stack, silicon (Si) and the diamond from room temperature to CVD growth temperatures. Simplified analytical wafer bow models underestimate the membrane bow for small sizes while numerical models replicate the stresses and bows with increased accuracy using temperature gradients. The largest tensile stress measured using Raman spectroscopy at room temperature was approximately 1.0 $\pm0.2$ GPa while surface profilometry shows membrane bows as large as \SI{58}{\micro\metre}. This large bow is caused by additional stresses from the Si frame in the initial heating phase which are held in place by the diamond and highlights challenges for any device fabrication using contact lithography. However, the bow can be reduced if the membrane is pre-stressed to become flat at CVD temperatures. In this way, a sufficient platform to grow diamond on GaN/III-N structures without wafer bonding can be realised.

High-lying Rydberg states of Mott-Wannier excitons are receiving considerable interest due to the possibility of adding long-range interactions to the physics of exciton-polaritons. Here, we study Rydberg excitation in bulk synthetic cuprous oxide grown by the optical float zone technique and compare the result with natural samples. X-ray characterization confirms both materials are mostly single crystal, and mid-infrared transmission spectroscopy revealed little difference between synthetic and natural material. The synthetic samples show principal quantum numbers up to $n=10$, exhibit additional absorption lines, plus enhanced spatial broadening and spatial inhomogeneity. Room temperature and cryogenic photoluminescence measurements reveal a significant excess of copper vacancies in the synthetic material. These measurements provide a route towards achieving \mbox{high-$n$} excitons in synthetic crystals, opening a route to scalable quantum devices., Comment: 10 pages, 8 figures, submitted to Phys. Rev. Materials

The fluorescent nitrogen-vacancy (NV) defect in diamond has remarkable photophysical properties, including high photostability, which allows stable fluorescence emission for hours; as a result, there has been much interest in using nanodiamonds (NDs) for quantum optics and biological imaging. Such applications have been limited by the complexity and heterogeneity of ND photophysics. Photophysics of the NV center in NDs have been studied before, but the lack of a sensitive and high-throughput method has limited the characterization of NDs. Here is reported a systematic analysis of NDs using two-color wide-field epifluorescence imaging coupled to high-throughput single-particle detection of single NVs in NDs with sizes down to 5-10 nm. By using fluorescence intensity ratios, the charge conversion of single NV center (NV- or NV0) is observed and the lifetimes of different NV charge states in NDs is measured. The discovery of reversible manipulation of NV charge states by pH is also presented. In addition to provide another mechanism to control the NV charge state in nanodiamonds, our findings open the possibility to perform pH nanosensing with a non-photobleachable probe., Comment: Manuscript: 30 pages, 5 figures; supplementary information: 12 pages, 11 figures

Growth of $>$100 $\mu$m thick diamond layer adherent on aluminium nitride is presented in this work. While thick films failed to adhere on untreated AlN films, hydrogen/nitrogen plasma treated AlN films retained the thick diamond layers. Clear differences in zeta potential measurement confirms the surface modification due to hydrogen/nitrogen plasma treatment. Areal Raman maps showed an increase in non-diamond carbon in the initial layers of diamond grown on pre-treated AlN. The presence of non-diamond carbon has minimal effect on the interface between diamond and AlN. The surfaces studied with x-ray photoelectron spectroscopy (XPS) revealed a clear distinction between pre-treated and untreated samples. The surface aluminium goes from nitrogen rich environment to an oxygen rich environment after pre-treatment. Cross section transmission electron microscopy shows a clean interface between diamond and AlN. Thermal barrier resistance between diamond and AlN was found to be in the range of 16 m$^2$K/GW which is a large improvement on the current state-of-the-art.

Hexagonal boron nitride (h-BN) is a critical material for 2D electronic devices for graphene and has attracted a considerable amount of attention owing to its structural similarity and semiconducting property. However, modifying its wide-band gap is a challenge. Hydrogenation is a potential method of altering the electrical properties, although is seldom experimentally measured. Here, the complex permittivity of h-BN after various hydrogen treatments have been investigated. For untreated h-BN, a frequency independent dielectric constant was measured ($\sim4.2 \pm0.2$) and an immeasurably low dielectric loss, demonstrating the ideal dielectric nature of h-BN across the $10^3$ to $10^{10}$ Hz range. However, after atomic H-plasma treatment in a microwave chemical vapour deposition (CVD) reactor, the complex permittivity amplifies dramatically, introducing dielectric dispersion through Debye-type dielectric relaxations ($\varepsilon_{\textrm{s}}\approx20\pm2$, $\varepsilon_{\infty}\approx4.2\pm0.2$) and a percolating long range conductivity ($\sim0.32$ mS/m). Annealing in molecular hydrogen at similar CVD temperatures showed minimal effect. Raman spectroscopy also detected minimal change in all samples, implying the increase is not due to other phases. This leads to the experimental conclusion that hydrogenation, through atomic H-plasma treatment, results in a moderate increase in room temperature electrical conductivity, an associated finite dielectric loss factor. The potential as a tunable wide-band gap semiconductor is highlighted however for insulating dielectric substrate applications, microwave CVD may destroy these desirable properties.

In this work we have demonstrated the growth of nanocrystalline diamond on boron nitride ceramic. We measured the zeta potential of the ceramics to select the diamond seeds. Diamond was then grown on the seeded ceramics using a microwave chemical vapour deposition system. A clear difference was found between the samples which were seeded with nanodiamond and the ones not seeded before growth. Raman spectroscopy confirmed the excellent quality of the diamond film. Dielectric measurements showed an increase in the dielectric constant of the material after diamond growth. The diamond was also doped with boron to make it superconducting. The film had a transition temperature close to 3.4K. Similar strategies can be applied for growth of diamond on other types of ceramics.

Based on the superconducting quantum interference device (SQUID) equations described by the resistively- and capacitively-shunted junction model coupled to the equation of motion of a damped harmonic oscillator, we provide simulations to quantitatively describe the interaction between a dc SQUID and an integrated doubly clamped cantilever. We have chosen to investigate an existing experimental configuration and have explored the motion of the cantilever and the reaction of the SQUID as a function of the voltage-flux $V(\Phi)$ characteristics. We clearly observe the Lorentz force back-action interaction and demonstrate how a sharp transition state drives the system into a nonlinear-like regime, and modulates the cantilever displacement amplitude, simply by tuning the SQUID parameters.

Chemical vapour deposition (CVD) grown nanocrystalline diamond is an attractive material for the fabrication of devices. For some device architectures, optimisation of its growth on silicon nitride is essential. Here, the effects of three pre-growth surface treatments, often employed as cleaning methods of silicon nitride, were investigated. Such treatments provide control over the surface charge of the substrate through modification of the surface functionality, allowing for the optimisation of electrostatic diamond seeding densities. Zeta potential measurements and X-ray photoelectron spectroscopy (XPS) were used to analyse the silicon nitride surface following each treatment. Exposing silicon nitride to an oxygen plasma offered optimal surface conditions for the electrostatic self-assembly of a hydrogen-terminated diamond nanoparticle monolayer. The subsequent growth of boron-doped nanocrystalline diamond thin films on modified silicon nitride substrates under CVD conditions produced coalesced films for oxygen plasma and solvent treatments, whilst pin-holing of the diamond film was observed following RCA-1 treatment. The sharpest superconducting transition was observed for diamond grown on oxygen plasma treated silicon nitride, demonstrating it to be of the least structural disorder. Modifications to the substrate surface optimise the seeding and growth processes for the fabrication of diamond on silicon nitride devices.

In this paper, the controlled production of high quality metal-free diamond nanoparticles is demonstrated. Milling with tempered steel is shown to leave behind iron oxide contamination which is difficult to remove. Milling with SiN alleviates this issue but generates more non diamond carbon. Thus the choice of milling materials is critically determined by the acceptable contaminants in the ultimate application. The removal of metal impurities, present in all commercially available nanoparticles, will open new possibilities towards the production of customised diamond nanoparticles, covering the most demanding quantum applications.

The silicon-vacancy (SiV) color center in diamond is a solid-state single photon emitter and spin quantum bit suited as a component in quantum devices. Here, we show that the SiV center in nanodiamond exhibits a strongly inhomogeneous distribution with regard to the center wavelengths and linewidths of the zero-phonon-line (ZPL) emission at room temperature. We find that the SiV centers separate in two clusters: one group exhibits ZPLs with center wavelengths within a narrow range of approximatly 730 nm to 742 nm and broad linewidths between 5 nm and 17 nm, whereas the second group comprises a very broad distribution of center wavelengths between 715 nm and 835 nm, but narrow linewidths from below 1 nm up to 4 nm. Supported by ab initio Kohn-Sham density functional theory calculations we show that the ZPL shifts of the first group are consistently explained by strain in the diamond lattice. Further, we suggest, that the second group showing the strongly inhomogeneous distribution of center wavelengths might be comprised of modified SiV centers. Whereas single photon emission is demonstrated for SiV centers of both clusters, we show that emitters from different clusters show different spectroscopic features such as variations of the phonon sideband spectra and different blinking dynamics.

In this paper the design of a simple, space constrained chemical vapour deposition reactor for diamond growth is detailed. Based on the design by NIRIM, the reactor is composed of a quartz discharge tube placed within a 2.45 GHz waveguide to create the conditions required for metastable growth of diamond. Utilising largely off-the-shelf components and a modular design, the reactor allows for easy modification, repair, and cleaning between growth runs. The elements of the reactor design are laid out with the CAD files, parts list, and control files made easily available to enable replication. Finally, the quality of nanocrystalline diamond films produced are studied with SEM and Raman spectroscopy, with the observation of clear faceting and a large diamond fraction suggesting the design offers deposition of diamond with minimal complexity.

Battery-like supercapacitors feature high power and energy densities as well as long-term capacitance retention. The utilized capacitor electrodes are thus better to have large surface areas, high conductivity, high stability, and importantly be of binder free. Herein, vertically aligned carbon nanofibers (CNFs) coated boron-doped diamonds (BDD) are employed as the capacitor electrodes to construct battery-like supercapacitors. Grown via a thermal chemical vapor deposition technique, these CNFs/BDD hybrid films are binder free and own porous structures, resulting in large surface areas. Meanwhile, the containment of graphene layers and copper metal catalysts inside CNFs/BDD leads to their high conductivity. Electric double layer capacitors (EDLCs) and pseudocapacitors (PCs) are then constructed in the inert electrolyte (1.0 M H2SO4 solution) and in the redox-active electrolyte (1.0 M Na2SO4 + 0.05 M Fe(CN)63-/4-), respectively. For assembled two-electrode symmetrical supercapacitor devices, the capacitances of EDLC and PC devices reach 30 and 48 mF cm-2 at 10 mV s-1, respectively. They remain constant even after 10 000 cycles. The power densities are 27.3 kW kg-1 and 25.3 kW kg-1 for EDLC and PC devices, together with their energy densities of 22.9 Wh kg-1 and 44.1 Wh kg-1, respectively. The performance of formed EDLC and PC devices is comparable to market-available batteries. Therefore, the vertically aligned CNFs/BDD hybrid film is a suitable capacitor electrode material to construct high-performance battery-like and industry-orientated supercapacitors for flexible power devices.

The chemical nature of the chemical mechanical polishing of diamond has been examined by adding various redox agents to the alkaline SF1 polishing slurry. Three oxidizing agents namely, hydrogen peroxide, potassium permanganate and ferric nitrate, and two reducing agents, oxalic acid and sodium thiosulfate, were added to the SF1 slurry. Oxalic acid produced the fastest polishing rate while hydrogen peroxide had very little effect on polishing, probably due to its volatile nature. X-ray photoelectron spectroscopy (XPS) reveals little difference in the surface oxygen content on the polished samples using various slurries. This suggests that the addition of redox agents do not increase the density of oxygen containing species on the surface but accelerates the process of attachment and removal of Si or O atoms within the slurry particles to the diamond surface.

Measurement of zeta potential of Ga and N-face gallium nitride has been carried out as function of pH. Both the faces show negative zeta potential in the pH range 5.5-9. The Ga face has an isoelectric point at pH 5.5. The N-face shows higher negative zeta potential due to larger concentration of adsorbed oxygen. Zeta potential data clearly showed that H-terminated diamond seed solution at pH 8 will be optimal for the self assembly of a monolayer of diamond nanoparticles on the GaN surface. Subsequent growth of thin diamond films on GaN seeded with H-terminated diamond seeds produced fully coalesced films confirming a seeding density in excess of 10$^{12}$ cm$^{-2}$. This technique removes the requirement for a low thermal conduction seeding layer like silicon nitride on GaN.