Single Crystal Diamond Membranes Research Articles

Single-photon emission from silicon-vacancy color centers in polycrystalline diamond membranes

Single-color centers in thin polycrystalline diamond membranes allow the platform to be used in integrated quantum photonics, hybrid quantum systems, and other complex functional materials. While single-crystal diamond membranes are still technologically challenging to fabricate as they cannot be grown on a non-diamond substrate, free-standing polycrystalline diamond membranes can be conveniently fabricated at large-scale from nanocrystalline diamond seeds on a substrate that can be selectively etched. However, their practical application for quantum photonics is so far limited by crystallographic defects, impurities, graphitic grain boundaries, small grain sizes, scattering loss, and strain. In this paper, we report on a single-photon source based on silicon-vacancy color centers in a polycrystalline diamond membrane. We discuss the spectroscopic approach and quantify the photon statistics, obtaining a g2(0) ≈ 0.04. Our findings hold promise for introducing polycrystalline diamond to quantum photonics and hybrid quantum systems.

Fabrication of thin diamond membranes by [formula omitted] implantation

Color centers in diamond are one of the most promising tools for quantum information science. Of particular interest is the use of single-crystal diamond membranes with nanoscale-thickness as hosts for color centers. Indeed, such structures guarantee a better integration with a variety of other quantum materials or devices, which can aid the development of diamond-based quantum technologies, from nanophotonics to quantum sensing. A common approach for membrane production is what is known as “smart-cut”, a process where membranes are exfoliated from a diamond substrate after the creation of a thin sub-surface amorphous carbon layer by He+ implantation. Due to the high ion fluence required, this process can be time-consuming. In this work, we demonstrated the production of thin diamond membranes by neon implantation of diamond substrates. With the target of obtaining membranes of ∼200 nm thickness and finding the critical damage threshold, we implanted different diamonds with 300 keV Ne+ ions at different fluences. We characterized the structural properties of the implanted diamonds and the resulting membranes through SEM, Raman spectroscopy, and photoluminescence spectroscopy. We also found that a SRIM model based on a two-layer diamond/sp2-carbon target better describes ion implantation, allowing us to estimate the diamond critical damage threshold for Ne+ implantation. Compared to He+ smart-cut, the use of a heavier ion like Ne+ results in a ten-fold decrease in the ion fluence required to obtain diamond membranes and allows to obtain shallower smart-cuts, i.e. thinner membranes, at the same ion energy.

Scanning Cavity Microscopy of a Single-Crystal Diamond Membrane

Spin-bearing color centers in the solid state are promising candidates for the realization of quantum networks and distributed quantum computing. A remaining key challenge is their efficient and reliable interfacing to photons. Incorporating minimally processed membranes into open-access microcavities represents a promising route for Purcellenhanced spin-photon interfaces: it enables significant emission enhancement and efficient photon collection, minimizes deteriorating influence on the quantum emitter, and allows for full spatial and spectral tunability, key for controllably addressing suitable emitters with desired optical and spin properties. Here, we study the properties of a high-finesse fiber Fabry-P\'erot microcavity with integrated single-crystal diamond membranes by scanning cavity microscopy. We observe spatially resolved the effects of the diamond-air interface on the cavity mode structure: a strong correlation of the cavity finesse and mode structure with the diamond thickness and surface topography, significant transverse-mode mixing under diamond-like conditions, and mode-character-dependent polarization-mode splitting. Our results reveal the influence of the diamond surface on the achievable Purcell enhancement, which helps to clarify the route towards optimized spin-photon interfaces.

A diamond-confined open microcavity featuring a high quality-factor and a small mode-volume

With a highly coherent, optically addressable electron spin, the nitrogen-vacancy (NV) center in diamond is a promising candidate for a node in a quantum network. A resonant microcavity can boost the flux of coherent photons emerging from single NV centers. Here, we present an open Fabry–Pérot microcavity geometry containing a single-crystal diamond membrane, which operates in a regime where the vacuum electric field is strongly confined to the diamond membrane. There is a field anti-node at the diamond–air interface. Despite the presence of surface losses, a finesse of F=11500 was observed. The quality (Q) factor for the lowest mode number is 120000; the mode volume V is estimated to be 3.9λ03, where λ0 is the free-space wavelength. We investigate the interplay between different loss mechanisms and the impact these loss channels have on the performance of the cavity. This analysis suggests that the surface waviness (roughness with a spatial frequency comparable to that of the microcavity mode) is the mechanism preventing the Q/V ratio from reaching even higher values. Finally, we apply the extracted cavity parameters to the NV center and calculate a predicted Purcell factor exceeding 150.

Telecommunication-wavelength two-dimensional photonic crystal cavities in a thin single-crystal diamond membrane

We demonstrate two-dimensional photonic crystal cavities operating at telecommunication wavelengths in a single-crystal diamond membrane. We use a high-optical-quality and thin (∼300 nm) diamond membrane, supported by a polycrystalline diamond frame, to realize fully suspended two-dimensional photonic crystal cavities with a high theoretical quality factor of ∼8 × 106 and a relatively small mode volume of ∼2(λ/n)3. The cavities are fabricated in the membrane using electron-beam lithography and vertical dry etching. We observe cavity resonances over a wide wavelength range spanning the telecommunication O- and S-bands (1360–1470 nm) with Q factors of up to ∼1800. Our method paves the way for on-chip diamond nanophotonic applications in the telecommunication-wavelength range.

Diamond membrane production: The critical role of radicals in the non-contact electrochemical etching of sp2 carbon

Sub-micrometre single crystal diamond membranes are of huge importance for next generation optical, quantum and electronic device applications. Electrochemical etching has proven a critical step in the production of such membranes. Etching is used to selectively remove a very thin layer of sub-surface sp2 carbon, prepared by ion implantation in bulk diamond, releasing the diamond membrane. Due to the nanosized dimensions, etching is typically carried out using non-contact electrochemistry in low conductivity solutions (bipolar arrangement) which whilst effective, results in extremely slow etch rates. In this work, a new method of non-contact electrochemical etching is presented which uses high conductivity, high concentration, fully dissociated aqueous electrolytes. Careful choice of the electrolyte anion results in significant improvements in the sp2 carbon etch rate. In particular, we show both chloride and sulfate electrolytes increase etch rates significantly (up to × 40 for sulfate) compared to our measurements using the current state-of-the-art solutions and methodologies. Electron paramagnetic resonance experiments, recorded after the electrode potential has been switched off, reveal sizeable hydroxyl radical concentrations at timescales > 107 longer than their lifetime (≤μs). These measurements highlight the importance of electrochemically initiated, solution chemistry radical generation and regeneration pathways in high concentration sulfate and chloride solutions for nano-etching applications.

A cavity-based optical antenna for color centers in diamond

An efficient atom–photon interface is a key requirement for the integration of solid-state emitters, such as color centers in diamond, into quantum technology applications. As other solid-state emitters, however, their emission into free space is severely limited due to the high refractive index of the bulk host crystal. In this work, we present a planar optical antenna based on two silver mirrors coated on a thin single crystal diamond membrane, forming a planar Fabry–Pérot cavity that improves the photon extraction from single tin vacancy (SnV) centers and their coupling to an excitation laser. Upon numerical optimization of the structure, we find theoretical enhancements in the collectible photon rate by a factor of 60 as compared to the bulk case. As a proof-of-principle demonstration, we fabricate single crystal diamond membranes with sub-μm thickness and create SnV centers by ion implantation. Employing off-resonant excitation, we show a sixfold enhancement of the collectible photon rate, yielding up to half a million photons per second from a single SnV center. At the same time, we observe a significant reduction of the required excitation power in accordance with theory, demonstrating the functionality of the cavity as an optical antenna. Due to its planar design, the antenna simultaneously provides similar enhancements for a large number of emitters inside the membrane. Furthermore, the monolithic structure provides high mechanical stability and straightforwardly enables operation under cryogenic conditions as required in most spin–photon interface implementations.

Nanofabrication of high Q, transferable diamond resonators.

Advancement of diamond based photonic circuitry requires robust fabrication protocols of key components - including diamond resonators and cavities. Here, we present 1D (nanobeam) photonic crystal cavities generated from single crystal diamond membranes utilising a metallic tungsten layer as a restraining, conductive and removable hard mask. The use of tungsten instead of a more conventional silicon oxide layer enables good repeatability and reliability of the fabrication procedures. The process yields high quality diamond cavities with quality factors (Q-factors) approaching 1 × 104. Finally, we show that the cavities can be picked up and transferred onto a trenched substrate to realise fully suspended diamond cavities. Our fabrication process demonstrates the capability of diamond membranes as modular components for broader diamond based quantum photonic circuitry.

Fabrication and Characterization of Single-Crystal Diamond Membranes for Quantum Photonics with Tunable Microcavities.

The development of quantum technologies is one of the big challenges in modern research. A crucial component for many applications is an efficient, coherent spin–photon interface, and coupling single-color centers in thin diamond membranes to a microcavity is a promising approach. To structure such micrometer thin single-crystal diamond (SCD) membranes with a good quality, it is important to minimize defects originating from polishing or etching procedures. Here, we report on the fabrication of SCD membranes, with various diameters, exhibiting a low surface roughness down to 0.4 nm on a small area scale, by etching through a diamond bulk mask with angled holes. A significant reduction in pits induced by micromasking and polishing damages was accomplished by the application of alternating Ar/Cl2 + O2 dry etching steps. By a variation of etching parameters regarding the Ar/Cl2 step, an enhanced planarization of the surface was obtained, in particular, for surfaces with a higher initial surface roughness of several nanometers. Furthermore, we present the successful bonding of an SCD membrane via van der Waals forces on a cavity mirror and perform finesse measurements which yielded values between 500 and 5000, depending on the position and hence on the membrane thickness. Our results are promising for, e.g., an efficient spin–photon interface.

Controlled Doping of GeV and SnV Color Centers in Diamond Using Chemical Vapor Deposition.

Group IV color centers in diamond (Si, Ge, Sn, and Pb) have recently emerged as promising candidates for realization of scalable quantum photonics. However, their synthesis in nanoscale diamond is still in its infancy. In this work we demonstrate controlled synthesis of selected group IV defects (Ge and Sn) into nanodiamonds and nanoscale single crystal diamond membranes by microwave plasma chemical vapor deposition. We take advantage of inorganic salts to prepare the chemical precursors that contain the required ions that are then incorporated into the growing diamond. Photoluminescence measurements confirm that the selected group IV emitters are present in the diamond without degrading its structural quality. Our results are important to expand the versatile synthesis of color centers in diamond.

Electrical excitation and charge-state conversion of silicon vacancy color centers in single-crystal diamond membranes

The silicon-vacancy (SiV) color center in diamond has recently emerged as a promising qubit for quantum photonics. However, the electrical control and excitation of the SiV centers are challenging due to the low density of free carriers in doped diamond. Here, we realize electrical excitation of SiV centers in a single-crystal diamond membrane, which is promising for scalable photonic architectures. We further demonstrate electrical switching of the charge states of the SiV centers by applying a forward bias voltage to the fabricated diamond-membrane devices and identify the position of the SiV−/SiV0 charge transition level. Our findings provide a perspective toward electrical triggering of color centers in diamond and accelerate the development of scalable quantum nanophotonic technologies.

Cavity-Enhanced Raman Scattering for In Situ Alignment and Characterization of Solid-State Microcavities

We report cavity-enhanced Raman scattering from a single-crystal diamond membrane embedded in a highly miniaturized fully-tunable Fabry-P\'{e}rot cavity. The Raman intensity is enhanced 58.8-fold compared to the corresponding confocal measurement. The strong signal amplification results from the Purcell effect. We show that the cavity-enhanced Raman scattering can be harnessed as a narrowband, high-intensity, internal light-source. The Raman process can be triggered in a simple way by using an optical excitation frequency outside the cavity stopband and is independent of the lateral positioning of the cavity mode with respect to the diamond membrane. The strong Raman signal emerging from the cavity output facilitates in situ mode-matching of the cavity mode to single-mode collection optics; it also represents a simple way of measuring the dispersion and spatial intensity-profile of the cavity modes. The optimization of the cavity performance via the strong Raman process is extremely helpful in achieving efficient cavity-outcoupling of the relatively weak emission of single color-centers such as nitrogen-vacancy centers in diamond or rare-earth ions in crystalline hosts with low emitter density.

Spin measurements of NV centers coupled to a photonic crystal cavity

Nitrogen-vacancy (NV) centers feature outstanding properties such as a spin coherence time of up to 1 s as well as a level structure offering the possibility to initialize, coherently manipulate, and optically read-out the spin degree of freedom of the ground state. However, only about 3% of their photon emission is channeled into the zero phonon line (ZPL), limiting both the rate of indistinguishable single photons and the signal-to-noise ratio (SNR) of coherent spin-photon interfaces. We here report on the enhancement of the SNR of the optical spin read-out achieved by tuning the mode of a two-dimensional photonic crystal (PhC) cavity into resonance with the NV-ZPL. PhC cavities are fabricated by focused ion beam milling in thin reactive ion etched ultrapure single crystal diamond membranes featuring modes with Q-factors of up to 8250 at mode volumes below one cubic wavelength. NV centers are produced in the cavities in a controlled fashion by a high resolution atomic force microscope implantation technique. On cavity resonance, we observe a lifetime shortening from 9.0 ns to 8.0 ns as well as an enhancement of the ZPL emission by almost one order of magnitude. Although on resonance the collection efficiency of ZPL photons and the spin-dependent fluorescence contrast are reduced, the SNR of the optical spin read-out is almost tripled for the cavity-coupled NV centers.

Bottom up engineering of single crystal diamond membranes with germanium vacancy color centers

Color centers in diamond have garnered significant attention for applications in integrated quantum photonics. The availability of thin (∼ hundred of nanometers) diamond membranes is paramount to achieve this goal. In this paper, we describe in detail a robust, reproducible and cost effective fabrication method that enables engineering high quality thin diamond membranes with uniform distribution of germanium vacancies employing microwave plasma chemical vapor deposition. We use a combination of different germanium precursors for homogeneous doping of the membranes to increase the probability of germanium incorporation into the diamond lattice. Our fabrication methodology can be further extended to implementation of other color centers in thin diamond membranes and be used for engineering quantum photonic devices.

Diamond photonics platform based on silicon vacancy centers in a single-crystal diamond membrane and a fiber cavity

We realize a potential platform for an efficient spin-photon interface, namely negatively-charged silicon-vacancy centers in a diamond membrane coupled to the mode of a fully-tunable, fiber-based, optical resonator. We demonstrate that introducing the thin ($\sim 200 \, \text{nm}$), single crystal diamond membrane into the mode of the resonator does not change the cavity properties, which is one of the crucial points for an efficient spin-photon interface. In particular, we observe constantly high Finesse values of up to $3000$ and a linear dispersion in the presence of the membrane. We observe cavity-coupled fluorescence froman ensemble of SiV$^{-}$ centers with an enhancement factor of $\sim 1.9$. Furthermore from our investigations we extract the ensemble absorption and extrapolate an absorption cross section of $(2.9 \, \pm \, 2) \, \cdot \, 10^{-12} \, \text{cm}^{2}$ for a single SiV$^{-}$ center, much higher than previously reported.

Single Crystal Diamond Membranes and Photonic Resonators Containing Germanium Vacancy Color Centers

Single crystal diamond membranes that host optically active emitters are highly attractive components for integrated quantum nanophotonics. In this work we demonstrate bottom-up synthesis of single crystal diamond membranes containing germanium vacancy (GeV) color centers. We employ a lift-off technique to generate the membranes and perform chemical vapor deposition in the presence of a germanium source to realize the in situ doping. Finally, we show that these membranes are suitable for engineering of photonic resonators such as microdisk cavities with quality factors of ∼1500. The robust and scalable approach to engineer single crystal diamond membranes containing emerging color centers is a promising pathway for the realization of diamond integrated quantum nanophotonic circuits on a chip.

Single crystal diamond membranes for nanoelectronics.

Single crystal, nanoscale diamond membranes are highly sought after for a variety of applications including nanophotonics, nanoelectronics and quantum information science. However, so far, the availability of conductive diamond membranes has remained an unreachable goal. In this work we present a complete nanofabrication methodology for engineering high aspect ratio, electrically active single crystal diamond membranes. The membranes have large lateral directions, exceeding ∼500 × 500 μm2 and are only several hundreds of nanometers thick. We further realize vertical single crystal p-n junctions made from the diamond membranes that exhibit onset voltages of ∼10 V and a current of several mA. Moreover, we deterministically introduce optically active color centers into the membranes, and demonstrate for the first time a single crystal nanoscale diamond LED. The robust and scalable approach to engineer the electrically active single crystal diamond membranes offers new pathways for advanced nanophotonic, nanoelectronic and optomechanical devices employing diamond.

Cell micro-irradiation with MeV protons counted by an ultra-thin diamond membrane

We report the development of thin single crystal diamond membranes suitable for dose control in targeted cell irradiation experiments with a proton microbeam. A specific design was achieved to deliver single protons with a hit detection efficiency approaching 100%. The membranes have thicknesses between 1.8 and 3 μm and are used as vacuum windows on the microbeam line. The impact of these transmission detectors on the microbeam spot size is estimated by Monte-Carlo simulations, indicating that a beam lateral resolution below 2 μm is achieved. This is confirmed by experiments showing the accumulation online of X-ray Repair Cross-Complementing protein 1 (XRCC1)-Green Fluorescent Protein (GFP) at DNA damaged sites in living cells.

Fabrication of a single sub-micron pore spanning a single crystal (100) diamond membrane and impact on particle translocation

The fabrication of sub-micron pores in single crystal diamond membranes, which span the entirety of the membrane, is described for the first time, and the translocation properties of polymeric particles through the pore investigated. The pores are produced using a combination of laser micromachining to form the membrane and electron beam induced etching to form the pore. Single crystal diamond as the membrane material, has the advantages of chemical stability and durability, does not hydrate and swell, has outstanding electrical properties that facilitate fast, low noise current-time measurements and is optically transparent for combined optical-conductance sensing. The resulting pores are characterized individually using both conductance measurements, employing a microcapillary electrochemical setup, and electron microscopy. Proof-of-concept experiments to sense charged polystyrene particles as they are electrophoretically driven through a single diamond pore are performed, and the impact of this new pore material on particle translocation is explored. These findings reveal the potential of diamond as a platform for pore-based sensing technologies and pave the way for the fabrication of single nanopores which span the entirety of a diamond membrane.

Channeling STIM analysis of radiation damage in single crystal diamond membrane

The use of focused ion beam transmission channeling patterns to monitor the damage creation process in thin diamond single crystal membrane is described. A 0.8MeV proton beam from the Ruđer Bošković Institute nuclear microprobe was used to perform Channeling Scanning Transmission Ion Microscopy (CSTIM) measurements. CSTIM was used instead of RBS channeling because of (several orders of magnitude) lower damage done to the sample during the measurements. Damage was introduced in selected areas by 15MeV carbon beam in range of fluences 3·1015–2·1017ions/cm2. Contrary to Ion Beam Induced Charge (IBIC), CSTIM is shown to be sensitive to the large fluences of ion beam radiation. Complementary studies of both IBIC and CSTIM are presented to show that very high fluence range can be covered by these two microprobe techniques, providing much wider information about the diamond radiation hardness. In addition micro Raman measurements were performed and the height of the GR 1 peak was correlated to the ion beam fluence.