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Showing papers on "Diamond published in 2014"


Journal ArticleDOI
TL;DR: A concise overview of the basic properties of diamond, from synthesis to electronic and magnetic properties of embedded NV centers, and how single NV centers can be harnessed for nanoscale sensing are described, including the physical quantities that may be detected, expected sensitivities, and the most common measurement protocols.
Abstract: Crystal defects in diamond have emerged as unique objects for a variety of applications, both because they are very stable and because they have interesting optical properties. Embedded in nanocrystals, they can serve, for example, as robust single-photon sources or as fluorescent biomarkers of unlimited photostability and low cytotoxicity. The most fascinating aspect, however, is the ability of some crystal defects, most prominently the nitrogen-vacancy (NV) center, to locally detect and measure a number of physical quantities, such as magnetic and electric fields. This metrology capacity is based on the quantum mechanical interactions of the defect's spin state. In this review, we introduce the new and rapidly evolving field of nanoscale sensing based on single NV centers in diamond. We give a concise overview of the basic properties of diamond, from synthesis to electronic and magnetic properties of embedded NV centers. We describe in detail how single NV centers can be harnessed for nanoscale sensing,...

1,232 citations


Journal ArticleDOI
12 Jun 2014-Nature
TL;DR: The direct synthesis of nt-diamond with an average twin thickness of ∼5 nm is reported, using a precursor of onion carbon nanoparticles at high pressure and high temperature, and the observation of a new monoclinic crystalline form of diamond coexisting with nt -diamond is observed.
Abstract: Nanotwinned diamond synthesized with onion carbon nanoparticles as precursors has much higher hardness and thermal stability than natural diamond; its enhanced hardness is due to the reduced size of its twin structures. Even diamond has its limitations when used in tools to cut and shape the hardest of materials. Materials scientists have therefore sought to synthesize materials that are harder than natural diamond, preferably with increased thermal stability. In air, natural diamond starts to oxidize at about 800 °C, leading to severe wear at high temperatures. Attempts to increase the hardness of diamond by decreasing its grain size have succeeded, but at the cost of even poorer thermal stability. Yongjun Tian and colleagues report the synthesis of synthetic diamond that is both ultrahard and has a dramatically enhanced thermal stability with an oxidization temperature of more than 1,000 °C. The material is synthesized using onion carbon nanoparticles as precursors and owes its enhanced hardness to a nanoscale structure consisting not of tiny grains, but of crystal 'twins' — domains of the crystal lattice related by symmetry. This result, which follows similar success with nanotwinned cubic boron nitride, suggests a general approach to making new, advanced carbon-based materials with exceptional properties. Although diamond is the hardest material for cutting tools, poor thermal stability has limited its applications, especially at high temperatures. Simultaneous improvement of the hardness and thermal stability of diamond has long been desirable. According to the Hall−Petch effect1,2, the hardness of diamond can be enhanced by nanostructuring (by means of nanograined and nanotwinned microstructures), as shown in previous studies3,4,5,6,7. However, for well-sintered nanograined diamonds, the grain sizes are technically limited to 10−30 nm (ref. 3), with degraded thermal stability4 compared with that of natural diamond. Recent success in synthesizing nanotwinned cubic boron nitride (nt-cBN) with a twin thickness down to ∼3.8 nm makes it feasible to simultaneously achieve smaller nanosize, ultrahardness and superior thermal stability5. At present, nanotwinned diamond (nt-diamond) has not been fabricated successfully through direct conversions of various carbon precursors3,6,7 (such as graphite, amorphous carbon, glassy carbon and C60). Here we report the direct synthesis of nt-diamond with an average twin thickness of ∼5 nm, using a precursor of onion carbon nanoparticles at high pressure and high temperature, and the observation of a new monoclinic crystalline form of diamond coexisting with nt-diamond. The pure synthetic bulk nt-diamond material shows unprecedented hardness and thermal stability, with Vickers hardness up to ∼200 GPa and an in-air oxidization temperature more than 200 °C higher than that of natural diamond. The creation of nanotwinned microstructures offers a general pathway for manufacturing new advanced carbon-based materials with exceptional thermal stability and mechanical properties.

546 citations


Journal ArticleDOI
TL;DR: The optical and spin resonances of the NV- center are observed under hydrostatic pressures up to 60 GPa and motivate powerful new techniques to measure pressure and image high-pressure magnetic and electric phenomena.
Abstract: The negatively charged nitrogen-vacancy (NV-) center in diamond has realized new frontiers in quantum technology. Here, the optical and spin resonances of the NV- center are observed under hydrostatic pressures up to 60 GPa. Our results motivate powerful new techniques to measure pressure and image high-pressure magnetic and electric phenomena. Additionally, molecular orbital analysis and semiclassical calculations provide insight into the effects of compression on the electronic orbitals of the NV- center.

365 citations


Journal ArticleDOI
TL;DR: In this article, a spin-based spin-strain interaction with a single-crystal diamond resonator has been studied and quantitatively characterized with axial and transverse strain sensitivities of the ground state spin.
Abstract: The development of hybrid quantum systems is central to the advancement of emerging quantum technologies, including quantum information science and quantum-assisted sensing. The recent demonstration of high-quality single-crystal diamond resonators has led to significant interest in a hybrid system consisting of nitrogen-vacancy centre spins that interact with the resonant phonon modes of a macroscopic mechanical resonator through crystal strain. However, the nitrogen-vacancy spin-strain interaction has not been well characterized. Here, we demonstrate dynamic, strain-mediated coupling of the mechanical motion of a diamond cantilever to the spin of an embedded nitrogen-vacancy centre. Via quantum control of the spin, we quantitatively characterize the axial and transverse strain sensitivities of the nitrogen-vacancy ground-state spin. The nitrogen-vacancy centre is an atomic scale sensor and we demonstrate spin-based strain imaging with a strain sensitivity of 3 × 10(-6) strain Hz(-1/2). Finally, we show how this spin-resonator system could enable coherent spin-phonon interactions in the quantum regime.

363 citations


Journal ArticleDOI
TL;DR: This work reports on single electronic spins coupled to the motion of mechanical resonators by a novel mechanism based on crystal strain, consisting of single-crystal diamond cantilevers with embedded nitrogen-vacancy center spins, and determines the unknown spin-strain coupling constants.
Abstract: We report on single electronic spins coupled to the motion of mechanical resonators by a novel mechanism based on crystal strain. Our device consists of single-crystal diamond cantilevers with embedded nitrogen-vacancy center spins. Using optically detected electron spin resonance, we determine the unknown spin-strain coupling constants and demonstrate that our system resides well within the resolved sideband regime. We realize coupling strengths exceeding 10 MHz under mechanical driving and show that our system has the potential to reach strong coupling. Our novel hybrid system forms a resource for future experiments on spin-based cantilever cooling and coherent spin-oscillator coupling.

328 citations


Journal ArticleDOI
TL;DR: In this article, the authors used an ensemble of 1e11 defect centers for sensing and achieved a photon shot noise limited field sensitivity of 0.9 pT/Hz^(1/2) at room temperature with an effective sensor volume of 8.5e-4 mm^3.
Abstract: Diamond defect centers are promising solid state magnetometers. Single centers allow for high spatial resolution field imaging but are limited in their magnetic field sensitivity to around 10 nT/Hz^(1/2) at room-temperature. Using defect center ensembles sensitivity can be scaled as N^(1/2) when N is the number of defects. In the present work we use an ensemble of 1e11 defect centers for sensing. By carefully eliminating all noise sources like laser intensity fluctuations, microwave amplitude and phase noise we achieve a photon shot noise limited field sensitivity of 0.9 pT/Hz^(1/2) at room-temperature with an effective sensor volume of 8.5e-4 mm^3. The smallest field we measured with our device is 100 fT. While this denotes the best diamond magnetometer sensitivity so far, further improvements using decoupling sequences and material optimization could lead to fT/Hz^(1/2) sensitivity.

327 citations


Journal ArticleDOI
TL;DR: In this article, an optical parametric oscillator in the telecom wavelength range is realized in a diamond system consisting of a ring resonator coupled to a diamond waveguide, and threshold powers as low as 20mW are measured and up to 20 new wavelengths are generated from a single-frequency pump laser.
Abstract: An optical parametric oscillator in the telecom wavelength range is realized in a diamond system consisting of a ring resonator coupled to a diamond waveguide. Threshold powers as low as 20 mW are measured and up to 20 new wavelengths are generated from a single-frequency pump laser. Despite progress towards integrated diamond photonics1,2,3,4, studies of optical nonlinearities in diamond have been limited to Raman scattering in bulk samples5. Diamond nonlinear photonics, however, could enable efficient, in situ frequency conversion of single photons emitted by diamond's colour centres6,7, as well as stable and high-power frequency microcombs8 operating at new wavelengths. Both of these applications depend crucially on efficient four-wave mixing processes enabled by diamond's third-order nonlinearity. Here, we have realized a diamond nonlinear photonics platform by demonstrating optical parametric oscillation via four-wave mixing using single-crystal ultrahigh-quality-factor (1 × 106) diamond ring resonators operating at telecom wavelengths. Threshold powers as low as 20 mW are measured, and up to 20 new wavelengths are generated from a single-frequency pump laser. We also report the first measurement of the nonlinear refractive index due to the third-order nonlinearity in diamond at telecom wavelengths.

312 citations


Journal ArticleDOI
TL;DR: B batch fabrication and mechanical measurements of single-crystal diamond cantilevers with thickness down to 85’nm, thickness uniformity better than 20 nm and lateral dimensions up to 240 μm are demonstrated, which could directly improve existing force and mass sensors by a simple substitution of resonator material.
Abstract: Single-crystal diamond nanomechanical resonators are intricate to fabricate, but expected to demonstrate large-quality factors. Here, the authors achieve batch fabrication of such resonators, demonstrating quality factors exceeding one million at room temperature.

302 citations


Journal ArticleDOI
TL;DR: The SiV- center is established as a solid-state spin-photon interface andHyperfine structure is observed in CPT measurements with the 29Si isotope which allows access to nuclear spin.
Abstract: The spin on a silicon defect in diamond can be prepared in a coherent quantum state, a promising sign that it could encode information in a quantum internet.

280 citations


Journal ArticleDOI
TL;DR: A recent review of diamond nanophotonics can be found in this paper, where the authors highlight the recent achievements in the field of diamond nano-graphs and convey a roadmap for future experiments and technological advancements.
Abstract: The burgeoning field of nanophotonics has grown to be a major research area, primarily because of the ability to control and manipulate single quantum systems (emitters) and single photons on demand For many years studying nanophotonic phenomena was limited to traditional semiconductors (including silicon and GaAs) and experiments were carried out predominantly at cryogenic temperatures In the last decade, however, diamond has emerged as a new contender to study photonic phenomena at the nanoscale Offering plethora of quantum emitters that are optically active at room temperature and ambient conditions, diamond has been exploited to demonstrate super-resolution microscopy and realize entanglement, Purcell enhancement and other quantum and classical nanophotonic effects Elucidating the importance of diamond as a material, this review will highlight the recent achievements in the field of diamond nanophotonics, and convey a roadmap for future experiments and technological advancements

273 citations


Journal ArticleDOI
TL;DR: The growth and characterization of novel large area h-BN hexagons using highly electropolished Cu substrate under atmospheric pressure CVD conditions are reported and it is found that the nucleation density ofh-BN is significantly reduced while domain sizes increase.
Abstract: Hexagonal-boron nitride (h-BN) or “white graphene” has many outstanding properties including high thermal conductivity, high mechanical strength, chemical inertness, and high electrical resistance, which open up a wide range of applications such as thermal interface material, protective coatings, and dielectric in nanoelectronics that easily exceed the current advertised benefits pertaining to the graphene-based applications. The development of h-BN films using chemical vapor deposition (CVD) has thus far led into nucleation of triangular or asymmetric diamond shapes on different metallic surfaces. Additionally, the average size of the triangular domains has remained relatively small (∼0.5 μm2) leading to a large number of grain boundaries and defects. While the morphology of Cu surfaces for CVD-grown graphene may have impacts on the nucleation density, domain sizes, thickness, and uniformity, the effects of the decreased roughness of Cu surface to develop h-BN films are unknown. Here, we report the growt...

Journal ArticleDOI
TL;DR: It is shown that isolated diamond nanoparticles as small as 1.6 nm, comprising only ∼400 carbon atoms, are capable of housing stable photoluminescent colour centres, namely the silicon vacancy (SiV), and fluorescence from SiVs is stable over time, and few or only single colour centres are found per nanocrystal.
Abstract: Diamond nanoparticles containing only about 400 atoms emit bright fluorescence due to silicon vacancy defects.

Journal ArticleDOI
TL;DR: In this paper, the authors adapted angled-etching techniques, previously developed for realization of diamond nanomechanical resonators, to fabricate racetrack resonators and photonic crystal cavities in bulk single-crystal diamond.
Abstract: Single-crystal diamond, with its unique optical, mechanical and thermal properties, has emerged as a promising material with applications in classical and quantum optics. However, the lack of heteroepitaxial growth and scalable fabrication techniques remains the major limiting factors preventing more wide-spread development and application of diamond photonics. In this work, we overcome this difficulty by adapting angled-etching techniques, previously developed for realization of diamond nanomechanical resonators, to fabricate racetrack resonators and photonic crystal cavities in bulk single-crystal diamond. Our devices feature large optical quality factors, in excess of 10 5 , and operate over a wide wavelength

Journal ArticleDOI
TL;DR: This work demonstrates a method of magnetic resonance imaging with single nuclear-spin sensitivity under ambient conditions that realizes a new platform for probing novel materials, monitoring chemical reactions, and manipulation of complex systems on surfaces at a quantum level.
Abstract: We demonstrate a method of magnetic resonance imaging with single nuclear-spin sensitivity under ambient conditions. Our method employs isolated electronic-spin quantum bits (qubits) as magnetic resonance “reporters” on the surface of high purity diamond. These spin qubits are localized with nanometer-scale uncertainty, and their quantum state is coherently manipulated and measured optically via a proximal nitrogen-vacancy color center located a few nanometers below the diamond surface. This system is then used for sensing, coherent coupling, and imaging of individual proton spins on the diamond surfacewith angstrom resolution. Our approach may enable direct structural imaging of complex molecules that cannot be accessed from bulk studies. It realizes a new platform for probing novel materials, monitoring chemical reactions, and manipulation of complex systems on surfaces at a quantum level.

Journal ArticleDOI
TL;DR: In this article, the vibronic structure of the spin-triplet optical transition in diamond nitrogen-vacancy (NV) centers is described using accurate first-principles methods based on hybrid functionals.
Abstract: In this work we present theoretical calculations and analysis of the vibronic structure of the spin-triplet optical transition in diamond nitrogen-vacancy (NV) centres. The electronic structure of the defect is described using accurate first-principles methods based on hybrid functionals. We devise a computational methodology to determine the coupling between electrons and phonons during an optical transition in the dilute limit. As a result, our approach yields a smooth spectral function of electron–phonon coupling and includes both quasi-localized and bulk phonons on equal footings. The luminescence lineshape is determined via the generating function approach. We obtain a highly accurate description of the luminescence band, including all key parameters such as the Huang–Rhys factor, the Debye–Waller factor, and the frequency of the dominant phonon mode. More importantly, our work provides insight into the vibrational structure of NV centres, in particular the role of local modes and vibrational resonances. In particular, we find that the pronounced mode at 65 meV is a vibrational resonance, and we quantify localization properties of this mode. These excellent results for the benchmark diamond (NV) centre provide confidence that the procedure can be applied to other defects, including alternative systems that are being considered for applications in quantum information processing.

Journal Article
TL;DR: In this paper, a three-qubit quantum error correction protocol was proposed to demonstrate the robustness of the encoded state against applied errors, paving the way towards extended quantum networks and surface-code quantum computing based on multi-qubits nodes.
Abstract: Quantum registers of nuclear spins coupled to electron spins of individual solid-state defects are a promising platform for quantum information processing. Pioneering experiments selected defects with favourably located nuclear spins with particularly strong hyperfine couplings. To progress towards large-scale applications, larger and deterministically available nuclear registers are highly desirable. Here, we realize universal control over multi-qubit spin registers by harnessing abundant weakly coupled nuclear spins. We use the electron spin of a nitrogen-vacancy centre in diamond to selectively initialize, control and read out carbon-13 spins in the surrounding spin bath and construct high-fidelity single- and two-qubit gates. We exploit these new capabilities to implement a three-qubit quantum-error-correction protocol and demonstrate the robustness of the encoded state against applied errors. These results transform weakly coupled nuclear spins from a source of decoherence into a reliable resource, paving the way towards extended quantum networks and surface-code quantum computing based on multi-qubit nodes.

Journal ArticleDOI
TL;DR: This work's method of combining nitrogen delta-doping growth and nanoscale depth imaging paves a way for studying spin noise present in diverse material surfaces.
Abstract: Sensitive nanoscale magnetic resonance imaging of target spins using nitrogen-vacancy (NV) centers in diamond requires a quantitative understanding of dominant noise at the surface. We probe this noise by applying dynamical decoupling to shallow NVs at calibrated depths. Results support a model of NV dephasing by a surface bath of electronic spins having a correlation rate of 200 kHz, much faster than that of the bulk N spin bath. Our method of combining nitrogen delta-doping growth and nanoscale depth imaging paves a way for studying spin noise present in diverse material surfaces.

Journal ArticleDOI
TL;DR: Measurements reveal a spin-state purity approaching unity in the excited state, highlighting the potential of the silicon-vacancy centre as an efficient spin-photon quantum interface.
Abstract: Colour centres in diamond have emerged as versatile tools for solid-state quantum technologies ranging from quantum information to metrology, where the nitrogen-vacancy centre is the most studied to date. Recently, this toolbox has expanded to include novel colour centres to realize more efficient spin-photon quantum interfaces. Of these, the silicon-vacancy centre stands out with highly desirable photonic properties. The challenge for utilizing this centre is to realize the hitherto elusive optical access to its electronic spin. Here we report spin-tagged resonance fluorescence from the negatively charged silicon-vacancy centre. Our measurements reveal a spin-state purity approaching unity in the excited state, highlighting the potential of the centre as an efficient spin-photon quantum interface.

Journal ArticleDOI
TL;DR: It is shown that defects in cubic diamond provide an explanation for the characteristic d-spacings and reflections reported for lonsdaleite and point to the need for re-evaluating the interpretations of many londaleite-related fundamental and applied studies.
Abstract: Lonsdaleite, also called hexagonal diamond, has been widely used as a marker of asteroidal impacts. It is thought to play a central role during the graphite-to-diamond transformation, and calculations suggest that it possesses mechanical properties superior to diamond. However, despite extensive efforts, lonsdaleite has never been produced or described as a separate, pure material. Here we show that defects in cubic diamond provide an explanation for the characteristic d-spacings and reflections reported for lonsdaleite. Ultrahigh-resolution electron microscope images demonstrate that samples displaying features attributed to lonsdaleite consist of cubic diamond dominated by extensive {113} twins and {111} stacking faults. These defects give rise to nanometre-scale structural complexity. Our findings question the existence of lonsdaleite and point to the need for re-evaluating the interpretations of many lonsdaleite-related fundamental and applied studies.

Journal ArticleDOI
TL;DR: Measurements of spin relaxation times on very shallow nitrogen-vacancy centers in high-purity diamond single crystals support the atomistic picture where impurities are associated with the top carbon layers, and not with terminating surface atoms or adsorbate molecules.
Abstract: We present measurements of spin relaxation times (T1, T1ρ, T2) on very shallow (≲5 nm) nitrogenvacancy centers in high-purity diamond single crystals. We find a reduction of spin relaxation times up to 30 times compared to bulk values, indicating the presence of ubiquitous magnetic impurities associated with the surface. Our measurements yield a density of 0.01–0.1μB=nm 2 and a characteristic correlation time of 0.28(3) ns of surface states, with little variation between samples and chemical surface terminations. A low temperature measurement further confirms that fluctuations are thermally activated. The data support the atomistic picture where impurities are associated with the top carbon layers, and not with terminating surface atoms or adsorbate molecules. The low spin density implies that the presence of a single surface impurity is sufficient to cause spin relaxation of a shallow nitrogen-vacancy center.

Journal ArticleDOI
TL;DR: In this article, a microwave plasma-assisted chemical vapor deposition diamond growth technique on (111)-oriented substrates, which yields perfect alignment (94% ± 2%) of as-grown NV centers along a single crystallographic direction.
Abstract: Synthetic diamond production is a key to the development of quantum metrology and quantum information applications of diamond. The major quantum sensor and qubit candidate in diamond is the nitrogen-vacancy (NV) color center. This lattice defect comes in four different crystallographic orientations leading to an intrinsic inhomogeneity among NV centers, which is undesirable in some applications. Here, we report a microwave plasma-assisted chemical vapor deposition diamond growth technique on (111)-oriented substrates, which yields perfect alignment (94% ± 2%) of as-grown NV centers along a single crystallographic direction. In addition, clear evidence is found that the majority (74% ± 4%) of the aligned NV centers were formed by the nitrogen being first included in the (111) growth surface and then followed by the formation of a neighboring vacancy on top. The achieved homogeneity of the grown NV centers will tremendously benefit quantum information and metrology applications.

Journal ArticleDOI
TL;DR: In this article, the state-of-the-art and future perspective of silicon and diamond isotope engineering for development of quantum information processing devices is described, where the authors describe the current state of the art and future perspectives of silicon-and diamond-isotope engineering.
Abstract: Some of the stable isotopes of silicon and carbon have zero nuclear spin, whereas many of the other elements that constitute semiconductors consist entirely of stable isotopes that have nuclear spins. Silicon and diamond crystals composed of nuclear-spin-free stable isotopes (28Si, 30Si, or 12C) are considered to be ideal host matrixes to place spin quantum bits (qubits) for quantum-computing and -sensing applications, because their coherent properties are not disrupted thanks to the absence of host nuclear spins. The present paper describes the state-of-the-art and future perspective of silicon and diamond isotope engineering for development of quantum information-processing devices.

Journal ArticleDOI
TL;DR: In this paper, the nitrogen-vacancy (NV) centers were created by shallow ion implantation followed by a slow, nanometer-by-nanometer removal of diamond material using oxidative etching in air.
Abstract: We present nanoscale nuclear magnetic resonance (NMR) measurements performed with nitrogen-vacancy (NV) centers located down to about 2 nm from the diamond surface. NV centers were created by shallow ion implantation followed by a slow, nanometer-by-nanometer removal of diamond material using oxidative etching in air. The close proximity of NV centers to the surface yielded large 1H NMR signals of up to 3.4 μT-rms, corresponding to ∼330 statistically polarized or ∼10 fully polarized proton spins in a (1.8 nm)3 detection volume.

Journal ArticleDOI
TL;DR: In this article, a highly stable Al2O3 gate oxide on a C-H bonded channel of diamond, high-temperature, and highvoltage metal-oxide-semiconductor field effect transistor (MOSFET) has been realized.
Abstract: By forming a highly stable Al2O3 gate oxide on a C-H bonded channel of diamond, high-temperature, and high-voltage metal-oxide-semiconductor field-effect transistor (MOSFET) has been realized. From room temperature to 400 °C (673 K), the variation of maximum drain-current is within 30% at a given gate bias. The maximum breakdown voltage (VB) of the MOSFET without a field plate is 600 V at a gate-drain distance (LGD) of 7 μm. We fabricated some MOSFETs for which VB/LGD > 100 V/μm. These values are comparable to those of lateral SiC or GaN FETs. The Al2O3 was deposited on the C-H surface by atomic layer deposition (ALD) at 450 °C using H2O as an oxidant. The ALD at relatively high temperature results in stable p-type conduction and FET operation at 400 °C in vacuum. The drain current density and transconductance normalized by the gate width are almost constant from room temperature to 400 °C in vacuum and are about 10 times higher than those of boron-doped diamond FETs.

Journal ArticleDOI
TL;DR: Using high purity nanodiamonds, this work achieves spin coherence comparable to that in bulk diamond, and nano-resolution magnetometry is achieved.
Abstract: The photoluminescent properties of electron spins at nitrogen–vacancy (NV) centres are promising for use in quantum information and magnetometry. It is now shown that the coherence times of NV centres in nanodiamonds can be engineered to be comparable to those of bulk diamond.

Journal ArticleDOI
TL;DR: An efficient method that can automatically explore the surface structures using structure swarm intelligence is developed and its application to a simple diamond surface reveals an unexpected surface reconstruction featuring self-assembled carbon nanotubes arrays.
Abstract: Surfaces of semiconductors are crucially important for electronics, especially when the devices are reduced to the nanoscale. However, surface structures are often elusive, impeding greatly the engineering of devices. Here we develop an efficient method that can automatically explore the surface structures using structure swarm intelligence. Its application to a simple diamond (100) surface reveals an unexpected surface reconstruction featuring self-assembled carbon nanotubes arrays. Such a surface is energetically competitive with the known dimer structure under normal conditions, but it becomes more favourable under a small compressive strain or at high temperatures. The intriguing covalent bonding between neighbouring tubes creates a unique feature of carrier kinetics (that is, one dimensionality of hole states, while two dimensionality of electron states) that could lead to novel design of superior electronics. Our findings highlight that the surface plays vital roles in the fabrication of nanodevices by being a functional part of them.

Journal ArticleDOI
TL;DR: In this paper, the nitrogen-vacancy centers in diamond (NV) attract great attention because they serve as a tool in many important applications and they have a polarizable spin S = 1 ground state and its spin st
Abstract: Nitrogen-vacancy centers in diamond (NV) attract great attention because they serve as a tool in many important applications. The NV center has a polarizable spin S = 1 ground state and its spin st ...

Journal ArticleDOI
TL;DR: In this paper, the vibronic structure of the spin-triplet optical transition in diamond nitrogen-vacancy centres is described using accurate first-principles methods based on hybrid functionals.
Abstract: In this work we present theoretical calculations and analysis of the vibronic structure of the spin-triplet optical transition in diamond nitrogen-vacancy centres. The electronic structure of the defect is described using accurate first-principles methods based on hybrid functionals. We devise a computational methodology to determine the coupling between electrons and phonons during an optical transition in the dilute limit. As a result, our approach yields a smooth spectral function of electron-phonon coupling and includes both quasi-localized and bulk phonons on equal footings. The luminescence lineshape is determined via the generating function approach. We obtain a highly accurate description of the luminescence band, including all key parameters such as the Huang-Rhys factor, the Debye-Waller factor, and the frequency of the dominant phonon mode. More importantly, our work provides insight into the vibrational structure of nitrogen vacancy centres, in particular the role of local modes and vibrational resonances. In particular, we find that the pronounced mode at 65 meV is a vibrational resonance, and we quantify localization properties of this mode. These excellent results for the benchmark diamond nitrogen-vacancy centre provide confidence that the procedure can be applied to other defects, including alternative systems that are being considered for applications in quantum information processing.

Journal ArticleDOI
TL;DR: For the first time, by ab initio computations of the Gibbs free energy, a phase diagram is obtained of quasi- two-dimensional carbon-diamond film versus multilayered graphene, which describes accurately the role of film thickness h and shows the feasibility of creating novel quasi-two-dimensional materials.
Abstract: We explore how a few-layer graphene can undergo phase transformation into thin diamond film under reduced or no pressure, if the process is facilitated by hydrogenation of the surfaces. Such a "chemically induced phase transition" is inherently nanoscale phenomenon, when the surface conditions directly affect thermodynamics, and the transition pressure depends greatly on film thickness. For the first time we obtain, by ab initio computations of the Gibbs free energy, a phase diagram (P, T, h) of quasi-two-dimensional carbon-diamond film versus multilayered graphene. It describes accurately the role of film thickness h and shows the feasibility of creating novel quasi-two-dimensional materials. Further, the role of finite diameter of graphene flakes and possible formation of the diamond films with the (110) surface are described as well.

Journal ArticleDOI
TL;DR: In this paper, quantum Monte Carlo calculations were performed to study the cohesive energy of carbon allotropes, including sp 3-bonded diamond, sp 2-bunded graphene, sp-sp 2 hybridized graphynes, and sp-bonding carbyne, and it was shown that γ-graphyne, the most energetically stable graphyne, turns out to be 6.766(6) eV/atom, which is smaller than that of graphene by 0.698(12)
Abstract: We have performed quantum Monte Carlo calculations to study the cohesion energetics of carbon allotropes, including sp 3-bonded diamond, sp 2-bonded graphene, sp–sp 2 hybridized graphynes, and sp-bonded carbyne. The computed cohesive energies of diamond and graphene are found to be in excellent agreement with the corresponding values determined experimentally for diamond and graphite, respectively, when the zero-point energies, along with the interlayer binding in the case of graphite, are included. We have also found that the cohesive energy of graphyne decreases systematically as the ratio of sp-bonded carbon atoms increases. The cohesive energy of γ-graphyne, the most energetically stable graphyne, turns out to be 6.766(6) eV/atom, which is smaller than that of graphene by 0.698(12) eV/atom. Experimental difficulty in synthesizing graphynes could be explained by their significantly smaller cohesive energies. Finally, we conclude that the cohesive energy of a newly proposed graphyne can be accurately estimated with the carbon–carbon bond energies determined from the cohesive energies of graphene and three different graphynes considered here.