Steven Prawer

Systematic variation of the Raman spectra of DLC films as a function of sp2:sp3 composition

Abstract We report the Raman spectra of a set of hydrogen-free diamond-like carbon (DLC) films prepared under conditions that result in different types of carbon bonding and for which the sp 2 :sp 3 content was independently determined by electron energy loss spectroscopy. The films were prepared using a mass selected C + ion beam deposition system covering the ion energy range 10 eV to 20 keV. Previous measurements have shown that the sp 2 component of the films decreases as the ion energy is increased from about 10 to 300 eV. For films made with ion energies in excess of 1 keV, the sp 2 component increases with increasing ion energy. The Raman spectra of these films show a broad asymmetric peak which narrows with decreasing sp 2 content. The spectra were fitted with a single skewed lorentzian peak described by the Breit-Wigner-Fano lineshape. The data presented may serve as a reference for DLC characterization. In particular, the parameters from the fits show a strong dependence on the sp 2 component of the films which may be used to identify unambiguously (hydrogen-free) DLC films of low sp 2 content (i.e. very “diamond-like” films).

Room-temperature coherent coupling of single spins in diamond

Coherent coupling between single quantum objects is at the very heart of modern quantum physics. When the coupling is strong enough to prevail over decoherence, it can be used to engineer quantum entangled states. Entangled states have attracted widespread attention because of applications to quantum computing and long-distance quantum communication. For such applications, solid-state hosts are preferred for scalability reasons, and spins are the preferred quantum system in solids because they offer long coherence times. Here we show that a single pair of strongly coupled spins in diamond, associated with a nitrogen-vacancy defect and a nitrogen atom, respectively, can be optically initialized and read out at room temperature. To effect this strong coupling, close proximity of the two spins is required, but large distances from other spins are needed to avoid deleterious decoherence. These requirements were reconciled by implanting molecular nitrogen into high-purity diamond.

Raman spectroscopy of diamond and doped diamond

The optimization of diamond films as valuable engineering materials for a wide variety of applications has required the development of robust methods for their characterization. Of the many methods used, Raman microscopy is perhaps the most valuable because it provides readily distinguishable signatures of each of the different forms of carbon (e.g. diamond, graphite, buckyballs). In addition it is non-destructive, requires little or no specimen preparation, is performed in air and can produce spatially resolved maps of the different forms of carbon within a specimen. This article begins by reviewing the strengths (and some of the pitfalls) of the Raman technique for the analysis of diamond and diamond films and surveys some of the latest developments (for example, surface-enhanced Raman and ultraviolet Raman spectroscopy) which hold the promise of providing a more profound understanding of the outstanding properties of these materials. The remainder of the article is devoted to the uses of Raman spectroscopy in diamond science and technology. Topics covered include using Raman spectroscopy to assess stress, crystalline perfection, phase purity, crystallite size, point defects and doping in diamond and diamond films.

Quantum measurement and orientation tracking of fluorescent nanodiamonds inside living cells

Fluorescent particles are routinely used to probe biological processes. The quantum properties of single spins within fluorescent particles have been explored in the field of nanoscale magnetometry, but not yet in biological environments. Here, we demonstrate optically detected magnetic resonance of individual fluorescent nanodiamond nitrogen-vacancy centres inside living human HeLa cells, and measure their location, orientation, spin levels and spin coherence times with nanoscale precision. Quantum coherence was measured through Rabi and spin-echo sequences over long (>10 h) periods, and orientation was tracked with effective 1° angular precision over acquisition times of 89 ms. The quantum spin levels served as fingerprints, allowing individual centres with identical fluorescence to be identified and tracked simultaneously. Furthermore, monitoring decoherence rates in response to changes in the local environment may provide new information about intracellular processes. The experiments reported here demonstrate the viability of controlled single spin probes for nanomagnetometry in biological systems, opening up a host of new possibilities for quantum-based imaging in the life sciences.

Diamond-based single-photon emitters

The exploitation of emerging quantum technologies requires efficient fabrication of key building blocks. Sources of single photons are extremely important across many applications as they can serve as vectors for quantum information—thereby allowing long-range (perhaps even global-scale) quantum states to be made and manipulated for tasks such as quantum communication or distributed quantum computation. At the single-emitter level, quantum sources also afford new possibilities in terms of nanoscopy and bio-marking. Color centers in diamond are prominent candidates to generate and manipulate quantum states of light, as they are a photostable solid-state source of single photons at room temperature. In this review, we discuss the state of the art of diamond-based single-photon emitters and highlight their fabrication methodologies. We present the experimental techniques used to characterize the quantum emitters and discuss their photophysical properties. We outline a number of applications including quantum key distribution, bio-marking and sub-diffraction imaging, where diamond-based single emitters are playing a crucial role. We conclude with a discussion of the main challenges and perspectives for employing diamond emitters in quantum information processing.

The Raman spectrum of nanocrystalline diamond

Abstract Nanometre sized diamond powder has been purified by centrifugation to remove contamination from sp2 bonded carbon. The purified powder has been characterized using electron energy loss spectroscopy (EELS) and Raman spectroscopy. The EELS spectra confirmed the absence of sp2 bonded carbon and showed strong contributions from surface plasmons. Strong relatively sharp peaks are observed in the Raman spectra at 500, 1140, 1132 and 1630 cm −1 . By comparing the Raman spectra of the nanodiamond clusters with that of amorphized diamond and with calculations of the vibrational density of states we are able to suggest the origin of features in the vibrational spectrum from nanocrystalline diamond.

Coherent population trapping of single spins in diamond under optical excitation

Coherent population trapping is demonstrated in single nitrogen-vacancy centers in diamond under optical excitation. For sufficient excitation power, the fluorescence intensity drops almost to the background level when the laser modulation frequency matches the 2.88 GHz splitting of the ground states. The results are well described theoretically by a four-level model, allowing the relative transition strengths to be determined for individual centers. The results show that all-optical control of single spins is possible in diamond.

Direct quantitative detection of the sp3 bonding in diamond-like carbon films using ultraviolet and visible Raman spectroscopy

The bonding in a series of unhydrogenated amorphous carbon films has been analyzed quantitatively using Raman spectroscopy excited by laser light in both the visible and ultraviolet regions of the spectrum. The asymmetry of the peak near 1550 cm−1 in the visible Raman spectra is correlated with the percentage of sp3 bonding in the films. The ultraviolet Raman spectra exhibit two broad Raman peaks at 1650 and 1100 cm−1, due to sp2 and sp3 vibrational modes, respectively. The former is a resonance feature associated with a large proportion of paired sp2 sites, while the latter is a weighted phonon density-of-states for the distorted random network of sp3 sites. The position and relative intensity of the two peaks are shown to be strongly correlated with the percentage of sp3 sites in the films, providing a reliable measure of sp3 bonding which is both semiquantitative and nondestructive.

Stark Shift Control of Single Optical Centers in Diamond

Lifetime-limited optical excitation lines of single nitrogen-vacancy (NV) defect centers in diamond have been observed at liquid helium temperature. They display unprecedented spectral stability over many seconds and excitation cycles. Spectral tuning of the spin-selective optical resonances was performed via the application of an external electric field (i.e., the Stark shift). A rich variety of Stark shifts were observed including linear as well as quadratic components. The ability to tune the excitation lines of single NV centers has potential applications in quantum information processing.

Implantation of labelled single nitrogen vacancy centers in diamond using N15

Nitrogen-vacancy (NV−) color centers in diamond were created by implantation of 7 keV N15(I=1∕2) ions into type IIa diamond. Optically detected magnetic resonance was employed to measure the hyperfine coupling of single NV− centers. The hyperfine spectrum from NV−15 arising from implanted N15 can be distinguished from NV−14 centers created by native N14(I=1) sites. Analysis indicates 1 in 40 implanted N15 atoms give rise to an optically observable NV−15 center. This report ultimately demonstrates a mechanism by which the yield of NV− center formation by nitrogen implantation can be measured.