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Quantum metrology is a powerful tool for explorations of fundamental physical phenomena and applications in material science and biochemical analysis. While in principle the sensitivity can be improved by increasing the density of sensing particles, in practice this improvement is severely hindered by interactions between them. Here, using a dense ensemble of interacting electronic spins in diamond, we demonstrate a novel approach to quantum metrology to surpass such limitations. It is based on a new method of robust quantum control, which allows us to simultaneously suppress the undesired effects associated with spin-spin interactions, disorder, and control imperfections, enabling a fivefold enhancement in coherence time compared to state-of-the-art control sequences. Combined with optimal spin state initialization and readout directions, this allows us to achieve an ac magnetic field sensitivity well beyond the previous limit imposed by interactions, opening a new regime of high-sensitivity solid-state ensemble magnetometers., publishedVersion

The application of transparent conducting oxides in electronic devices like solar cells or displays is common. By transferring this technology to quantum sensing and computing in the form of microwave conductors, it is possible to benefit from the advantages of these materials. By using indium tin oxide (ITO), it is demonstrated that at an arbitrary position below the conductor, an arbitrary elliptical microwave polarization can be produced by two independent sources. This is independent of the geometry and size of the ITO, whereby a non-resonant microwave approach can be chosen. Using single nitrogen vacancy (NV) centers in diamond in combination with a cross-like ITO structure, each NV center can be addressed with an ideal (clockwise or anticlockwise) microwave polarization. By optimizing the coupling of the microwave field to the NV centers and minimizing the conductor size, the creation of smaller devices compared to common approaches is possible., publishedVersion

The simultaneous control of the number and position of negatively charged nitrogen-vacancy (NV) centers in diamond was achieved. While single near-surface NV centers are known to exhibit outstanding capabilities in external spin sensing, trade-off relationships among the accuracy of the number and position, and the coherence of NV centers have made the use of such engineered NV centers difficult. Namely, low-energy nitrogen implantation with lithographic techniques enables the nanoscale position control but results in degradation of the creation yield and the coherence property. In this paper, we show that low-energy nitrogen ion implantation to a 12C (99.95%)-enriched homoepitaxial diamond layer using nanomask is applicable to create shallow NV centers with a sufficiently long coherence time for external spin sensing, at a high creation yield. Furthermore, the NV centers were arranged in a regular array so that 40% lattice sites contain single NV centers. The XY8-k measurements using the individual NV centers reveal that the created NV centers have depths from 2 to 12 nm, which is comparable to the stopping range of nitrogen ions implanted at 2.5 keV. We show that the position-controlled NV centers are capable of external spin sensing with a ultra-high spatial resolution., publishedVersion

This thesis is dedicated to applications of nanodiamonds with colour centres for imaging and magnetic field sensing. Diamond nanocrystals with optically active defects such as nitrogen-vacancy (NV) or silicon-vacancy (SiV) can be used as optical markers. They are characterized by highly stable emission in contrast to other known optical markers. Owing to this they are attractive for studies of biological systems. First part of this thesis demonstrates application of nanodiamonds for drug delivery process. Stabilization of the nanocrystal’s surface in different solutions was achieved by coating with HSA-protein. Utilizing protein-protected nanodiamonds as carriers for chemotherapy drug (Doxorubicin), targeted delivery to the acidic tumor was demonstrated. Pre-clinical test proved the effectivity of this method compared to free drug molecules. The negatively charged nitrogen-vacancy centre due to unique combination of its optical and spin properties can be used as an atomic scale magnetic sensor. It combines in one high sensitivity and high resolution. In second part of this thesis these properties are exploited for detection of the metallo-protein – ferritin. The measurements of spin relaxation times allow to reveal the presence of ferritin in close vicinity of NV centre. The demonstrated experiments pave the way to a new method of ferritin’s core investigation, which is invaluable for diagnostics of different diseases.

The sensitivity of Magnetic Resonance Imaging (MRI) depends strongly on nuclear spin polarisation and, motivated by this observation, dynamical nuclear spin polarisation has recently been applied to enhance MRI protocols (Kurhanewicz, J., et al., Neoplasia 13, 81 (2011)). Nuclear spins associated with the 13 C carbon isotope (nuclear spin I = 1/2) in diamond possess uniquely long spin lattice relaxation times (Reynhardt, E.C. and G.L. High, Prog. in Nuc. Mag. Res. Sp. 38, 37 (2011)) If they are present in diamond nanocrystals, especially when strongly polarised, they form a promising contrast agent for MRI. Current schemes for achieving nuclear polarisation, however, require cryogenic temperatures. Here we demonstrate an efficient scheme that realises optically induced 13 C nuclear spin hyperpolarisation in diamond at room temperature and low ambient magnetic field. Optical pumping of a Nitrogen-Vacancy (NV) centre creates a continuously renewable electron spin polarisation which can be transferred to surrounding 13 C nuclear spins. Importantly for future applications we also realise polarisation protocols that are robust against an unknown misalignment between magnetic field and crystal axis., Comment: This is the revision submitted to NJP

Very early on, the diamond industry formed a culturally uniform global monopoly, run by De Beers. But gradually new factors emerged, which it was unable to fully control: advances in synthetic diamond production; the geographical diversification of mining, trading and cutting; the intrusion of powerful mining companies and determined actors from outside the system; a loss of image for diamonds as a result of bloody conflict and trafficking in Africa; and changing techniques and consumer behaviour. Since 2002 De Beers has had to completely change strategy. The diamond industry is more «globalised » than before, but diversified and polycentric.

En utilisant une démarche de type "Chimie du Solide", le rôle des principaux facteurs caractérisant la surface du substrat (composition chimique, structure et liaisons chimiques) sur la germination de cristallites de diamant, ainsi que leur morphologie, a ete mis en évidence. La densité de nucléation et le rapport Csp2/Csp3 ont pu notamment etre corrélés a la diffusion du carbone dans le substrat. Afin de contrôler celle-ci, des couches superficielles de composes covalents tels que les nitrures et les borures ont été utilisées. Elles ont permis d'atteindre des densités très importantes de nucléi de diamant pour des temps de dépôt relativement courts. L'ensemble des résultats concernant le dépôt par hétéroépitaxie du diamant a permis de proposer une méthodologie au niveau du choix du substrat et des espèces réactives pour l'obtention de couches minces de nitrure de bore cubique.; non disponible

Diamond has excellent optical properties including broadband transmissivity, low self-absorption, and a high refractive index, which have prompted its use for optical sensing applications. Thin- film diamond strip waveguides (DSWGs) combined with tunable quantum cascade lasers (tQCLs) providing an emission wave- length range of 5.78–6.35 mm (1735–1570 cm"1) have been used to obtain mid-infrared (MIR) spectra of proteins, thereby enabling the analysis of their secondary structure via the amide I band. Three different proteins were analyzed, namely bovine serum albumin (BSA), myoglobin, and g-globulin. The secondary structure of BSA and myoglobin has a major contribution of a-helices, whereas g-globulins are rich in b-sheet structures, which is reflected in the amide I band. A comparison of the spectra obtained via the combination of the tQCL and DSWG with spectra obtained using conventional Fourier transform infrared (FTIR) spectroscopy and a commercial diamond attenuated total reflection (ATR) element has been performed. It is shown that the main features evident in FTIR-ATR spectra are also obtained using tQCL-DSWG sensors., acceptedVersion

Diamond has excellent optical properties including broadband transmissivity, low self- absorption and a high refractive index, which have prompted its use in for optical sensing applications. Thin-film diamond strip waveguides (DSWGs) combined with tunable quantum cascade lasers (tQCLs) providing an emission wavelength range of 5.78-6.35 μm (1735-1570 cm-1) have been used to obtain mid-infrared (MIR) spectra of proteins, thereby enabling the analysis of their secondary structure via the amide I band. Three different proteins were analyzed, namely bovine serum albumin (BSA), myoglobin, and γ-globulin. The secondary structure of BSA and myoglobin has a major contribution of -helices, whereas γ-globulins are rich in β-sheet structures, which is reflected in the amide I band. A comparison of the spectra obtained via the combination of the tQCL and DSWG with spectra obtained using conventional Fourier transform infrared (FTIR) spectroscopy and a commercial diamond attenuated total reflection (ATR) element has been performed. It is shown that the main features evident in FTIR-ATR spectra are also obtained using tQCL-DSWG sensors., submittedVersion