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 SiV centers in nanodiamonds exhibit 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 ≈730-742 nm and broad linewidths between 5 and 17 nm, whereas the second group comprises a very broad distribution of center wavelengths between 715 and 835 nm, but narrow linewidths from below 1 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 a new class of silicon-related defects. Whereas single photon emission is demonstrated for defect 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.
Bulk silicon carbide (SiC) is a very promising material system for bio-applications and quantum sensing. However, its optical activity lies beyond the near infrared spectral window for in-vivo imaging and fiber communications due to a large forbidden energy gap. Here, we report the fabrication of SiC nanocrystals and isolation of different nanocrystal fractions ranged from 600 nm down to 60 nm in size. The structural analysis reveals further fragmentation of the smallest nanocrystals into ca. 10-nm-size clusters of high crystalline quality, separated by amorphization areas. We use neutron irradiation to create silicon vacancies, demonstrating near infrared photoluminescence. Finally, we detect, for the first time, room-temperature spin resonances of these silicon vacancies hosted in SiC nanocrystals. This opens intriguing perspectives to use them not only as in-vivo luminescent markers, but also as magnetic field and temperature sensors, allowing for monitoring various physical, chemical and biological processes.
Thin films of single-wall carbon nanotubes (SWNTs) can be deposited onto solid substrates by evaporation-induced self-assembly. However, for this process to become more accessible to thin-film-based device fabrication requires optimization and a better understanding of the parameters and mechanisms governing nanoparticle film growth. Here, we focus on the role of contact-line (CL) dynamics at the edge of a receding meniscus for the deposition of thin nanoparticle films from colloidal suspensions. We find that film deposition rates can be increased by up to 2 orders of magnitude over earlier reports if parameters such as SWNT concentration, surfactant concentration, and height of the capillary bridge from which particles are deposited are properly adjusted. Most importantly we have also discovered that CL dynamics leading to the formation of striped films (coffee stains) are best described by dynamical pinning and kink-induced zipping. The existence of critical SWNT and surfactant concentrations as well as their role in determining stripe characteristics can be well accounted for by the proposed dynamical pinning and zipping model.
Nanoparticles, especially from carbon, have great potential in biomedicine. However, prior to clinical use, biocompatibility and biodistribution of these nanoobjects have to be assessed. Currently, particle detection is mostly based on surface-bound labels, inevitably altering materials' properties by surface modification. Further obstacles include bleaching, dissociation of labels from the surface, weak emission of fluorophores due to insufficient tissue opacity or hampered light penetration or the need for specific excitation wavelengths. These characteristics greatly constrain employment of such nanoparticles to address complex analytical questions. To overcome these drawbacks, the use of intrinsic structural features of nanoobjects is highly desirable: the particle surface remains unchanged and the nanoobject exhibits its innate behavior. Thus, for sensitive detection and quantification, labels should be incorporated in the nanoparticle core, thereby avoiding cleavage and warranting unchanged surface characteristics. The incorporation of clinically approved radionuclide 32 P into the lattice of nanodiamond particles using highly defined ion implantation is described here. The properties, uptake, and biodistribution are studied in vivo, in the developing hen's egg model (hen's egg test on chorioallantoic membrane assay). It is found that 32 P labeling of diamond nanoparticles allows their reliable localization and sensitive quantification in a cost efficient, highly reliable, and safe way using available autoradiographic devices and analytical methods.
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