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Controlled crystallization, melting and vitrification are important fundamental processes in nature and technology. However, the microscopic details of these fundamental phenomena still lack understanding, in particular how the cooling rate and presence of a wall influence the crystal nucleation and glass formation. Thermoresponsive microgels provide the possibility to study phase transitions on a single-particle level, owing to the ability to tune the particle size with temperature. In this study, we employ composite microgels consisting of a hard core and a crosslinked poly(N-isopropyl acrylamide-co-methacrylic acid) shell to study the crystallization of dense suspensions of soft colloids near a wall using confocal microscopy. We investigate the effect of cooling rate on the fluid-to-solid transition close to the sample wall. The structures formed during cooling range from glassy in case of a rapid temperature quench, to crystalline when a slow cooling rate is used. Detailed analysis of the final structure reveals that the cooling rate also sets the degree of alignment of the crystal domains with the wall as a result of a balance between homogeneous and heterogenous crystal nucleation. The results presented here yield valuable insight into the microscopic details of temperature-controlled crystallization near a wall. This understanding will help pave the way towards optimal crystallization conditions for microgel applications., Comment: Main: 10 pages, 9 figures; SI: 7 pages, 5 figures

The self-organization of clusters of particles is a fundamental phenomenon across various physical systems, including hydrodynamic and colloidal systems. One example is that of dense spherical particles submerged in a fluid and subjected to horizontal oscillations. The interaction of the particles with the oscillating flow leads to the formation of one-particle-thick chains or multiple-particle-wide bands. In this study, we model the hydrodynamic interactions between such particles and parallel chains using simplified potentials. We first focus on the hydrodynamic interactions between chains, which we characterize using data from numerical simulations. Based on these interactions, we propose a simplified model potential, called the Siren potential, which combines the representative hydrodynamic interactions: short-range attraction, mid-range repulsion, and long-range attraction. Through one-dimensional Monte Carlo simulations, we successfully replicate the characteristic patterns observed in hydrodynamic experiments and draw the phase diagram for the model potential. We extend our analysis to two-dimensional systems, introducing a dipole-capillary model potential that accounts for both chain formation and Siren-like chain interactions. This potential is based on colloidal particles at an interface, where chain formation is driven by an external electric field inducing a dipole moment parallel to the interface in each particle. The capillary force contributes the long-range attraction. Starting with parallel chains, the patterns in the two-dimensional Monte Carlo simulations of this colloidal system are similar to those observed in the hydrodynamic experiments. Still, the model potentials help clarify the dynamic behavior of the particles and chains due to the complex interactions encountered in both hydrodynamic and colloidal systems, drawing parallels between them., Comment: 17 pages, 15 figures, under review at Physical Review E

Light-emitting complex defects in silicon have been considered a potential platform for quantum technologies based on spin and photon degrees of freedom working at telecom wavelengths. Their integration in complex devices is still in its infancy, and it was mostly focused on light extraction and guiding. Here we address the control of the electronic states of carbon-related impurities (G-centers) via strain engineering. By embedding them in patches of silicon on insulator and topping them with SiN, symmetry breaking along [001] and [110] directions is demonstrated, resulting in a controlled splitting of the zero phonon line (ZPL), as accounted for by the piezospectroscopic theoretical framework. The splitting can be as large as 18 meV and it is finely tuned by selecting patch size or by moving in different positions on the patch. Some of the split, strained ZPLs are almost fully polarized and their overall intensity is enhanced up to 7 times with respect to the flat areas, whereas their recombination dynamics is slightly affected. Our technique can be extended to other impurities and Si-based devices such as suspended bridges, photonic crystal microcavities, Mie resonators, and integrated photonic circuits., Comment: 14 pages; 10 figures

We report successful incorporation of an ensemble of G centers in silicon-on-insulator (SOI) microrings using ion implantation and conventional nanofabrication. The coupling between the emitters and the resonant modes of the microrings is studied using continuous-wave and time-resolved microphotoluminescence (PL) experiments. We observe the resonant modes of the microrings on PL spectra, on the wide spectral range that is covered by G centers emission. By finely tuning the size of the microrings, we match their zero-phonon line at 1278 nm with a resonant mode of quality factor around 3000 and volume 7.2 (lambda over n)^3. The zero-phonon line intensity is enhanced by a factor of 5, both in continuous-wave and time-resolved measurements. This is attributed to the Purcell enhancement of zero-phonon spontaneous emission into the resonant mode and quantitatively understood considering the distribution of the G centers dipoles. Despite the enhancement of the zero-phonon emission, we do not observe any sizeable decrease of the average lifetime of the G centers, which points at a low radiative yield (<10%). We reveal the detrimental impact of parasitic defects in heavily implanted silicon, and discuss the perspectives for quantum electrodynamics experiments with individual color centers in lightly implanted SOI rings. Our results provide key information for the development of deterministic single photon sources for integrated quantum photonics., Comment: 24 pages, 7 figures, submitted to an international journal with peer review

The nanoscale localization of individual paramagnetic defects near an electrical circuit is an important step for realizing hybrid quantum devices with strong spin-microwave photon coupling. Here, we demonstrate the fabrication of an array of individual NV centers in diamond near a metallic nanowire deposited on top of the substrate. We determine the relative position of each NV center with $\sim$10\,nm accuracy, using it as a vector magnetometer to measure the field generated by passing a dc current through the wire., Comment: 6 pages, 5 figures

We report the detection of individual emitters in silicon belonging to seven different families of optically-active point defects. These fluorescent centers are created by carbon implantation of a commercial silicon-on-insulator wafer usually employed for integrated photonics. Single photon emission is demonstrated over the [1.1,1.55]-$\mu$m range, spanning the O- and C-telecom bands. We analyse their photoluminescence spectrum, dipolar emission and optical relaxation dynamics at 10K. For a specific family, we show a constant emission intensity at saturation from 10K to temperatures well above the 77K-liquid nitrogen temperature. Given the advanced control over nanofabrication and integration in silicon, these novel artificial atoms are promising candidates for Si-based quantum technologies.

We report on the creation and characterization of the luminescence properties of high-purity diamond substrates upon F ion implantation and subsequent thermal annealing. Their room-temperature photoluminescence emission consists of a weak emission line at 558 nm and of intense bands in the 600 - 750 nm spectral range. Characterization at liquid He temperature reveals the presence of a structured set of lines in the 600 - 670 nm spectral range. We discuss the dependence of the emission properties of F-related optical centers on different experimental parameters such as the operating temperature and the excitation wavelength. The correlation of the emission intensity with F implantation fluence, and the exclusive observation of the afore-mentioned spectral features in F-implanted and annealed samples provides a strong indication that the observed emission features are related to a stable F-containing defective complex in the diamond lattice., Comment: 10 pages, 5 figures

Given its unrivaled potential of integration and scalability, silicon is likely to become a key platform for large-scale quantum technologies. Individual electron-encoded artificial atoms either formed by impurities or quantum dots have emerged as a promising solution for silicon-based integrated quantum circuits. However, single qubits featuring an optical interface needed for large-distance exchange of information have not yet been isolated in such a prevailing semiconductor. Here we show the isolation of single optically-active point defects in a commercial silicon-on-insulator wafer implanted with carbon atoms. These artificial atoms exhibit a bright, linearly polarized single-photon emission at telecom wavelengths suitable for long-distance propagation in optical fibers. Our results demonstrate that despite its small bandgap (~ 1.1 eV) a priori unfavorable towards such observation, silicon can accommodate point defects optically isolable at single scale, like in wide-bandgap semiconductors. This work opens numerous perspectives for silicon-based quantum technologies, from integrated quantum photonics to quantum communications and metrology.

This paper presents a novel variational formulation to simulate linear free-surface flow. The variational formulation is suitable for higher-order finite elements and higher-order and higher-continuity shape functions as employed in Isogeometric Analysis (IGA). The novel formulation combines the interior and free-surface problems in one monolithic formulation. This leads to exact energy conservation and superior performance in terms of accuracy when compared to a traditional segregated formulation. This is confirmed by the numerical computation of traveling waves in a periodic domain and a three-dimensional sloshing problem. The isogeometric approach shows significant improved performance compared to traditional finite elements. Even on very coarse quadratic NURBS meshes the dispersion error is virtually absent.

We report on the creation and characterization of Pb-related color centers in diamond upon ion implantation and subse- quent thermal annealing. Their optical emission in photoluminescence (PL) regime consists of an articulated spectrum with intense emission peaks at 552.1 nm and 556.8 nm, accompanied by a set of additional lines in the 535700 nm range. The attribution of the PL emission to stable Pb-based defects is corroborated by the correlation of its intensity with the implantation fluence of Pb ions, while none of the reported features is observed in reference samples implanted with C ions. Furthermore, PL measurements performed as a function of sample temperature (143-300 K range) and un- der different excitation wavelengths (532 nm, 514 nm, 405 nm) suggest that the complex spectral features observed in Pb-implanted diamond might be related to a variety of different defects and/or charge states. This work follows from previous reports on optically active centers in diamond based on group IV impurities, such as Si, Ge and Pb. In perspective, a comprehensive study of this set of defect complexes could bring significant insight on the common features involved in their formation and opto-physical properties, thus offering a solid basis for the devel- opment of a new generation of quantum-optical devices., Comment: 7 pages, 4 figures

The fabrication of luminescent defects in single-crystal diamond upon Sn implantation and annealing is reported. The relevant spectral features of the optical centers (emission peaks at 593.5 nm, 620.3 nm, 630.7 nm and 646.7 nm) are attributed to Sn-related defects through the correlation of their photoluminescence (PL) intensity with the implantation fluence. Single Sn-related defects were identified and characterized through the acquisition of their second-order auto-correlation emission functions, by means of Hanbury-Brown-Twiss interferometry. The investigation of their single-photon emission regime as a function of excitation laser power revealed that Sn-related defects are based on three-level systems with a 6 ns radiative decay lifetime. In a fraction of the studied centers, the observation of a blinking PL emission is indicative of the existence of a dark state. Furthermore, absorption dependence from the polarization of the excitation radiation with about 45 percent contrast was measured. This work shed light on the existence of a new optical center associated with a group-IV impurity in diamond, with similar photo-physical properties to the already well-known Si-V and Ge-V emitters, thus providing results of interest from both the fundamental and applicative points of view., Comment: 10 pages, 4 figures

We demonstrate experimentally Hanbury Brown and Twiss (HBT) interferometry at a hard X-ray Free Electron Laser (XFEL) on a sample diffraction patterns. This is different from the traditional approach when HBT interferometry requires direct beam measurements in absence of the sample. HBT analysis was carried out on the Bragg peaks from the colloidal crystals measured at Linac Coherent Light Source (LCLS). We observed high degree (80%) spatial coherence of the full beam and the pulse duration of the monochromatized beam on the order of 11 fs that is significantly shorter than expected from the electron bunch measurements., Comment: 32 pages, 10 figures, 2 tables

We addressed the carrier dynamics in so-called G-centers in silicon (consisting of substitutional-interstitial carbon pairs interacting with interstitial silicons) obtained via ion implantation into a silicon-on-insulator wafer. For this point defect in silicon emitting in the telecommunication wavelength range, we unravel the recombination dynamics by time-resolved photoluminescence spectroscopy. More specifically, we performed detailed photoluminescence experiments as a function of excitation energy, incident power, irradiation fluence and temperature in order to study the impact of radiative and non-radiative recombination channels on the spectrum, yield and lifetime of G-centers. The sharp line emitting at 969 meV ($\sim$1280 nm) and the broad asymmetric sideband developing at lower energy share the same recombination dynamics as shown by time-resolved experiments performed selectively on each spectral component. This feature accounts for the common origin of the two emission bands which are unambiguously attributed to the zero-phonon line and to the corresponding phonon sideband. In the framework of the Huang-Rhys theory with non-perturbative calculations, we reach an estimation of 1.6$\pm$0.1 $\angstrom$ for the spatial extension of the electronic wave function in the G-center. The radiative recombination time measured at low temperature lies in the 6 ns-range. The estimation of both radiative and non-radiative recombination rates as a function of temperature further demonstrate a constant radiative lifetime. Finally, although G-centers are shallow levels in silicon, we find a value of the Debye-Waller factor comparable to deep levels in wide-bandgap materials. Our results point out the potential of G-centers as a solid-state light source to be integrated into opto-electronic devices within a common silicon platform.

Micrometer width and nanometer thick wires with different shapes were produced $\approx 3~\upmu$m below the surface of a diamond crystal using a microbeam of He$^+$ ions with 1.8~MeV energy. Initial samples are amorphous and after annealing at $T\approx 1475$~K, the wires crystallized into a graphite-like structures, according to confocal Raman spectroscopy measurements. The electrical resistivity at room temperature is only one order of magnitude larger than the in-plane resistivity of highly oriented pyrolytic bulk graphite and shows a small resistivity ratio($\rho(2{\rm K})/\rho(315{\rm K}) \approx 1.275$). A small negative magnetoresistance below $T=200$~K was measured and can be well understood taking spin-dependent scattering processes into account. The used method provides the means to design and produce millimeter to micrometer sized conducting circuits with arbitrary shape embedded in a diamond matrix., Comment: 12 pages, 5 figures, to be published in Journal of Physics D: Applied Physics (Feb. 2017)

An emerging branch of electronics, the optospintronics, would be highly boosted if the control of magnetic order by light is implemented in magnetic semiconductors nanostructures being compatible with the actual technology. Here we show that the ferromagnetic magnetization of low Fe-doped ZnO nanowires prepared by carbothermal process is enhanced under illumination up to temperatures slightly below room temperature. This enhancement is related to the existence of an oxygen vacancy V$_{\rm O}$ in the neighbouring of an antiferromagnetic superexchange Fe$^{3+}$-Fe$^{3+}$ pair. Under illumination the V$_{\rm O}$ is ionized to V$_{\rm O}^+$ giving an electron to a close Fe$^{3+}$ ion from the antiferromagnetic pair. This light excited electron transition allows the transition of Fe$^{3+}$ to Fe$^{2+}$ forming stable ferromagnetic double exchange pairs, increasing the total magnetization. The results here presented indicate an efficient way to influence the magnetic properties of ZnO based nanostructures by light illumination at high temperatures., Comment: 4 pages with 4 figures, to be published in Appl. Phys. Lett. (2016)

We present results of a coherent x-ray diffractive imaging experiment performed on a single colloidal crystal grain. The full three-dimensional (3D) reciprocal space map measured by an azimuthal rotational scan contained several orders of Bragg reflections together with the coherent interference signal between them. Applying the iterative phase retrieval approach, the 3D structure of the crystal grain was reconstructed and positions of individual colloidal particles were resolved. As a result, an exact stacking sequence of hexagonal close-packed layers including planar and linear defects were identified., Comment: 8 pages, 5 figures

We analyze the impact of electric field and magnetic field fluctuations in the decoherence of the electronic spin associated with a single nitrogen-vacancy (NV) defect in diamond by engineering spin eigenstates protected either against magnetic noise or against electric noise. The competition between these noise sources is analyzed quantitatively by changing their relative strength through modifications of the environment. This study provides significant insights into the decoherence of the NV electronic spin, which is valuable for quantum metrology and sensing applications., Comment: 8 pages, 4 figures, including supplementary informations

We propose an original analog method to perform instantaneous and quantitative spectral analysis of microwave signals. An ensemble of nitrogen-vacancy (NV) centers held in a diamond plate is pumped by a 532 nm laser. Its photoluminescence is imaged through an optical microscope and monitored by a digital camera. The microwave signal is converted to an oscillating magnetic field in the area of the NV centers by a loop shaped antenna. Induced magnetic resonances are detected through a decrease of the NV centers photoluminescence. A magnetic field gradient induces a Zeeman shift of the resonances and transforms the frequency information into spatial information, which allows for the simultaneous analysis of the microwave signal in the entire frequency bandwidth of the device. The time dependent spectral analysis of an amplitude modulated microwave signal is demonstrated over a bandwidth of 600 MHz, associated to a frequency resolution of 7 MHz and a refresh rate of 4 ms. With such integration time, a field of a few hundreds of {\mu}W can be detected. Since the optical properties of NV centers can be maintained even in high magnetic field, we estimate that an optimized device could allow frequency analysis in a range of 30 GHz, only limited by the amplitude of the magnetic field gradient. In addition, an increase of the NV centers quantity could lead both to an increase of the microwave sensitivity and to a decrease of the minimum refresh rate down to a few {\mu}s., Comment: 9 pages, 2 figures

Understanding the dynamics of molecules adsorbed to surfaces or confined to small volumes is a matter of increasing scientific and technological importance. Here, we demonstrate a pulse protocol using individual paramagnetic nitrogen vacancy (NV) centers in diamond to observe the time evolution of 1H spins from organic molecules located a few nanometers from the diamond surface. The protocol records temporal correlations among the interacting 1H spins, and thus is sensitive to the local system dynamics via its impact on the nuclear spin relaxation and interaction with the NV. We are able to gather information on the nanoscale rotational and translational diffusion dynamics by carefully analyzing the time dependence of the NMR signal. Applying this technique to various liquid and solid samples, we find evidence that liquid samples form a semi-solid layer of 1.5 nm thickness on the surface of diamond, where translational diffusion is suppressed while rotational diffusion remains present. Extensions of the present technique could be adapted to highlight the chemical composition of molecules tethered to the diamond surface or to investigate thermally or chemically activated dynamical processes such as molecular folding.

The magneto-transport properties of single proton-implanted ZnO and of Li(7\%)-doped ZnO microwires have been studied. The as-grown microwires were highly insulating and not magnetic. After proton implantation the Li(7\%) doped ZnO microwires showed a non monotonous behavior of the negative magneto-resistance (MR) at temperature above 150 K. This is in contrast to the monotonous NMR observed below 50 K for proton-implanted ZnO. The observed difference in the transport properties of the wires is related to the amount of stable Zn vacancies created at the near surface region by the proton implantation and Li doping. The magnetic field dependence of the resistance might be explained by the formation of a magnetic/non magnetic heterostructure in the wire after proton implantation., Comment: 6 pages with 5 figures

The nitrogen-vacancy (NV) color center in diamond is an atom-like system in the solid-state which specific spin properties can be efficiently used as a sensitive magnetic sensor. An external magnetic field induces Zeeman shifts of the NV center levels which can be measured using Optically Detected Magnetic Resonance (ODMR). In this work, we exploit the ODMR signal of an ensemble of NV centers in order to quantitatively map the vectorial structure of a magnetic field produced by a sample close to the surface of a CVD diamond hosting a thin layer of NV centers. The reconstruction of the magnetic field is based on a maximum-likelihood technique which exploits the response of the four intrinsic orientations of the NV center inside the diamond lattice. The sensitivity associated to a 1 {\mu}m^2 area of the doped layer, equivalent to a sensor consisting of approximately 10^4 NV centers, is of the order of 2 {\mu}T/sqrt{Hz}. The spatial resolution of the imaging device is 400 nm, limited by the numerical aperture of the optical microscope which is used to collect the photoluminescence of the NV layer. The versatility of the sensor is illustrated by the accurate reconstruction of the magnetic field created by a DC current inside a copper wire deposited on the diamond sample., Comment: 11 pages, 5 figures, figure 4 added, results unchanged

In this work, we explore the ability of plasma assisted chemical vapor deposition (PACVD) operating under high power densities to produce thin high-quality diamond layers with a controlled doping with negatively-charged nitrogen-vacancy (NV-) centers. This luminescent defect possesses specific physical characteristics that make it suitable as an addressable solid-state electron spin for measuring magnetic fields with unprecedented sensitivity. To this aim, a relatively large number of NV- centers (> 10^12 cm^-3) should ideally be located in a thin diamond layer (a few tens of nm) close to the surface which is particularly challenging to achieve with the PACVD technique. Here we show that intentional temperature variations can be exploited to tune NV- creation efficiency during growth, allowing engineering complex stacking structures with a variable doping. Because such a temperature variation can be performed quickly and without any change of the gas phase composition, thin layers can be grown. Measurements show that despite the temperature variations, the luminescent centers incorporated using this technique exhibit spin coherence properties similar to those reached in ultra-pure bulk crystals, which suggests that they could be successfully employed in magnetometry applications., Comment: 13 pages, 5 figures, corrected bibliography

We report on the noise spectrum experienced by few nanometer deep nitrogen-vacancy centers in diamond as a function of depth, surface coating, magnetic field and temperature. Analysis reveals a double-Lorentzian noise spectra consistent with a surface electronic spin bath, with slower dynamics due to spin-spin interactions and faster dynamics related to phononic coupling. These results shed new light on the mechanisms responsible for surface noise affecting shallow spins at semiconductor interfaces, and suggests possible directions for further studies. We demonstrate dynamical decoupling from the surface noise, paving the way to applications ranging from nanoscale NMR to quantum networks.

We develop an efficient back gate for silicon-on-insulator (SOI) devices operating at cryogenic temperatures, and measure the quadratic hyperfine Stark shift parameter of arsenic donors in isotopically purified $^{28}$Si-SOI layers using such structures. The back gate is implemented using MeV ion implantation through the SOI layer forming a metallic electrode in the handle wafer, enabling large and uniform electric fields up to $\sim$ 2 V/$\mu$m to be applied across the SOI layer. Utilizing this structure we measure the Stark shift parameters of arsenic donors embedded in the $^{28}$Si SOI layer and find a contact hyperfine Stark parameter of $\eta_a=-1.9\pm0.2\times10^{-3} \mu$m$^2$/V$^2$. We also demonstrate electric-field driven dopant ionization in the SOI device layer, measured by electron spin resonance., Comment: 5 pages, 3 figures

We present nanoscale 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 uT-rms, corresponding to ~330 statistically polarized or ~10 fully polarized proton spins in a ~(1.8 nm)^3 detection volume., Comment: 5 pages, 3 figures

We present a time-resolved infrared (IR) pump and extreme-ultraviolet (XUV) probe diffraction experiment to investigate ultrafast structural dynamics in colloidal crystals with picosecond resolution. The experiment was performed at the FLASH facility at DESY with a fundamental wavelength of 8 nm. In our experiment, the temporal changes of Bragg peaks were analyzed and their frequency components were calculated using Fourier analysis. Periodic modulations in the colloidal crystal were localized at a frequency of about 4-5 GHz. Based on the Lamb theory, theoretical calculations of vibrations of the isotropic elastic polystyrene spheres of 400 nm in size reveal a 5.07 GHz eigenfrequency of the ground (breathing) mode., Comment: 12 pages, 3 figures

We investigate spin and optical properties of individual nitrogen-vacancy centers located within 1-10 nm from the diamond surface. We observe stable defects with a characteristic optically detected magnetic resonance spectrum down to lowest depth. We also find a small, but systematic spectral broadening for defects shallower than about 2 nm. This broadening is consistent with the presence of a surface paramagnetic impurity layer [Tisler et al., ACS Nano 3, 1959 (2009)] largely decoupled by motional averaging. The observation of stable and well-behaved defects very close to the surface is critical for single-spin sensors and devices requiring nanometer proximity to the target., Comment: 5 pages, 4 figures, and Supplementary Material

We describe a technique for fabricating micro- and nano-structures incorporating fluorescent defects in diamond with a positional accuracy in the hundreds of nanometers. Using confocal fluorescence microscopy and focused ion beam (FIB) etching we first locate a suitable defect with respect to registration marks on the diamond surface and then etch a structure using these coordinates. We demonstrate the technique here by etching an 8 micron diameter hemisphere positioned such that a single negatively charged nitrogen-vacancy defect lies at its origin. This type of structure increases the photon collection efficiency by removing refraction and aberration losses at the diamond-air interface. We make a direct comparison of the fluorescence photon count rate before and after fabrication and observe an 8-fold increase due to the presence of the hemisphere.