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arXiv:1309.4870 · Physical Review B

Systematic study of defect-related quenching of NV luminescence in diamond with time-correlated single-photon counting spectroscopy

D. Gatto Monticone, Franco Quercioli, Raffaella Mercatelli, Silvia Soria, Stefano Borini, Tommaso Poli, Maurizio M. Vannoni, E. Vittone, P. Olivero

Published Oct 2, 2013• 56 citations
arXivHTMLPDF

Abstract

We report on the systematic characterization of photoluminescence (PL) lifetimes in NV${}^{\ensuremath{-}}$ and NV${}^{0}$ centers in 2-MeV H${}^{+}$-implanted type Ib diamond samples by means of a time-correlated single-photon counting (TCSPC) microscopy technique. A dipole-dipole resonant energy transfer model was applied to interpret the experimental results, allowing a quantitative correlation of the concentration of both native (single substitutional nitrogen atoms) and ion-induced (isolated vacancies) PL-quenching defects with the measured PL lifetimes. The TCSPC measurements were carried out in both frontal (i.e., laser beam probing the main sample surface along the same normal direction of the previously implanted ions) and lateral (i.e., laser beam probing the lateral sample surface orthogonally with respect to the same ion implantation direction) geometries. In particular, the latter geometry allowed a direct probing of the centers lifetime along the strongly nonuniform damage profiles of MeV ions in the crystal. The extrapolation of empirical quasiexponential decay parameters allowed the systematic estimation of the mean quantum efficiency of the centers as a function of intrinsic and ion-induced defect concentration, which is of direct relevance for the current studies on the use of diamond color centers for photonic applications.

DOI
10.1103/physrevb.88.155201

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We report on the systematic characterization of photoluminescence (PL) lifetimes in NV\ensuremath−{}^{\ensuremath{-}}\ensuremath− and NV0{}^{0}0 centers in 2-MeV H+{}^{+}+-implanted type Ib diamond samples by means of a time-correlated single-photon counting (TCSPC) microscopy technique. A dipole-dipole resonant energy transfer model was applied to interpret the experimental results, allowing a quantitative correlation of the concentration of both native (single substitutional nitrogen atoms) and ion-induced (isolated vacancies) PL-quenching defects with the measured PL lifetimes. The TCSPC measurements were carried out in both frontal (i.e., laser beam probing the main sample surface along the same normal direction of the previously implanted ions) and lateral (i.e., laser beam probing the lateral sample surface orthogonally with respect to the same ion implantation direction) geometries. In particular, the latter geometry allowed a direct probing of the centers lifetime along the strongly nonuniform damage profiles of MeV ions in the crystal. The extrapolation of empirical quasiexponential decay parameters allowed the systematic estimation of the mean quantum efficiency of the centers as a function of intrinsic and ion-induced defect concentration, which is of direct relevance for the current studies on the use of diamond color centers for photonic applications.
We report depth-resolved photoluminescence measurements of nitrogen-vacancy (NV−) centers formed along the tracks of swift heavy ions (SHIs) in type Ib synthetic single crystal diamonds that had been doped with 100 ppm nitrogen during crystal growth. Analysis of the spectra shows that NV− centers are formed preferentially within regions where electronic stopping processes dominate and not at the end of the ion range where elastic collisions lead to the formation of vacancies and defects. Thermal annealing further increases NV yields after irradiation with SHIs preferentially in regions with high vacancy densities. NV centers formed along the tracks of single swift heavy ions can be isolated with lift-out techniques for explorations of color center qubits in quasi-1D registers with an average qubit spacing of a few nanometers and of order 100 color centers per micrometer along 10 to 30-μm-long percolation chains.
Precise control over the spatial distribution and charge state of nitrogen-vacancy (NV) centers in diamond is a key requirement for further advancing this platform in quantum sensing and photonic applications. Here, we investigate nitrogen ion implantation as a scalable method to engineer NV centers in bulk single-crystalline (SC) and a 5 μ m -thick polycrystalline (PC) diamond membrane. Nitrogen-doped regions (1–80 ppm) were fabricated using a 0.7 MeV ion beam and high-temperature annealing, with NV center formation verified by confocal fluorescence imaging and spectral analysis. In SC bulk diamond, we estimate the NV concentration from spectral analysis and model the fluorescence response as a function of implantation dose, capturing both the initial increase at low concentrations and a saturation behavior at higher doses due to quenching mechanisms. In contrast, PC diamond membranes show a weaker dependence at low implantation fluences, consistent with pre-existing nitrogen impurities, thus making a statistical model significantly more complex. The activation yield is found to be of order of 1%, which is lower than in N-rich diamond samples, as implanted N is predominantly interstitial. Photoluminescence spectroscopy indicates that NV 0 is the dominant charge state in both materials, with a laser-power-dependent redistribution between neutral and negative charge states. Optically detected magnetic resonance (ODMR) measurements in SC bulk diamond resolve the hyperfine structure and allow extraction of the dephasing time ( T 2 ∗ ), while in PC diamond membranes, where NV centers tend do form near the grain boundaries, the ODMR signals are observed but spectral resolution is currently limited by impurities, grain-dependent NV orientations, and photoluminescence background.
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, 620.3, 630.7, 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 autocorrelation emission functions, by means of Hanbury-Brown and 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 on the polarization of the excitation radiation with ∼45% 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 photophysical 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.
Diamond is a promising platform for the development of technological applications in quantum optics and photonics. The quest for color centers with optimal photo-physical properties has led in recent years to the search for novel impurity-related defects in this material. Here, we report on a systematic investigation of the photo-physical properties of two He-related (HR) emission lines at 535.2 nm and 559.7 nm (as measured at a temperature of 25 K) created in three different diamond substrates upon implantation with 1.3 MeV He+ ions and subsequent annealing. The spectral features of the HR centers were studied in an “optical grade” diamond substrate as a function of several physical parameters, namely, the measurement temperature, the excitation wavelength, and the intensity of external electric fields. The emission lifetimes of the 535.2 nm and 559.7 nm lines were also measured by means of time-gated photoluminescence measurements. The Stark shifting of the HR centers under the application of an external electrical field was observed in a CVD diamond film equipped with buried graphitic electrodes, suggesting the lack of inversion symmetry in the defects' structure. Furthermore, the photoluminescence mapping under 405 nm excitation of a “detector grade” diamond sample implanted at a He+ ion fluence of 1 × 1010 cm−2 enabled us to identify the spectral features of both the HR emission lines from the same localized optical spots. The reported results provide an insight into the structure of He-related defects in diamond and their possible utilization in practical applications.
Nitrogen-vacancy (NV) color centers in diamond are excellent quantum sensors possessing high sensitivity and nano-scale spatial resolution. Their integration in photonic structures is often desired, since it leads to an increased photon emission and also allows the realization of solid-state quantum technology architectures. Here, we report the fabrication of diamond nano-pillars with diameters up to 1000 nm by electron beam lithography and inductively coupled plasma reactive ion etching in nitrogen-rich diamonds (type Ib) with [100] and [111] crystal orientations. The NV centers were created by keV-He ion bombardment and subsequent annealing, and we estimate an average number of NVs per pillar to be 4300 ± 300 and 520 ± 120 for the [100] and [111] samples, respectively. Lifetime measurements of the NVs’ excited state showed two time constants with average values of τ1 ≈ 2 ns and τ2 ≈ 8 ns, which are shorter as compared to a single color center in a bulk crystal (τ ≈ 10 ns). This is probably due to a coupling between the NVs as well as due to interaction with bombardment-induced defects and substitutional nitrogen (P1 centers). Optically detected magnetic resonance measurements revealed a contrast of about 5% and average coherence and relaxation times of T2 [100] = 420 ± 40 ns, T2 [111] = 560 ± 50 ns, and T1 [100] = 162 ± 11 μs, T1 [111] = 174 ± 24 μs. These pillars could find an application for scanning probe magnetic field imaging.
A systematic photoluminescence (PL) investigation of the spectral emission properties of individual optical defects fabricated in diamond upon ion implantation and annealing is reported. Three spectral lines at 620, 631, and 647 nm are identified and attributed to the SnV center due to their occurrence in the PL spectra of the very same single‐photon emitting defects. It is shown that the relative occurrence of the three spectral features can be modified by oxidizing the sample surface following thermal annealing. The relevant emission properties of each class of individual emitters, including the excited state emission lifetime and the emission intensity saturation parameters are reported.