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Optics Express

Fabrication of nitrogen vacancy color centers by femtosecond pulse laser illumination

Yan Liu, Gengxu Chen, Min Suk Song, Xueting Ci, Botao Wu, E Wu, Heping Zeng

Published May 17, 2013• 64 citations
Publisher

Abstract

We report on a novel method to fabricate single, multiple and large-area high-density ensembles of nitrogen vacancy (NV) color centers in synthetic type Ib bulk diamond by femtosecond laser illumination. Electron beams generated in propagation of intense infrared laser pulses in air sputtered on a diamond sample under high temperature aroused by the laser illumination, creating NV color centers. Typical photoluminescence (PL) spectra of NV centers could be observed on the illuminated spots. Photon streams from individual photoluminescent points exhibited anti-bunching effect by the second-order correlation measurement, evidencing single and multiple photon-emitters around the laser illuminated spots.

DOI
10.1364/oe.21.012843

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We report on a novel method to fabricate single, multiple and large-area high-density ensembles of nitrogen vacancy (NV) color centers in synthetic type Ib bulk diamond by femtosecond laser illumination. Electron beams generated in propagation of intense infrared laser pulses in air sputtered on a diamond sample under high temperature aroused by the laser illumination, creating NV color centers. Typical photoluminescence (PL) spectra of NV centers could be observed on the illuminated spots. Photon streams from individual photoluminescent points exhibited anti-bunching effect by the second-order correlation measurement, evidencing single and multiple photon-emitters around the laser illuminated spots.
Nitrogen-vacancy (NV) centers in diamond are expected to be quantum sensing devices such as magnetic and electric fields, temperature, pressure and so on. The generation of NV centers by irradiations of femtosecond laser pulses has been reported. Femtosecond laser can write NV centers in diamond directly and this direct writing can realize a flexible spatial arrangement of NV centers. As the application of the laser system, we have constructed the femtosecond laser irradiation platform for creating the quantum sensing device, such as NV centers. The femtosecond laser pulse is focused on a sample surface by an objective lens and laser pulse intensity is controlled by attenuators. By use of this irradiation apparatus, we have irradiated diamond samples to create NV centers. We could confirm several graphitization spots, but the signal intensity from NV center did not exist. To use the irradiation platform for creating NV centers in diamond, it needs some improvement, more increasing the repetition rate of irradiation laser and/or impurity nitrogen density in diamond sample.
Diamond nanocrystals containing nitrogen–vacancy (NV) color centers have been used in recent years as fluorescent probes for near-field and cellular imaging. In this work, we report that an infrared (IR) pulsed excitation beam can quench the photoluminescence of a NV color center in a diamond nanocrystal (size <50 nm) with an extinction ratio as high as ≈90%. We attribute this effect to the heating of the nanocrystal consecutive to multi-photon absorption by the diamond matrix. This quenching is reversible: the photoluminescence intensity goes back to its original value when the IR laser beam is turned off, with a typical response time of 100 ps, allowing for fast control of NV color center photoluminescence. We used this effect to achieve the sub-diffraction-limited imaging of fluorescent diamond nanocrystals on a coverglass. For that, as in the ground state depletion super-resolution technique, we combined the green excitation laser beam with the control IR depleting one after shaping its intensity profile in a doughnut form, so that the emission comes only from the sub-wavelength size central part.
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.
High-density nitrogen-vacancy (NV) centers exceeding 1016/cm3 inside a diamond can be achieved by femtosecond laser irradiation. The number of pulses and pulse energy were adjusted considering the increasing trend of the NV concentration and damage generation. The NV concentration first grew as the number of laser pulses was increased, and then the concentration was temporarily saturated or decreased. By increasing the number of laser pulses more than 2.5–5 × 107, the concentration increased again. The Hahn-echo measurement revealed that electron spins of the substitutional nitrogen center (P1) were dominant source for decoherence and the number of paramagnetic defects induced by the laser irradiation was not significant for degradation of spin coherence of the laser-induced NV centers even without a post-annealing process. Such high-dense ensemble NV centers are crucial for a high-sensitive quantum sensor.
Defects in diamond have evolved as unique object for their potential application for Optical imaging and Nano-photonics. High pressure high temperature (HPHT) grown type-Ib diamond particles were milled down to the size of ~ 80 nm and purified to remove iron & graphitic carbon impurities and irradiated with 35 KeV He+ ions to create vacancies in the diamond lattice. Vacancies diffuse close to substitutional nitrogen impurities of nano-diamond particles upon thermal treatment. Characteristic sharp emission of NV centers were observed at 575.5 nm and 637.9 nm corresponding to NV° and NV− charged states in addition to a broad emission in the range 550-750 nm. Structural and photo-physical behavior of these fluorescent diamonds was found to depend on the method of purification adopted. Samples purified through acid reflux were found suitable for bio-imaging applications while, sample purified through air oxidation shows properties desirable for Nano-photonic applications. Photon-correlation measurements of emission from individual diamond nanoparticles using Hanbury Brown and Twiss interferometer (HBT) shows anti-bunching curve with g2(t)= 0 confirming their suitability as single photon source. Such sources of indistinguishable photons are highly desirable for quantum computation and quantum optics applications.
Diamond nanocrystals containing highly photoluminescent color centers are attractive, nonclassical, and near-field light sources. For near-field applications, the size of the nanocrystal is crucial, since it defines the optical resolution. Nitrogen-vacancy (NV) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamonds with sizes down to 25 nm can hold a single NV color center with bright and stable photoluminescence.