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Applied Physics Letters

Narrow-linewidth diamond single-photon sources prepared via femtosecond laser

Si Jian Gao, Si‐Yu Yin, Zhaoxin Liu, Zongda Zhang, Zhen‐Nan Tian, Qi‐Dai Chen, Nian‐Ke Chen, Hong‐Bo Sun

Published Jan 10, 2022• 16 citations
Publisher

Abstract

Nitrogen-vacancy (NV) color centers in diamonds with narrow optical linewidths are commonly used as solid-state single-photon sources that emit indistinguishable photons. However, NV color centers prepared using ion implantation typically have large optical linewidths of over 100 MHz. Herein, we used the femtosecond laser direct writing (FsLDW) technique to prepare single NV color centers in diamond with a narrow optical linewidth of 13.05 ± 0.2 MHz and a long decoherence time of 445 ± 27.6 μs. In addition, the density functional theory was adopted to establish calculation models and illustrate why single NV color centers prepared by FsLDW have narrower linewidths compared to those of the ion implantation method. Thus, this study provides an effective reference for the preparation of narrow-linewidth single-color centers in diamonds and other wide-gap crystals.

DOI
10.1063/5.0079335

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Nitrogen-vacancy (NV) color centers in diamonds with narrow optical linewidths are commonly used as solid-state single-photon sources that emit indistinguishable photons. However, NV color centers prepared using ion implantation typically have large optical linewidths of over 100 MHz. Herein, we used the femtosecond laser direct writing (FsLDW) technique to prepare single NV color centers in diamond with a narrow optical linewidth of 13.05 ± 0.2 MHz and a long decoherence time of 445 ± 27.6 μs. In addition, the density functional theory was adopted to establish calculation models and illustrate why single NV color centers prepared by FsLDW have narrower linewidths compared to those of the ion implantation method. Thus, this study provides an effective reference for the preparation of narrow-linewidth single-color centers in diamonds and other wide-gap crystals.
The nitrogen-vacancy center (NV) in diamond, with its exceptional spin coherence and convenience in optical spin initialization and readout, is increasingly used both as a quantum sensor and as a building block for quantum networks. Employing photonic structures for maximizing the photon collection efficiency in these applications typically leads to broadened optical linewidths for the emitters, which are commonly created via nitrogen ion implantation. With studies showing that only native nitrogen atoms contribute to optically coherent NVs, a natural conclusion is to either avoid implantation completely or substitute nitrogen implantation by an alternative approach to vacancy creation. Here, we demonstrate that implantation of carbon ions yields a comparable density of NVs as implantation of nitrogen ions and that it results in NV populations with narrow optical linewidths and low charge-noise levels even in thin diamond microstructures. We measure a median NV linewidth of 150 MHz for structures thinner than 5 μm, with no trend of increasing linewidths down to the thinnest measured structure of 1.9 μm. We propose a modified NV creation procedure in which the implantation is carried out after instead of before the diamond fabrication processes and confirm our results in multiple samples implanted with different ion energies and fluences.
High Resolution Image Download MS PowerPoint Slide We report on pulsed-laser-induced generation of nitrogen-vacancy (NV) centers in diamond facilitated by a solid-immersion lens (SIL). The SIL enables laser writing at energies as low as 5.8 nJ per pulse and allows vacancies to be formed close to a diamond surface without inducing surface graphitization. We operate in the previously unexplored regime, where lattice vacancies are created following tunneling breakdown rather than multiphoton ionization. We present three samples in which NV center arrays were laser-written at distances between ∼1 and 40 μm from a diamond surface, all presenting narrow distributions of optical linewidths with means between 62.1 and 74.5 MHz. The linewidths include the effect of long-term spectral diffusion induced by a 532 nm repump laser for charge-state stabilization, thereby emphasizing the particularly low-charge-noise environment of the created color centers. Such high-quality NV centers are excellent candidates for practical applications employing two-photon quantum interference with separate NV centers. Finally, we propose a model for disentangling power broadening from inhomogeneous broadening in the NV center optical linewidth.
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.
The negatively charged nitrogen-vacancy (NV) center in diamond is among the most promising solid-state systems implementations of a quantum bit. However, integration of the NV center into any efficient photonic environment requires microstructuring the diamond at below-micrometer scale. Preserving the low NV zero-phonon line inhomogeneous broadening during this process is a major challenge with standard NV creation methods. This issue severely limits practical applications of NV centers. Initial studies on pulsed-laser assisted creation of NVs yielded promising results by creating NVs with low inhomogeneous broadening at desired spatial locations in diamond [1]. Crucially, the lattice damage resulting from implantation of energetic ions was avoided. However, the method relied on a narrow window of parameters for successful writing. We widen this window by using a solid immersion lens (SIL), which facilitates laser writing over a broad range of pulse energies and allows for vacancy formation close to a diamond surface without inducing surface graphitization. We operate in the previously unexplored regime where lattice vacancies are created following tunneling breakdown rather than multiphoton ionization [2]. We present NV arrays that have been created between 1 and 40 µm from a diamond surface, all presenting optical linewidth distributions with means as low as 61.0±22.8 MHz [2], including spectral diffusion induced by off-resonant repump for charge stabilization. This emphasizes the exceptionally low charge-noise environment of laser-written NVs. Such high-quality NV centers are excellent candidates for practical applications employing two-photon quantum interference with separate NV centers. Finally, we propose a model for disentangling power broadening from inhomogeneous broadening in the NV zero-phonon line optical linewidth [2]. [1] Y.-C. Chen, P. S. Salter, S. Knauer, … and J. M. Smith, Nat. Photonics 11, 77 (2017). [2] V. Yurgens, J.A Zuber, S. Flågan, M. De Luca, B.J. Shields, I. Zardo, P. Maletinsky, R.J. Warburton, and T. Jakubczyk, ACS Photonics 8, 1726–1734 (2021)
Nitrogen-vacancy (NV) centers in diamond with coherent optical transitions are a promising candidate for quantum science and technology protocols. A widely used strategy for their creation is nitrogen-ion implantation and high-temperature annealing. The data presented in this work show that while low-strain, narrow-optical-linewidth NV centers are formed from naturally occurring 14{}^{14}14N atoms, NV centers formed from the implanted 15{}^{15}15N atoms show broadened optical transitions and experience higher strain. These results have immediate implications for the positioning accuracy of current NV center creation protocols.
The development of material-processing techniques that can be used to generate optical diamond nanostructures containing a single-color center is an important problem in quantum science and technology. In this work, we present the combination of ion implantation and top-down diamond nanofabrication in two scenarios: diamond nanopillars and diamond nanowires. The first device consists of a 'shallow' implant (∼20 nm) to generate nitrogen-vacancy (NV) color centers near the top surface of the diamond crystal prior to device fabrication. Individual NV centers are then mechanically isolated by etching a regular array of nanopillars in the diamond surface. Photon anti-bunching measurements indicate that a high yield (>10%) of the devices contain a single NV center. The second device demonstrates 'deep' (∼1 μm) implantation of individual NV centers into diamond nanowires as a post-processing step. The high single-photon flux of the nanowire geometry, combined with the low background fluorescence of the ultrapure diamond, allowed us to observe sustained photon anti-bunching even at high pump powers.