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Giant nonlinear optical effects induced by nitrogen-vacancy centers in diamond crystals

Hidemi Shigekawa, 0000000688, HASE Muneaki, 0000000736, Motojima Mari, Suzuki Takara, Kainuma Yuta, An Toshu

Published Oct 1, 2019• 24 citations
OpenAlex

Abstract

We investigate the effect of nitrogen-vacancy (NV) centers in single crystal diamond on nonlinear optical effects using 40 fs femtosecond laser pulses. The near infrared femtosecond pulses allow us to study purely nonlinear optical effects, such as optical Kerr effect (OKE) and two-photon absorption (TPA), relating to unique optical transitions by electronic structures with NV centers. It is found that both the nonlinear optical effects are enhanced by the introduction of NV centers in the N$^{+}$ dose levels of 2.0$\times$10$^{11}$ and 1.0$\times$10$^{12}$ N$^{+}$/cm$^{2}$. In particular, our data demonstrate that the OKE signal is strongly enhanced for the heavily implanted type-IIa diamond. We suggest that the strong enhancement of the OKE is possibly originated from cascading OKE, where the high-density NV centers effectively break the inversion symmetry near the surface region of diamond.

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Spectrally stable near-surface implanted nitrogen vacancy centers in diamond and the role of surface proximity

Srivatsa Chakravarthi, Christian Pederson, Zeeshawn Kazi +2 more

Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by $^{15}$N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths ($<$ 60 MHz) are observed for the majority of the normal-implant (7$^\circ$, $\approx$ 100 nm deep) $^{15}$NV centers. Long-term stability of the NV$^-$ charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85$^\circ$, $\approx$ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.

•May 20, 2021•0 citations
We investigate the effect of nitrogen-vacancy (NV) centers in single crystal diamond on nonlinear optical effects using 40 fs femtosecond laser pulses. The near infrared femtosecond pulses allow us to study purely nonlinear optical effects, such as optical Kerr effect (OKE) and two-photon absorption (TPA), relating to unique optical transitions by electronic structures with NV centers. It is found that both the nonlinear optical effects are enhanced by the introduction of NV centers in the N+^{+}+ dose levels of 2.0×\times×1011^{11}11 and 1.0×\times×1012^{12}12 N+^{+}+/cm2^{2}2. In particular, our data demonstrate that the OKE signal is strongly enhanced for the heavily implanted type-IIa diamond. We suggest that the strong enhancement of the OKE is possibly originated from cascading OKE, where the high-density NV centers effectively break the inversion symmetry near the surface region of diamond.
Nonlinear optical absorption in commercially available diamond crystals containing nitrogen-vacancy (NV) centers is investigated using femtosecond open-aperture Z-scan measurements at a wavelength of 1032 nm. Experiments were performed on a high-purity electronic-grade diamond and on samples with moderate and high NV concentrations. While the undoped crystal exhibits third-order nonlinear absorption, the NV-doped samples show a pronounced saturable absorption response. To elucidate the microscopic origin of this effect, the Z-scan results are analysed in conjunction with linear transmission spectra, which reveal the presence of additional nitrogen-related defect complexes, including H2 ( NVN−\hbox {NVN}^{-}NVN− ) centers. Although the excitation wavelength is detuned from the principal zero-phonon lines of both NV and H2 defects, it overlaps with the broader near-infrared absorption band associated with vibronic transitions. A quantitative analysis based on an effective two-level model indicates that the observed saturable absorption is most consistently explained by a dominant contribution from H2 defects, while a weaker off-resonant contribution from NV centers cannot be excluded. The extracted parameters, including the linear absorption coefficient and saturation intensity, are supported by a reconstruction of the defect-related absorbance spectrum and by consistency with previously reported nonlinear refractive index data. These results highlight the importance of complex defect environments in determining the nonlinear optical response of NV-doped diamond and provide insight into defect-specific contributions relevant for diamond-based nonlinear and quantum photonic applications.
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.
Scalable realizations of quantum network technologies utilizing the nitrogen-vacancy (NV) center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by 15N^{15}\mathrm{N}15N ion implantation and high-temperature vacuum annealing. The origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near-lifetime-limited optical linewidths (<60MHz)(<60 \mathrm{MHz})(<60MHz) are observed for the majority of the normal-implant (${7}^{\ensuremath{\circ}}$, $\ensuremath{\approx}100$ nm deep) 15NV^{15}\mathrm{NV}15NV centers. Long-term stability of the ${\mathrm{NV}}^{\ensuremath{-}}$ charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion energy, and thus lattice damage profile. In contrast to the normal-implant condition, NVs from an oblique implant (${85}^{\ensuremath{\circ}}$, $\ensuremath{\approx}20$ nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
Diamond color centers such as the nitrogen-vacancy (NV) center have been extensively studied as a popular platform that enables quantum sensing and computing applications. For highly sensitive sensing NV ensembles have significantly stronger signals than individual NV centers and can create strong light fields, which are also essentially required by novel concepts that need a large sensing volume, such as cavity coupling and readout, laser threshold magnetometry and multi-pass geometries. On top of strong signals, low optical material losses are the other key consideration for these techniques, by means of low optical absorption of signal light and low birefringence of the diamond crystal. In this work, we study systematically the behavior of absorption in the NV emission range around 700nm and birefringence with increasing nitrogen- and NV-doping, as well as their behavior during NV creation via diamond growth, electron beam irradiation and annealing treatments. Absorption correlates with increased nitrogen-doping yet single substitutional nitrogen atoms (Ns0 or P1 centers) do not seem to be the direct absorber. The high nitrogen doping level in the growth leads to high absorption in the whole UV-Vis range, which is the main contributors to the high absorption at 700 nm. When treating the diamond for an enhanced NV concentration, ‘over irradiating’ the diamond with too high fluence is harmful in the sense of creating neutral vacancies that increase absorption at the wavelength range of interest. Opposite to the absorption, birefringence reduces with increasing nitrogen doping and shows better homogeneity. After-growth treatments show a minor and if any a positive (i.e. reducing) influence on diamond birefringence. Multiple crystal defect concentrations and their changes are identified via absorption spectroscopy during the material processing steps and thus we identify potential causes of absorption and birefringence. From this we suggest strategies to fabricate CVD diamonds with high NV density yet low absorption and low birefringence
Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by 15^{15}15N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths (<<< 60 MHz) are observed for the majority of the normal-implant (7∘^\circ∘, ≈\approx≈ 100 nm deep) 15^{15}15NV centers. Long-term stability of the NV−^-− charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85∘^\circ∘, ≈\approx≈ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.