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Optoelectronics Instrumentation and Data Processing

Raman and ODMR Spectroscopy of NV Centers in Nanolayers and Nanopillars of $$\mathbf{{\langle 111\rangle}}$$ Diamond after Etching with a Focused Beam of Ga Ions

I. A. Kartashov, Sergey N. Podlesny, Valentin A. Antonov, V. P. Popov, Yuri N. Palyanov

Published Dec 1, 2023• 0 citations
Publisher

Abstract

The spectral characteristics of the optically detected magnetic resonance of negatively charged nitrogen–vacancy (NV $${}^{-}$$ ) centers in synthetic diamonds and nanopillars on their surface formed by a focused Ga $${}^{+}$$ ion beam, when the lower spin sublevels are populated with microwave radiation, are studied. In the course of studies for emerging spin resonances at different values of the external magnetic field, both a significant decrease in the gyromagnetic ratio and a significant drop in the photoluminescence contrast are revealed for the directions of the NV $${}^{-}$$ centers inclined to the axis of the nanopillars due to residual defects from ion etching recorded on Raman spectra in the form of peaks from amorphous carbon and graphite and the stresses they create.

DOI
10.3103/s8756699023060067

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Raman and ODMR Spectroscopy of NV Centers in Nanolayers and Nanopillars of ⟨111⟩\mathbf{{\langle 111\rangle}}⟨111⟩ Diamond after Etching with a Focused Beam of Ga Ions
The spectral characteristics of the optically detected magnetic resonance of negatively charged nitrogen–vacancy (NV −{}^{-}− ) centers in synthetic diamonds and nanopillars on their surface formed by a focused Ga +{}^{+}+ ion beam, when the lower spin sublevels are populated with microwave radiation, are studied. In the course of studies for emerging spin resonances at different values of the external magnetic field, both a significant decrease in the gyromagnetic ratio and a significant drop in the photoluminescence contrast are revealed for the directions of the NV −{}^{-}− centers inclined to the axis of the nanopillars due to residual defects from ion etching recorded on Raman spectra in the form of peaks from amorphous carbon and graphite and the stresses they create.
The nanolayers and nanomembranes with the 30–300 thickness and the 0.5 ppm NV– center content were produced by 50 keV H2+{\text{H}}_{2}^{ + }H2+​ ion implantation in Ib type (111) diamond plates and vacuum or high pressure annealing with subsequent lift-off process. The similar NV– content nanolayers were formed by N+ ion implantation in IIa type (111) diamond plates and similar annealings. 〈111〉 oriented nanopillars were produced on both types of nanolayers using focused ion beam (FIB) with Ga+ 30 keV maskless milling. The unusual optically detected magnetic resonances (ODMRs) were measured in a single nanopillars with a height of 500‒700 nm and of 250 nm in diameter covered by an amorphous a-C:Ga nanolayer in the 0‒20 G magnetic field. They demonstrated both a significant decrease in the gyromagnetic ratio and the quenching of photoluminescence (PL) signal from the NV– centers inclined to the nanopillar axis by the conductive a‑C:Ga nanolayer and stresses created by it. The multistep O2 RIE plasma etching restored the normal ODMR resonance frequencies and intensities for all four NV–center orientations in (111) diamond nanopillars.
Abstract The diamond nitrogen-vacancy center with a negative charge (NV−) exhibits exceptional optical properties and enables highly sensitive detection of multiple physical quantities. The development of a simple and efficient method for fabricating NV− centers in diamonds holds significant importance in promoting their widespread application. The fabrication method of NV− centers is explored in this work, utilizing high-energy photons emitted by argon ions to induce vacancies in type Ia diamond substrates. The processed samples are optical characterized, and the characteristic peak and zero phonon line corresponding to the NV− center can be observed in Raman and photoluminescence spectra respectively. The concentration of NV− centers in samples could reach up to 153.9 ppb, estimated by integrating the fluorescence intensity of the photoemission spectrum. The samples exhibit the spin characterization of NV− centers, which achieve a maximum contrast of 1.5% in the optical detection magnetic resonance (ODMR) spectra.
Shallow, negatively-charged Nitrogen-Vacancy centers (NV-) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV0 centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm2). Raman spectroscopy, optically-detected-magnetic-resonance (ODMR) and charge-photoconversion fluorescence detection are applied to characterize the properties and dynamics of NV- and NV0 centers. We demonstrate that high laser power strongly promotes photoconversion of NV0 to NV- centers. Surprisingly, the excess NV- population is stable over a time scale of one hundred milliseconds after switching off the laser, resulting in long-lived enrichment of shallow NV-. The beneficial effect of photoconversion is less marked in nanostructured samples. Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV- centers in diamond.
Negatively charged nitrogen-vacancy (NV) centers and other color centers in diamonds have emerged as promising platforms for quantum communication, quantum information processing, and nanoscale sensing, owing to their long spin coherence times, fast spin control, and efficient photon coupling. Deterministic placement of individual color centers into nanophotonic structures is critical for scalable device integration, and ion implantation is the most viable technique. Nanofabrication processes, including diamond etching, are essential to realize these structures but can introduce crystal strain through lattice damage. In this work, we investigate the impact of ion implantation and nanofabrication-induced strain on the electronic spin levels of NV-centers. We demonstrate that the zero-field continuous-wave optically detected magnetic resonance (CW-ODMR) spectroscopy serves as a sensitive probe of local crystal strain. We report the presence of a shear strain feature in diamond substrates arising from the ion-implantation and nanofabrication processes, as evidenced by the asymmetric splitting black observed in the zero-field CW-ODMR spectrum of NV-centers.
Etching experiments were performed that reveal the vertical distribution of optically active nitrogen-vacancy (NV) centers in diamond created in close proximity to a surface through ion implantation and annealing. The NV distribution depends strongly on the native nitrogen concentration, and spectral measurements of the neutral and negatively charged NV peaks give evidence for electron depletion effects in lower-nitrogen material. The results are important for potential quantum information and magnetometer devices where NV centers must be created in close proximity to a surface for coupling to optical structures.