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Journal of Physics Conference Series

Peculiarities of optical and ODMR Spectra of Nitrogen–Vacancy Color Centers in Diamond Crystals

Alexander K. Dmitriev, Anton K. Vershovskii

Published Oct 27, 2014• 2 citations
Publisher

Abstract

The optical and ODMR spectra of nitrogen vacancy (NV) centers in diamond were investigated as applied to the development of micro-scale diamond magnetometer sensor. It is shown that the NV 0 center (unlike the NV − center) has an absorption line in the UV range. The inversion of the zero phonon line of the NV − center was observed and explained. ODMR signals in high magnetic fields (as compared with inner fields in the crystal) as well as in weak fields also were investigated. We propose the solution to the problem of the magnetometer sensitivity reduction at low magnetic field, that is of interest for quantum magnetometry applications.

DOI
10.1088/1742-6596/541/1/012090

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•Sep 11, 2023•0 citations
The optical and ODMR spectra of nitrogen vacancy (NV) centers in diamond were investigated as applied to the development of micro-scale diamond magnetometer sensor. It is shown that the NV 0 center (unlike the NV − center) has an absorption line in the UV range. The inversion of the zero phonon line of the NV − center was observed and explained. ODMR signals in high magnetic fields (as compared with inner fields in the crystal) as well as in weak fields also were investigated. We propose the solution to the problem of the magnetometer sensitivity reduction at low magnetic field, that is of interest for quantum magnetometry applications.
Magnetometry with nitrogen-vacancy (NV) centers in diamond has shown great promise in recent years. In particular, absorption-based magnetometry techniques, employing a cavity to enhance the absorption length, can improve the contrast and sensitivity compared to conventional techniques based on reading out the NV−^-− triplet fluorescence. The absorption techniques rely on magnetic-field-dependent absorption at the NV−^-− singlet zero phonon line at 1042 \,nm and its phonon sideband. In a cavity-enhanced spectroscopy approach, we study pump-laser- and microwave-induced cavity signal changes at room temperature over a spectral range of 680-1050 \,nm. Through normalization, we eliminate the cavity-enhancement effect and provide quasi-single-pass values for the absorption and optically detected magnetic resonance (ODMR) contrast. The highest contrast is found at 1042 \,nm, but multiple points of high contrast are found at the peaks of the phonon sideband. Additionally, cavity-enhanced ODMR contrasts in the range of 50-80 %\,\%% are presented. We further measure the broadband singlet absorption cross section at room temperature with a novel method through microwave-induced signal changes. This method is insensitive to pump-laser-induced signal changes by other defects and quantifies the room-temperature absorption strength of the singlet transition and its entire phonon sideband. We determine the absorption cross section at 1042 \,nm to be σ1042 ★=(0.89±0.14)⋅10−21 m2σ^{\,\bigstar}_{1042}=(0.89\pm0.14)\cdot 10^{-21}\,\text{m}^2σ1042★​=(0.89±0.14)⋅10−21m2 or σ1042 ▲=(2.9±0.5)⋅10−21 m2σ^{\,\blacktriangle}_{1042}=(2.9\pm0.5)\cdot 10^{-21}\,\text{m}^2σ1042▲​=(2.9±0.5)⋅10−21m2. depending on the employed 532 \,nm NV−^-− absorption cross section.
Nitrogen Vacancy (NV) centers are point defects in diamond that allow magnetic field sensing based on Optically Detected Magnetic Resonance (ODMR). They are processed in ultrapure single-domain CVD grown diamond crystals and can be operated at room temperature. This results in solid-state sensors with a wide variety of applications. Ensemble of NV centers can be used to perform wide-field magnetic imaging with sensitivity in the nT range. Single NV centers can also be processed, which allows sensing at the atomic scale. This possibility, combined with its unique coherence properties, make NV center an ideal candidate for quantum sensing.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.
Magnetometry with nitrogen-vacancy (NV) centers in diamond has so far been measured via emission of light from NV centers or via absorption at the singlet transition at 1042 nm. Here, we demonstrate a phenomenon of broadband optical absorption by the NV centers starting in the emission wavelength and reaching up to 1000 nm. The measurements are enabled by a high-finesse cavity, which is used for room-temperature continuous wave pump-probe experiments. The red to infrared probe beam shows the typical optically detected magnetic resonance (ODMR) signal of the NV spin with contrasts up to 42 %. This broadband optical absorption has not yet been reported in terms of NV magnetometry. We argue that the lower level of the absorbing transition could be the energetically lower NV singlet state, based on the increased optical absorption for a resonant microwave field and the spectral behavior. Investigations of the photon-shot-noise-limited sensitivity show improvements with increasing probe wavelength, reaching an optimum of 7.5pT/Hz. The results show significantly improved ODMR contrast compared to emission-based magnetometry. This opens a new detection wavelength regime with coherent laser signal detection for high-sensitivity NV magnetometry.
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