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Applied Physics Letters

Magnetometry based on the excited-state lifetimes of a single nitrogen-vacancy center in diamond

Felix M. Stürner, Yan Liu, Pierre-Olivier Colard, Matthew Markham, Fedor Jelezko

Published Sep 27, 2021• 25 citations
Publisher

Abstract

So far most well-established quantum sensing techniques based on the negatively charged nitrogen-vacancy (NV) center in diamond utilize the recorded fluorescence intensity to detect the electronic spin states. However, the fluorescence intensity of a NV center is not only dependent on its spin state, but also affected by measurement issues, such as fluctuations of the excitation laser power and charge state transformation of the NV center. Instabilities in terms of output power or polarization changes in the laser source as well as sample drifts during a measurement are common factors that weaken the precision. Here, we demonstrate proof-of-principle of a sensing method making use of the excited-state lifetimes of a NV center for magnetometry experiments.

DOI
10.1063/5.0070639

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So far most well-established quantum sensing techniques based on the negatively charged nitrogen-vacancy (NV) center in diamond utilize the recorded fluorescence intensity to detect the electronic spin states. However, the fluorescence intensity of a NV center is not only dependent on its spin state, but also affected by measurement issues, such as fluctuations of the excitation laser power and charge state transformation of the NV center. Instabilities in terms of output power or polarization changes in the laser source as well as sample drifts during a measurement are common factors that weaken the precision. Here, we demonstrate proof-of-principle of a sensing method making use of the excited-state lifetimes of a NV center for magnetometry experiments.
We propose and experimentally demonstrate a method to strongly increase the sensitivity of spin measurements on nitrogen-vacancy (NV) centers in diamond, which can be readily implemented in existing quantum sensing experiments. While charge state transitions of this defect are generally considered a parasitic effect to be avoided, we show here that these can be used to significantly increase the NV center's spin contrast, a key quantity for high sensitivity magnetometry and high fidelity state readout. The protocol consists of a two-step procedure, in which the charge state of the defect is first purified by a strong laser pulse, followed by weak illumination to obtain high spin polarization. We observe a relative improvement of the readout contrast by 17 %, and infer a reduction of the initialization error of more than 50 %. The contrast enhancement is accompanied by a beneficial increase of the readout signal. For long sequence durations, typically encountered in high-resolution magnetometry, a measurement speedup by a factor of >1.5 is extracted, and we find that the technique is beneficial for sequences of any duration. Additionally, our findings give detailed insight into the charge and spin polarization dynamics of the NV center, and provide actionable insights for direct optical, spin-to-charge, and electrical readout of solid-state spin centres.
The electron spin of the negatively charged the nitrogen vacancy center $({\mathrm{NV}}^{\ensuremath{-}}$) in diamond can be optically polarized through intersystem crossing, which enables the defect to be used for quantum computation and metrology. In this work, we studied the electron spin depolarization effect of the NV center induced by charge state conversion, which was proven to be a spin-independent process. The spin-state initialization fidelity was largely affected by the charge state conversion process. As a result, the optical polarization of the electron spin decreased about 1414%(31%14) with a high-power continuous-wave (pulsed) green laser. Moreover, the undefined fluorescence anomalous saturation effect of the NV center was analyzed and explained in detail based on the spin depolarization. The results demonstrated that a weak laser should be used for initialization of the NV center. In addition, the power and polarization of a laser for NV spin detection should be carefully adjusted to obtain the highest fluorescence signal. Our work also provided information that can increase the understanding of the charge state conversion and spin polarization processes of the NV center for quantum information and sensing.
The nitrogen-vacancy (NV) center in diamond enables optical initialization and readout of its electronic spin, forming the basis of a wide range of quantum sensing and metrology applications. A central challenge in such measurements is the coexistence of two charge states, NV- and NV0: While detection protocols rely on the spin-dependent properties of NV-, fluorescence from NV0 does not carry useful contrast and is typically removed as background, reducing the available signal. Here, we show that the origin of NV0 emission depends strongly on the excitation wavelength in nitrogen-containing diamond. Using ensembles of NV centers with varying nitrogen concentrations, we compare excitation at the NV0 zero-phonon line (ZPL) at 575 nm with the commonly used 532 nm. We find that excitation at 575 nm generates NV0 predominantly through spin-selective tunneling from the excited state of NV- to nearby nitrogen donors, such that the NV0 emission follows the spin polarization of NV-. As a result, the NV0 fluorescence contributes to the measurable spin contrast, allowing the full fluorescence signal to be used for detection. This result opens opportunities for improved sensitivity in NV-based sensing applications.
Nitrogen vacancy (NV) centers in diamond have attracted considerable recent interest for use in quantum sensing, promising increased sensitivity for applications ranging from geophysics to biomedicine. Conventional sensing schemes involve monitoring the change in red fluorescence from the NV center under green laser and microwave illumination. Due to the strong fluorescence background from emission in the NV triplet state and low relative contrast of any change in output, sensitivity is severely restricted by a high optical shot noise level. Here, we propose a means to avoid this issue, by using the change in green pump absorption through the diamond as part of a semiconductor external cavity laser run close to the lasing threshold. We show that theoretical sensitivity to the magnetic field on the pT/Hz\sqrt{\mathrm{Hz}}Hz​ level is possible using a diamond with an optimal density of NV centers. We discuss the physical requirements and limitations of the method, particularly the role of amplified spontaneous emission near threshold and explore realistic implementations using current technology.
The nitrogen vacancy (NV) center in diamond is a versatile color center used for magnetometry, quantum computing, and quantum communications. In this article, using a single laser beam as a pump and probe, we measure the spin states of the NV center using the Faraday effect and use such measurements to develop a novel magnetic field sensor. Using the spin-state-dependent effect on the left and right circularly polarized light, we probe and confirm the existence of spin-orbit coupling in the NV center at room temperature. The sensitivity of our magnetometer is 350 350~350 nT/Hz\sqrt{Hz}Hz​, limited by the background produced by the laser trapped inside the diamond. We argue that by using an optical cavity and a high-purity diamond, sensitivities in the femtotesla level can be achieved.
The negatively charged nitrogen vacancy center in diamond is widely used for quantum sensing due to the sensitivity of the spin triplet in the electronic ground state to external perturbations such as strain and electromagnetic fields, which makes it an excellent probe for changes in these perturbations.The spin state can be measured through optically detected magnetic resonance, which is most commonly achieved by detecting the photoluminescence after exciting the spin-triplet transition.Recently, methods have been proposed and demonstrated that use the absorption of the infrared singlet transition at 1042 nm instead.These methods, however, require cryogenic temperatures or external cavities to enhance the absorption signal.Here, we report on our efforts to optimize the magnetometer sensitivity at room temperature and without cavities.We reach a sensitivity of 18 pT/ √ Hz, surpassing previously reported values, and a calculated shot-noise limit of 5 pT/ √ Hz .We also report on a defect that is native to diamond grown by chemical vapor deposition and thus absent in high-pressure high-temperature diamond, the excitation of which impacts the measured singlet absorption signal.