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arXiv:1702.05332 · Applied Physics Letters

Enhanced concentrations of nitrogen-vacancy centers in diamond through TEM irradiation

Demitry Farfurnik, Nir Alfasi, Sergei Masis, Yaron Kauffmann, E. Farchi, Yoav Romach, Yonatan Hovav, Eyal Buks, Nir Bar‐Gill

Published Sep 18, 2017• 46 citations
arXivHTMLPDF

Abstract

The studies of many-body dynamics of interacting spin ensembles, as well as quantum sensing in solid state systems, are often limited by the need for high spin concentrations, along with efficient decoupling of the spin ensemble from its environment. In particular, for an ensemble of nitrogen-vacancy (NV) centers in diamond, high conversion efficiencies between nitrogen (P1) defects and NV centers are essential while maintaining long coherence times of an NV ensemble. In this work, we study the effect of electron irradiation on the conversion efficiency and the coherence time of various types of diamond samples with different initial nitrogen concentrations. The samples were irradiated using a 200 keV transmission electron microscope. Our study reveals that the efficiency of NV creation strongly depends on the initial conversion efficiency and on the initial nitrogen concentration. The irradiation of the examined samples exhibits an order of magnitude improvement in the NV concentration (up to ∼1011 NV/cm2), without degradation in their coherence time of ∼180 μs. We address the potential of this technique toward the study of many-body physics of NV ensembles and the creation of non-classical spin states for quantum sensing.

DOI
10.1063/1.4993257

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The studies of many-body dynamics of interacting spin ensembles, as well as quantum sensing in solid state systems, are often limited by the need for high spin concentrations, along with efficient decoupling of the spin ensemble from its environment. In particular, for an ensemble of nitrogen-vacancy (NV) centers in diamond, high conversion efficiencies between nitrogen (P1) defects and NV centers are essential while maintaining long coherence times of an NV ensemble. In this work, we study the effect of electron irradiation on the conversion efficiency and the coherence time of various types of diamond samples with different initial nitrogen concentrations. The samples were irradiated using a 200 keV transmission electron microscope. Our study reveals that the efficiency of NV creation strongly depends on the initial conversion efficiency and on the initial nitrogen concentration. The irradiation of the examined samples exhibits an order of magnitude improvement in the NV concentration (up to ∼1011 NV/cm2), without degradation in their coherence time of ∼180 μs. We address the potential of this technique toward the study of many-body physics of NV ensembles and the creation of non-classical spin states for quantum sensing.
We describe experimental steps toward the observation of many-body dynamics in optically-addressable spin ensembles (NV centers) in diamond. We study the effect of electron irradiation using a 200 keV transmission electron microscope (TEM) on the conversion efficiency and the coherence times of various types of diamond samples with different initial nitrogen concentrations. Using fluorescence images obtained by confocal microscopy, we observe an order of magnitude improvement in the NV concentration (up to ~1011 NV/cm2), without any degradation in their coherence times of ~180 μs (for a Hahn-Echo experiment). We address the potential of this technique for studying many-body physics of ensembles of NV spins: our simulations show that by implementing a simple dynamical decoupling protocol, dipolar interactions could be distinguished from ordinary interactions with the spin-bath environment. These outcomes could contribute to the creation of non-classical spin states, e.g. for quantum sensing.
The study of quantum many-body spin physics in realistic solid-state platforms has been a long-standing goal in quantum and condensed-matter physics. We demonstrate separate steps required to reach this goal using nitrogen-vacancy (NV) centers in diamond. First, standard (TEM) electron irradiation is used for the enhancement of N to NV conversion efficiencies by over an order-of-magnitude. Second, robust pulsed and continuous dynamical decoupling (DD) techniques enable the preservation of arbitrary states of the ensemble. These combined efforts could lead to the desired interaction-dominated regime. Finally, we simulate the effects of continuous and pulsed microwave (MW) control on the resulting NV-NV many body dynamics in a realistic spin-bath environment. We emphasize that dominant interaction sources could be identified and decoupled by the application of proper pulse sequences, and the modification of such sequences could lead to the creation engineered interaction Hamiltonians. Such interaction Hamiltonians could pave the way toward the creation of non-classical states, e.g. spin-squeezed states, which were not yet demonstrated in the solid-state, and could eventually lead to magnetic sensing beyond the standard quantum limit (SQL).
Abstract The nitrogen-vacancy (NV) center in diamond is a promising quantum system for magnetometry applications exhibiting optical readout of minute energy shifts in its spin sub-levels. Key material requirements for NV ensembles are a high NV − concentration, a long spin coherence time and a stable charge state. However, these are interdependent and can be difficult to optimize during diamond growth and subsequent NV creation. In this work, we systematically investigate the NV center formation and properties in bulk chemical vapor deposition (CVD) diamond. The nitrogen flow during growth is varied by over four orders of magnitude, resulting in a broad range of single substitutional nitrogen concentrations of 0.2–20 parts per million. For a fixed nitrogen concentration, we optimize electron-irradiation fluences with two different accelerated electron energies, and we study defect formation via optical characterizations. We discuss a general approach to determine the optimal irradiation conditions, for which an enhanced NV concentration and an optimum of NV charge states can both be satisfied. We achieve spin–spin coherence times T 2 ranging from 45.5 to 549 μ s for CVD diamonds containing 168 to 1 parts per billion NV − centers, respectively. This study shows a pathway to engineer properties of NV-doped CVD diamonds for improved sensitivity.
We systematically investigate the NV center creation and properties in bulk chemical vapor deposition (CVD) diamond, throughout growth, electron-beam irradiation, and annealing steps. We study diamond series grown with a varying nitrogen flow over 4 orders of magnitude, resulting in a broad range of single substitutional nitrogen (P1 center) densities from 0.2 to 20 ppm. We investigate in-situ P1 and NV creations, as well as NV charge states distributions. As the next step, we optimize electron-irradiation fluences for a fixed nitrogen concentration, with two different accelerated electron energies. We bring up a general approach to determine the optimal irradiation conditions, and discuss criteria for P1 to NV conversion ratios in the context of stable NV charge states. Through all these optimizations, we enhance the NV- concentration remarkably in our CVD diamond samples, without sacrificing their Hahn-echo coherence time T2. We achieve NV concentrations from 1 to 168 ppb with T2 from 549 to 45.5 µs respectively. This study shows a pathway to engineer targeted, optimized properties of NV-ensembles in bulk CVD diamonds for improved sensitivity.
Abstract A nitrogen vacancy (NV) center in diamond is a promising platform for the study of quantum sensing and quantum many-body physics. It is essential for such study to realize a system in which NV centers interact with one another. This requires the fabrication of highly concentrated NV centers, as the centers must exist within a few nanometers of one another. Only a few such samples have been fabricated, because the required irradiation of several-MV electron beams over long periods makes such sample preparation difficult. Here, highly concentrated NV ensembles ([NV] = 8.5 × 1018 cm-3) were created by narrowing the electron beam of a transmission electron microscope to generate large amounts of vacancies in highly concentrated nitrogen-doped CVD diamond ([N] = 8 × 1020 cm-3). This result reduces the difficulty of producing high-concentration NV ensembles and is expected to promote the development of many-body quantum physics.
NV- center has been paid attention as a quantum sensor for highly sensitive detection of magnetic field, electric field, temperature and strain, etc.. Electron beam irradiation followed by subsequent thermal annealing is known as the effective procedures to create NV- center in diamond. The electron irradiation generates vacancies in diamond and the annealing enables vacancies to diffuse in the lattice. Then diffused vacancies are captured by nitrogen atoms, and as a result, NV centers are created. In addition, substitutional nitrogen atom at a lattice site (P1 center) also acts as a donor for NV center, the charge state of NV centers changes from neutral (NV0) to NV-. Creation high concentration of ensemble NV- centers is needed to achieve high sensitively sensing. The magnetic sensitivity is proportional to the reciprocal of the number of NV centers and T2 (spin coherence time), i.e., high concentration NV- centers with long T2 increase the sensitivity. P1 center has an important role for being a component of NV- centers and acting as donor to the NV center. But it also plays a role as decoherence source (decrease in magnetic field sensitivity). Therefore, it is important to create high concentration of NV- centers considering the amount of P1 centers. In current study, we investigate irradiation fluence dependence of the creation behavior of NV centers in type-Ib diamonds by using electron spin resonance (ESR) and photo-luminescence (PL) to understand the creation mechanism of NV- center. The values of T2 are also evaluated by Hahn-echo measurement, since it is one of the key parameters for highly sensitive magnetometry. Then, we discuss the creation mechanism of NV centers based on concentrations of defects.