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arXiv:2306.02966 · Nano Letters

Multicone Diamond Waveguides for Nanoscale Quantum Sensing

Tianqi Zhu, J. Rhensius, Konstantin Herb, Viraj G. Damle, Gabriel Puebla‐Hellmann, Christian L. Degen, Erika Janitz

Published Nov 7, 2023• 19 citations
arXivHTMLPDF

Abstract

The long-lived electronic spin of the nitrogen-vacancy (NV) center in diamonds is a promising quantum sensor for detecting nanoscopic magnetic and electric fields in various environments. However, the poor signal-to-noise ratio (SNR) of prevalent optical spin-readout techniques presents a critical challenge in improving measurement sensitivity. Here, we address this limitation by coupling individual NVs to optimized diamond nanopillars, thereby enhancing the collection efficiency of fluorescence. Guided by near-field optical simulations, we predict improved performance for tall (≥5 μm) pillars with tapered sidewalls. This is subsequently verified by fabricating and characterizing a representative set of structures using a newly developed nanofabrication process. We observe increased SNR for optimized devices, owing to improved emission collimation and directionality. Promisingly, these devices are compatible with low-numerical-aperture collection optics and a reduced tip radius, reducing experimental overhead and facilitating improved spatial resolution for scanning applications.

DOI
10.1021/acs.nanolett.3c02120

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The long-lived electronic spin of the nitrogen-vacancy (NV) center in diamonds is a promising quantum sensor for detecting nanoscopic magnetic and electric fields in various environments. However, the poor signal-to-noise ratio (SNR) of prevalent optical spin-readout techniques presents a critical challenge in improving measurement sensitivity. Here, we address this limitation by coupling individual NVs to optimized diamond nanopillars, thereby enhancing the collection efficiency of fluorescence. Guided by near-field optical simulations, we predict improved performance for tall (≥5 μm) pillars with tapered sidewalls. This is subsequently verified by fabricating and characterizing a representative set of structures using a newly developed nanofabrication process. We observe increased SNR for optimized devices, owing to improved emission collimation and directionality. Promisingly, these devices are compatible with low-numerical-aperture collection optics and a reduced tip radius, reducing experimental overhead and facilitating improved spatial resolution for scanning applications.
The nitrogen-vacancy (NV) center in diamond has been developed as a promising platform for quantum sensing, especially for magnetic field measurements in the nano-tesla range with a nano-meter resolution. Optical spin readout performance has a direct effect on the signal-to-noise ratio (SNR) of experiments. In this work, we introduce an online optimization method to customize the laser waveform for readout. Both simulations and experiments reveal that our new scheme optimizes the optically detected magnetic resonance in NV center. The SNR of optical spin readout has been witnessed a 44.1% increase in experiments. In addition, we applied the scheme to the Rabi oscillation experiment, which shows an improvement of 46.0% in contrast and a reduction of 12.1% in mean deviation compared to traditional constant laser power SNR optimization. This scheme is promising to improve sensitivities for a wide range of NV-based applications in the future.
Nitrogen-vacancy (NV) centers in diamond are versatile room-temperature quantum sensors whose sensitivity is often limited by photon collection. Shaping the diamond into nanopillar antennas increases photon collection, and packing these pillars into a dense array promises to combine this collection gain with the parallel throughput of the widefield quantum diamond microscope. However, optical interactions among the pillars in the array can limit its performance. The study combines finite-difference time-domain (FDTD) simulation with two experimental modalities, a home-built confocal microscope and a widefield microscope, on a (111) diamond parabolic nanopillar array of four geometries spanning two tip diameters (0.4 and 0.8 \textmu m) and edge-to-edge gaps of 0.5-1.6 \textmu m. The pillars enhance NV collection broadband, with band-integrated enhancements of 10.4×10.4\times10.4× and 6.0×6.0\times6.0× for the two tips, consistent with simulation. The geometry-mediated transport is quantified through the photons transported from the pillars to the gap and to neighboring pillars by the gap-to-pillar ratio (G/PG/PG/P) and the neighbor fraction (χ\chiχ): G/PG/PG/P falls with increasing gap across all three methods (widefield 50.4%→31.4%50.4\%\rightarrow31.4\%50.4%→31.4%, confocal 26.2%→12.1%26.2\%\rightarrow12.1\%26.2%→12.1%, simulated χ\chiχ 7.7%→2.6%7.7\%\rightarrow2.6\%7.7%→2.6%), establishing the coupling as a robust physical feature governed by the base-to-base gap rather than the pitch. These optical interactions can influence the performance of the sensor where χ\chiχ biases the accuracy while G/PG/PG/P blurs the spatial resolution, and both grow as the pitch shrinks, capping the density-for-sensitivity gain and identifying the base-to-base gap and the pillar taper as the geometric parameters a purpose-designed sensing array must control. Whether the transported light is spin-active NV−^-− emission, and therefore biases ODMR readout rather than merely adding background, remains to be confirmed, and is identified as the central next step toward array-based widefield sensing.
Nitrogen-vacancy (NV) color centers in diamond are excellent quantum sensors possessing high sensitivity and nano-scale spatial resolution. Their integration in photonic structures is often desired, since it leads to an increased photon emission and also allows the realization of solid-state quantum technology architectures. Here, we report the fabrication of diamond nano-pillars with diameters up to 1000 nm by electron beam lithography and inductively coupled plasma reactive ion etching in nitrogen-rich diamonds (type Ib) with [100] and [111] crystal orientations. The NV centers were created by keV-He ion bombardment and subsequent annealing, and we estimate an average number of NVs per pillar to be 4300 ± 300 and 520 ± 120 for the [100] and [111] samples, respectively. Lifetime measurements of the NVs’ excited state showed two time constants with average values of τ1 ≈ 2 ns and τ2 ≈ 8 ns, which are shorter as compared to a single color center in a bulk crystal (τ ≈ 10 ns). This is probably due to a coupling between the NVs as well as due to interaction with bombardment-induced defects and substitutional nitrogen (P1 centers). Optically detected magnetic resonance measurements revealed a contrast of about 5% and average coherence and relaxation times of T2 [100] = 420 ± 40 ns, T2 [111] = 560 ± 50 ns, and T1 [100] = 162 ± 11 μs, T1 [111] = 174 ± 24 μs. These pillars could find an application for scanning probe magnetic field imaging.
Nitrogen vacancy centers in diamond are among the leading solid state quantum platforms, offering exceptional spatial resolution and sensitivity for applications such as magnetic field sensing, thermometry, and bioimaging. However, in high background environments,such as those encountered in in vitro diagnostics, the performance of NV based sensors can be compromised by strong background fluorescence, particularly from substrates such as nitrocellulose. In this work, we analytically and experimentally investigate the use of pulsed laser excitation combined with time gating techniques to suppress background fluorescence and enhance the signal to noise ratio in NV based quantum sensing, with an emphasis on spin enhanced biosensing. Through experimental studies using mixed ensembles of silicon vacancy and NV centers in bulk diamond, as well as fluorescent nanodiamonds on NC substrates, we demonstrate significant improvements in NV spin resonance visibility, demonstrated by an increase of the SNR by up to 4x, and a resulting measurement time reduction by 16x. The presented technique and results here can help significantly increase the readout efficiency and speed in future applications of NV centers in high background environments, such as in IVD, where the NV centers are used as a fluorescent label for biomolecules.
Diamond NV centers have transformed quantum sensing by enabling precise measurement of magnetic and electric fields, temperature, pressure, and strain, all within a reliable solid-state platform, at room temperature, down to the nanoscale. These capabilities position NV-based sensors as alternatives to cryogenic SQUIDs or atomic gas systems, with transformative potential across biomedical imaging, autonomous navigation, and industrial non-destructive testing (NDT). Despite promising prototypes—such as fiber-integrated endoscopes, CMOS-compatible sensors, and microfluidic chips—the development of widescale applications is hampered due to challenges in diamond micro/nanofabrication and photonic integration. Our group addresses these limitations through diamond processing techniques and hybrid material platforms. We develop methods for fabricating quantum-grade diamond nanostructures, including nanopillars optimized for neuronal electric field sensing and other photonic cavity applications. Additionally, we explore the integration of NV-rich diamond membranes within photonic systems to improve the spin photon interaction and efficient conversion of the pump beam. Collaborating with industry partner Kwantek, we also work on a compact fiber-endoscope prototype enabling NDT in constrained environments. These innovations will improve the state-of-the-art NV magnetometry to reduce system footprint and cost, critical for future industrialisation.
Photonic structures in diamond are key to most of its application in quantum technology. Here, we demonstrate tapered nanowaveguides structured directly onto the diamond substrate hosting shallow-implanted nitrogen vacancy (NV) centers. By optimization based on simulations and precise experimental control of the geometry of these pillar-shaped nanowaveguides, we achieve a net photon flux up to ∼ 1.7 × 10(6) s(-1). This presents the brightest monolithic bulk diamond structure based on single NV centers so far. We observe no impact on excited state lifetime and electronic spin dephasing time (T2) due to the nanofabrication process. Possessing such high brightness with low background in addition to preserved spin quality, this geometry can improve the current nanomagnetometry sensitivity ∼ 5 times. In addition, it facilitates a wide range of diamond defects-based magnetometry applications. As a demonstration, we measure the temperature dependency of T1 relaxation time of a single shallow NV center electronic spin. We observe the two-phonon Raman process to be negligible in comparison to the dominant two-phonon Orbach process.