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1.
Open Res Eur ; 4: 44, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-39148583

RESUMEN

Nitrogen-vacancy (NV) centers in diamond have emerged as promising quantum sensors due to their highly coherent and optically addressable spin states with potential applications in high-sensitivity magnetometry. Homogeneously addressing large ensembles of NV centers offers clear benefit in terms of sensing precision as well as in fundamental studies of collective effects. Such experiments require a spatially uniform, intense, and broadband microwave field that can be difficult to generate. Previous approaches, such as copper wires, loop coils, and planar structures, have shown limitations in field homogeneity, bandwidth, and integration in compact devices. In this paper, we present a coplanar waveguide (CPW) gold coil patterned on a 3 × 3 mm 2 diamond substrate, offering full integration, enhanced stability, and broad bandwidth suitable for various NV sensing applications. Coil fabricated on diamond offers several advantages for magnetometry with NV centers ensemble, including enhanced heat dissipation, seamless integration, scalability, and miniaturization potential. We optimize critical geometrical parameters to achieve a homogeneous magnetic field with a coefficient of variation of less than 6% over an area of 0.5 mm 2 and present experimental results confirming the performance of the proposed CPW coil.


In recent years, there has been significant interest in using nitrogen-vacancy (NV) centers in diamond as quantum sensors for high-sensitivity magnetometry. These NV centers, particularly the negatively charged ones, offer promising applications due to their coherent spin states that can be manipulated using microwave fields and optically detected magnetic resonance techniques. However, to improve measurement precision and signal-to-noise ratio, it's advantageous to address large ensembles of NV centers, which requires a spatially uniform, intense, and broadband microwave field. Various methods, such as copper wires, loop coils, and planar structures, have been explored to achieve this, but with limited capability. To address their limitations, a coplanar waveguide (CPW) gold coil patterned on a CVD diamond substrate is proposed. This design offers a highly homogeneous magnetic field, full integration with the diamond substrate, scalability, miniaturization, and efficient heat dissipation, making it a promising solution for NV magnetometry applications. Experimental results confirm its performance, making it a remarkable advancement in this area.

2.
Nano Lett ; 24(22): 6474-6479, 2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38767585

RESUMEN

Experimental noise often contains information about the interactions of a system with its environment, but establishing a relation between the measured time fluctuations and the underlying physical observables is rarely apparent. Here, we leverage a multidimensional and multisensor analysis of spectral diffusion to investigate the dynamics of trapped carriers near subdiffraction clusters of nitrogen-vacancy (NV) centers in diamond. We establish statistical correlations in the spectral fluctuations we measure as we recursively probe the cluster optical resonances, which we then exploit to reveal proximal traps. Further, we deterministically induce Stark shifts in the cluster spectrum, ultimately allowing us to pinpoint the relative three-dimensional positions of interacting NVs as well as the location and charge sign of surrounding traps. Our results can be generalized to other color centers and provide opportunities for the characterization of photocarrier dynamics in semiconductors and the manipulation of nanoscale spin-qubit clusters connected via electric fields.

3.
ACS Nano ; 18(8): 6523-6532, 2024 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-38369724

RESUMEN

Scanning-probe and wide-field magnetic microscopes based on nitrogen-vacancy (NV) centers in diamond have enabled advances in the study of biology and materials, but each method has drawbacks. Here, we implement an alternative method for nanoscale magnetic microscopy based on optical control of the charge state of NV centers in a dense layer near the diamond surface. By combining a donut-beam super-resolution technique with optically detected magnetic resonance spectroscopy, we imaged the magnetic fields produced by single 30 nm iron-oxide nanoparticles. The magnetic microscope has a lateral spatial resolution of ∼100 nm, and it resolves the individual magnetic dipole features from clusters of nanoparticles with interparticle spacings down to ∼190 nm. The magnetic feature amplitudes are more than an order of magnitude larger than those obtained by confocal magnetic microscopy due to the narrower optical point-spread function and the shallow depth of NV centers. We analyze the magnetic nanoparticle images and sensitivity as a function of the microscope's spatial resolution and show that the signal-to-noise ratio for nanoparticle detection does not degrade as the spatial resolution improves. We identify sources of background fluorescence that limit the present performance, including diamond second-order Raman emission and imperfect NV charge state control. Our method, which uses <10 mW laser power and can be parallelized by patterned illumination, introduces a promising format for nanoscale magnetic imaging.

4.
Nano Lett ; 24(5): 1660-1666, 2024 Feb 07.
Artículo en Inglés | MEDLINE | ID: mdl-38266180

RESUMEN

Scalable and addressable integrated manipulation of qubits is crucial for practical quantum information applications. Different waveguides have been used to transport the optical and electrical driving pulses, which are usually required for qubit manipulation. However, the separated multifields may limit the compactness and efficiency of manipulation and introduce unwanted perturbation. Here, we develop a tapered fiber-nanowire-electrode hybrid structure to realize integrated optical and microwave manipulation of solid-state spins at nanoscale. Visible light and microwave driving pulses are simultaneously transported and concentrated along an Ag nanowire. Studied with spin defects in diamond, the results show that the different driving fields are aligned with high accuracy. The spatially selective spin manipulation is realized. And the frequency-scanning optically detected magnetic resonance (ODMR) of spin qubits is measured, illustrating the potential for portable quantum sensing. Our work provides a new scheme for developing compact, miniaturized quantum sensors and quantum information processing devices.

5.
Adv Opt Mater ; 11(6)2023 Mar 17.
Artículo en Inglés | MEDLINE | ID: mdl-37920689

RESUMEN

Nitrogen-vacancy (NV) centers in nanodiamond hold great promise for creating superior biological labels and quantum sensing methods. Yet, inefficient photon generation and extraction from excited NV centers restricts the achievable sensitivity and temporal resolution. Herein, we report an entirely complementary route featuring pyramidal hyperbolic metasurface to modify the spontaneous emission of NV centers. Fabricated using nanosphere lithography, the metasurface consists of alternatively stacked silica-silver thin films configured in a pyramidal fashion, and supports both spectrally broadband Purcell enhancement and spatially extended intense local fields owing to the hyperbolic dispersion and plasmonic coupling. The enhanced photophysical properties are manifested as a simultaneous amplification to the spontaneous decay rate and emission intensity of NV centers. We envision the reported pyramidal metasurface could serve as a versatile platform for creating chip-based ultrafast single-photon sources and spin-enhanced quantum biosensing strategies, as well as aiding in further fundamental understanding of photoexcited species in condensed phases.

6.
ACS Nano ; 17(17): 16491-16500, 2023 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-37594320

RESUMEN

Nitrogen vacancy (NV) centers in fluorescent nanodiamonds (FNDs) draw widespread attention as quantum sensors due to their room-temperature luminescence, exceptional photo- and chemical stability, and biocompatibility. For bioscience applications, NV centers in FNDs offer high-spatial-resolution capabilities that are unparalleled by other solid-state nanoparticle emitters. On the other hand, pursuits to further improve the optical properties of FNDs have reached a bottleneck, with intense debate in the literature over which of the many factors are most pertinent. Here, we describe how substantial progress can be achieved using a correlative transmission electron microscopy and photoluminescence (TEMPL) method that we have developed. TEMPL enables a precise correlative analysis of the fluorescence brightness, size, and shape of individual FND particles. Augmented with machine learning, TEMPL can be used to analyze a large, statistically meaningful number of particles. Our results reveal that FND fluorescence is strongly dependent on particle shape, specifically, that thin, flake-shaped particles are up to several times brighter and that fluorescence increases with decreasing particle sphericity. Our theoretical analysis shows that these observations are attributable to the constructive interference of light waves within the FNDs. Our findings have significant implications for state-of-the-art sensing applications, and they offer potential avenues for improving the sensitivity and resolution of quantum sensing devices.

7.
Prog Nucl Magn Reson Spectrosc ; 134-135: 20-38, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37321756

RESUMEN

Nanodiamonds containing fluorescent Nitrogen-Vacancy (NV) centers are the smallest single particles, of which a magnetic resonance spectrum can be recorded at room temperature using optically-detected magnetic resonance (ODMR). By recording spectral shift or changes in relaxation rates, various physical and chemical quantities can be measured such as the magnetic field, orientation, temperature, radical concentration, pH or even NMR. This turns NV-nanodiamonds into nanoscale quantum sensors, which can be read out by a sensitive fluorescence microscope equipped with an additional magnetic resonance upgrade. In this review, we introduce the field of ODMR spectroscopy of NV-nanodiamonds and how it can be used to sense different quantities. Thereby we highlight both, the pioneering contributions and the latest results (covered until 2021) with a focus on biological applications.


Asunto(s)
Nanodiamantes , Nanodiamantes/química , Nitrógeno/química , Espectroscopía de Resonancia Magnética/métodos , Microscopía Fluorescente , Imagen por Resonancia Magnética
8.
ACS Nano ; 17(11): 10474-10485, 2023 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-37212793

RESUMEN

Quantum sensing with spin defects in diamond, such as the nitrogen vacancy (NV) center, enables the detection of various chemical species on the nanoscale. Molecules or ions with unpaired electronic spins are typically probed by their influence on the NV center's spin relaxation. Whereas it is well-known that paramagnetic ions reduce the NV center's relaxation time (T1), here we report on the opposite effect for diamagnetic ions. We demonstrate that millimolar concentrations of aqueous diamagnetic electrolyte solutions increase the T1 time of near-surface NV center ensembles compared to pure water. To elucidate the underlying mechanism of this surprising effect, single and double quantum NV experiments are performed, which indicate a reduction of magnetic and electric noise in the presence of diamagnetic electrolytes. In combination with ab initio simulations, we propose that a change in the interfacial band bending due to the formation of an electric double layer leads to a stabilization of fluctuating charges at the interface of an oxidized diamond. This work not only helps to understand noise sources in quantum systems but could also broaden the application space of quantum sensors toward electrolyte sensing in cell biology, neuroscience, and electrochemistry.

9.
Materials (Basel) ; 16(8)2023 Apr 21.
Artículo en Inglés | MEDLINE | ID: mdl-37110108

RESUMEN

We propose a scheme for detecting single microwave photons using dipole-induced transparency (DIT) in an optical cavity resonantly coupled to a spin-selective transition of a negatively charged nitrogen-vacancy (NV-) defect in diamond crystal lattices. In this scheme, the microwave photons control the interaction of the optical cavity with the NV- center by addressing the spin state of the defect. The spin, in turn, is measured with high fidelity by counting the number of reflected photons when the cavity is probed by resonant laser light. To evaluate the performance of the proposed scheme, we derive the governing master equation and solve it through both direct integration and the Monte Carlo approach. Using these numerical simulations, we then investigate the effects of different parameters on the detection performance and find their corresponding optimized values. Our results indicate that detection efficiencies approaching 90% and fidelities exceeding 90% could be achieved when using realistic optical and microwave cavity parameters.

10.
ACS Sens ; 8(4): 1667-1675, 2023 04 28.
Artículo en Inglés | MEDLINE | ID: mdl-37043367

RESUMEN

We present an alternative to conventional Electron Paramagnetic Resonance (EPR) spectroscopy equipment. Avoiding the use of bulky magnets and magnetron equipment, we use the photoluminescence of an ensemble of Nitrogen-Vacancy centers at the surface of a diamond. Monitoring their relaxation time (or T1), we detected their cross-relaxation with a compound of interest. In addition, the EPR spectra are encoded through a localized magnetic field gradient. While recording previous data took 12 min per data point with individual NV centers, we were able to reconstruct a full spectrum at once in 3 s, over a range from 3 to 11 G. In terms of sensitivity, only 0.5 µL of a 1 µM hexaaquacopper(II) ion solution was necessary.


Asunto(s)
Diamante , Imanes , Diamante/química , Espectroscopía de Resonancia Magnética/métodos , Espectroscopía de Resonancia por Spin del Electrón/métodos , Campos Magnéticos
11.
Nanomaterials (Basel) ; 13(5)2023 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-36903827

RESUMEN

Magnetometers based on nitrogen-vacancy (NV) centers in diamonds have promising applications in fields of living systems biology, condensed matter physics, and industry. This paper proposes a portable and flexible all-fiber NV center vector magnetometer by using fibers to substitute all conventional spatial optical elements, realizing laser excitation and fluorescence collection of micro-diamond with multi-mode fibers simultaneously and efficiently. An optical model is established to investigate multi-mode fiber interrogation of micro-diamond to estimate the optical performance of NV center system. A new analysis method is proposed to extract the magnitude and direction of the magnetic field, combining the morphology of the micro-diamond, thus realizing µm-scale vector magnetic field detection at the tip of the fiber probe. Experimental testing shows our fabricated magnetometer has a sensitivity of 0.73 nT/Hz1/2, demonstrating its feasibility and performance in comparison with conventional confocal NV center magnetometers. This research presents a robust and compact magnetic endoscopy and remote-magnetic measurement approach, which will substantially promote the practical application of magnetometers based on NV centers.

12.
Nano Lett ; 23(2): 422-428, 2023 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-36602464

RESUMEN

A broad effort is underway to understand and harness the interaction between superconductors and spin-active color centers with an eye on hybrid quantum devices and novel imaging modalities of superconducting materials. Most work, however, overlooks the interplay between either system and the environment created by the color center host. Here we use a diamond scanning probe to investigate the spin dynamics of a single nitrogen-vacancy (NV) center proximal to a superconducting film. We find that the presence of the superconductor increases the NV spin coherence lifetime, a phenomenon we tentatively rationalize as a change in the electric noise due to a superconductor-induced redistribution of charge carriers near induced redistribution of charge carriers near the NV. We then build on these findings to demonstrate transverse-relaxation-time-weighted imaging of the superconductor film. These results shed light on the dynamics governing the spin coherence of shallow NVs, and promise opportunities for new forms of noise spectroscopy and imaging of superconductors.

13.
ACS Appl Mater Interfaces ; 15(2): 3287-3296, 2023 Jan 18.
Artículo en Inglés | MEDLINE | ID: mdl-36602594

RESUMEN

Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying the fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling thin and highly tunable spintronic devices. To realize high-quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here, the study of exfoliated flakes of cobalt-substituted Fe5GeTe2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic imaging with nitrogen-vacancy centers in diamond, ferromagnetism at room temperature was observed in CFGT flakes as thin as 16 nm corresponding to 16 layers. This result expands the portfolio of thin room-temperature 2D magnet flakes exfoliated from robust single crystals that reach a thickness regime relevant to practical spintronic applications. The Curie temperature Tc of CFGT ranges from 310 K in the thinnest flake studied to 328 K in the bulk. To investigate the prospect of high-temperature monolayer ferromagnetism, Monte Carlo calculations were performed, which predicted a high value of Tc of ∼270 K in CFGT monolayers. Pathways toward further enhancing monolayer Tc are discussed. These results support CFGT as a promising platform for realizing high-quality room-temperature 2D magnet devices.

14.
Nano Lett ; 22(24): 9876-9882, 2022 12 28.
Artículo en Inglés | MEDLINE | ID: mdl-36480706

RESUMEN

Atomic-scale magnetic field sensors based on nitrogen vacancy (NV) defects in diamonds are an exciting platform for nanoscale nuclear magnetic resonance (NMR) spectroscopy. The detection of NMR signals from a few zeptoliters to single molecules or even single nuclear spins has been demonstrated using NV centers close to the diamond surface. However, fast molecular diffusion of sample molecules in and out of the nanoscale detection volumes impedes their detection and limits current experiments to solid-state or highly viscous samples. Here, we show that restricting diffusion by confinement enables nanoscale NMR spectroscopy of liquid samples. Our approach uses metal-organic frameworks (MOF) with angstrom-sized pores on a diamond chip to trap sample molecules near the NV centers. This enables the detection of NMR signals from a liquid sample, which would not be detectable without confinement. These results set the route for nanoscale liquid-phase NMR with high spectral resolution.


Asunto(s)
Estructuras Metalorgánicas , Nitrógeno/química , Espectroscopía de Resonancia Magnética/métodos , Imagen por Resonancia Magnética , Diamante/química
15.
Ultramicroscopy ; 242: 113624, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36215942

RESUMEN

In this work, we present a novel, compact, power efficient and variable magnetic field source design for magnetic field imaging microscopy. The device is based on a pair of diametrically magnetized permanent magnet cylinders with electro-mechanical rotation control and ferrite flux homogenizers. A Hall probe and NV centers in diamond are used to demonstrate a proof of concept of a proposed magnetic field setup and to characterize the homogeneity of the produced magnetic field on a micrometer scale. Numerical simulation results are compared with experimental results showing good agreement of the distribution of the magnetic field in the setup. As a result, a magnetic field source with a tunable field amplitude in the range from 1 mT to 222 mT is demonstrated, achieving a magnetic field homogeneity of 2 ppm/µm or 0.5 µT/µm at 222 mT in a 25 × 25 µm field of view.

16.
Nanoscale Res Lett ; 17(1): 95, 2022 Sep 26.
Artículo en Inglés | MEDLINE | ID: mdl-36161373

RESUMEN

Ensembles of negatively charged nitrogen-vacancy centers (NV-) in diamond have been proposed for sensing of magnetic fields and paramagnetic agents, and as a source of spin-order for the hyperpolarization of nuclei in magnetic resonance applications. To this end, strongly fluorescent nanodiamonds (NDs) represent promising materials, with large surface areas and dense ensembles of NV-. However, surface effects tend to favor the less useful neutral form, the NV0 centers, and strategies to increase the density of shallow NV- centers have been proposed, including irradiation with strong laser power (Gorrini in ACS Appl Mater Interfaces. 13:43221-43232, 2021). Here, we study the fluorescence properties and optically detected magnetic resonance (ODMR) of NV- centers as a function of laser power in strongly fluorescent bulk diamond and in nanodiamonds obtained by nanomilling of the native material. In bulk diamond, we find that increasing laser power increases ODMR contrast, consistent with a power-dependent increase in spin-polarization. Conversely, in nanodiamonds we observe a non-monotonic behavior, with a decrease in ODMR contrast at higher laser power. We hypothesize that this phenomenon may be ascribed to more efficient NV-→NV0 photoconversion in nanodiamonds compared to bulk diamond, resulting in depletion of the NV- pool. A similar behavior is shown for NDs internalized in macrophage cells under the typical experimental conditions of imaging bioassays. Our results suggest strong laser irradiation is not an effective strategy in NDs, where the interplay between surface effects and local microenvironment determine the optimal experimental conditions.

17.
Nanotechnology ; 34(1)2022 Oct 20.
Artículo en Inglés | MEDLINE | ID: mdl-36170794

RESUMEN

The recently-developed ability to control phosphorous-doping of silicon at an atomic level using scanning tunneling microscopy, a technique known as atomic precision advanced manufacturing (APAM), has allowed us to tailor electronic devices with atomic precision, and thus has emerged as a way to explore new possibilities in Si electronics. In these applications, critical questions include where current flow is actually occurring in or near APAM structures as well as whether leakage currents are present. In general, detection and mapping of current flow in APAM structures are valuable diagnostic tools to obtain reliable devices in digital-enhanced applications. In this paper, we used nitrogen-vacancy (NV) centers in diamond for wide-field magnetic imaging (with a few-mm field of view and micron-scale resolution) of magnetic fields from surface currents flowing in an APAM test device made of a P delta-doped layer on a Si substrate, a standard APAM witness material. We integrated a diamond having a surface NV ensemble with the device (patterned in two parallel mm-sized ribbons), then mapped the magnetic field from the DC current injected in the APAM device in a home-built NV wide-field microscope. The 2D magnetic field maps were used to reconstruct the surface current densities, allowing us to obtain information on current paths, device failures such as choke points where current flow is impeded, and current leakages outside the APAM-defined P-doped regions. Analysis on the current density reconstructed map showed a projected sensitivity of ∼0.03 A m-1, corresponding to a smallest-detectable current in the 200µm wide APAM ribbon of ∼6µA. These results demonstrate the failure analysis capability of NV wide-field magnetometry for APAM materials, opening the possibility to investigate other cutting-edge microelectronic devices.

18.
Nano Lett ; 22(18): 7714-7723, 2022 09 28.
Artículo en Inglés | MEDLINE | ID: mdl-35946594

RESUMEN

Measuring the mechanical interplay between cells and their surrounding microenvironment is vital in cell biology and disease diagnosis. Most current methods can only capture the translational motion of fiduciary markers in the deformed matrix, but their rotational motions are normally ignored. Here, by utilizing single nitrogen-vacancy (NV) centers in nanodiamonds (NDs) as fluorescent markers, we propose a linear polarization modulation (LPM) method to monitor in-plane rotational and translational motions of the substrate caused by cell traction forces. Specifically, precise orientation measurement and localization with background suppression were achieved via optical polarization selective excitation of single NV centers with precisions of ∼0.5°/7.5 s and 2 nm/min, respectively. Additionally, we successfully applied this method to monitor the multidimensional movements of NDs attached to the vicinity of cell focal adhesions. The experimental results agreed well with our theoretical calculations, demonstrating the practicability of the NV-based LPM method in studying mechanobiology and cell-material interactions.


Asunto(s)
Nanodiamantes , Movimiento (Física) , Nitrógeno , Tracción
19.
Nanomaterials (Basel) ; 12(13)2022 Jun 29.
Artículo en Inglés | MEDLINE | ID: mdl-35808069

RESUMEN

The implantation of diamonds with helium ions has become a common method to create hundreds-nanometers-thick near-surface layers of NV centers for high-sensitivity sensing and imaging applications; however, optimal implantation dose and annealing temperature are still a matter of discussion. In this study, we irradiated HPHT diamonds with an initial nitrogen concentration of 100 ppm using different implantation doses of helium ions to create 200-nm thick NV layers. We compare a previously considered optimal implantation dose of ∼1012 He+/cm2 to double and triple doses by measuring fluorescence intensity, contrast, and linewidth of magnetic resonances, as well as longitudinal and transversal relaxation times T1 and T2. From these direct measurements, we also estimate concentrations of P1 and NV centers. In addition, we compare the three diamond samples that underwent three consequent annealing steps to quantify the impact of processing at 1100 °C, which follows initial annealing at 800 °C. By tripling the implantation dose, we have increased the magnetic sensitivity of our sensors by 28±5%. By projecting our results to higher implantation doses, we demonstrate that it is possible to achieve a further improvement of up to 70%. At the same time, additional annealing steps at 1100 °C improve the sensitivity only by 6.6 ± 2.7%.

20.
Nano Lett ; 22(10): 3889-3896, 2022 05 25.
Artículo en Inglés | MEDLINE | ID: mdl-35507005

RESUMEN

Nanoindentation based on atomic force microscopy (AFM) can measure the elasticity of biomaterials and cells with high spatial resolution and sensitivity, but relating the data to quantitative mechanical properties depends on information on the local contact, which is unclear in most cases. Here, we demonstrate nonlocal deformation sensing on biorelevant soft matters upon AFM indentation by using nitrogen-vacancy centers in nanodiamonds, providing data for studying both the elasticity and capillarity without requiring detailed knowledge about the local contact. Using fixed HeLa cells for demonstration, we show that the apparent elastic moduli of the cells would have been overestimated if the capillarity was not considered. In addition, we observe that both the elastic moduli and the surface tensions are reduced after depolymerization of the actin cytoskeleton in cells. This work demonstrates that the nanodiamond sensing of nonlocal deformation with nanometer precision is particularly suitable for studying mechanics of soft biorelevant materials.


Asunto(s)
Nanodiamantes , Acción Capilar , Elasticidad , Células HeLa , Humanos , Microscopía de Fuerza Atómica
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