Ensemble Of Nitrogen-vacancy Centers Research Articles

Deep polarization of the ensemble nitrogen-vacancy centers in the diamond induced by an Airy beam with a long focal depth

Deep polarization of the ensemble nitrogen-vacancy centers in the diamond induced by an Airy beam with a long focal depth

Investigation of zero-phonon line characteristics in ensemble nitrogen-vacancy centers at 1.6 K–300 K

The ensemble of nitrogen-vacancy (NV) centers is widely used in quantum information transmission, high-precision magnetic field, and temperature sensing due to their advantages of long-lived state and the ability to be pumped by optical cycling. In this study, we investigate the zero-phonon line behavior of the two charge states of NV centers by measuring the photoluminescence of the NV center at 1.6 K-300 K. The results demonstrate a positional redshift, an increase in line width, and a decrease in fluorescence intensity for the ZPL of NV0 and NV- as the temperature increased. In the range of 10 K to 140 K, the peak shift with high concentrations of NV- revealed an anomaly of bandgap reforming. The peak position undergoes a blueshift and then a redshift as temperature increases. Furthermore, the transformation between NV0 and NV- with temperature changes has been obtained in diamonds with different nitrogen concentrations. This study explored the ZPL characteristics of NV centers in various temperatures, and the findings are significant for the development of high-resolution temperature sensing and high-precision magnetic field sensing in ensemble NV centers.

Diamond surface functionalization via visible light–driven C–H activation for nanoscale quantum sensing

Nitrogen-vacancy (NV) centers in diamond are a promising platform for nanoscale NMR sensing. Despite significant progress toward using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. Such sensing requires that target molecules are immobilized within nanometers of NV centers with long spin coherence. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C-H bonds on single-crystal diamond surfaces under ambient conditions using visible light, forming C-F, C-Cl, C-S, and C-N bonds at the surface. This method is compatible with NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof-of-principle demonstration, we use shallow ensembles of NV centers to detect nuclear spins from surface-bound functional groups. Our approach to surface functionalization opens the door to deploying NV centers as a tool for chemical sensing and single-molecule spectroscopy.

Integrated coplanar waveguide coil on diamond for enhanced homogeneous broadband NV magnetometry

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 mm2 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 mm2 and present experimental results confirming the performance of the proposed CPW coil.

Infrared vertical external cavity surface emitting laser threshold magnetometer

Nitrogen-vacancy (NV) centers have considerable promise as high sensitivity magnetometers; however, they are commonly limited by inefficient collection and low contrasts. Laser threshold magnetometry (LTM) enables efficient collection and high contrasts, providing a path toward higher sensitivity magnetometry. We demonstrate an infrared LTM using an ensemble of NV centers in a single-crystal diamond plate integrated into a vertical external cavity surface emitting laser. The laser was tuned to the spin-dependent absorption line of the NV centers, allowing for optical readout by monitoring the laser output power. We demonstrate a magnetic sensitivity of 7.5 nT/Hz in the frequency range between 10 and 50 Hz. Furthermore, the contrast and the projected photon shot noise limited (PSNL) sensitivity are shown to improve significantly by operating close to the lasing threshold, achieving 18.4% and 26.6 pT/Hz near the threshold. In addition, an unexpected saturable absorption phenomenon was observed near the threshold, which enhanced the contrast and projected PSNL sensitivity.

Fiber-taper collected emission from NV centers in high-Q/V diamond microdisks.

Fiber-coupled microdisks are a promising platform for enhancing the spontaneous emission from color centers in diamond. The measured cavity-enhanced emission from the microdisk is governed by the effective volume (V) of each cavity mode, the cavity quality factor (Q), and the coupling between the microdisk and the fiber. Here we observe room temperature photoluminescence from an ensemble of nitrogen-vacancy centers into high Q/V microdisk modes, which when combined with coherent spectroscopy of the microdisk modes, allows us to elucidate the relative contributions of these factors. The broad emission spectrum acts as an internal light source facilitating mode identification over several cavity free spectral ranges. Analysis of the fiber taper collected microdisk emission reveals spectral filtering both by the cavity and the fiber taper, the latter of which we find preferentially couples to higher-order microdisk modes. Coherent mode spectroscopy is used to measure Q ∼ 1 × 105 - the highest reported values for diamond microcavities operating at visible wavelengths. With realistic optimization of the microdisk dimensions, we predict that Purcell factors of ∼50 are within reach.

Fast coherent control of nitrogen-14 spins associated with nitrogen-vacancy centers in diamonds using dynamical decoupling

Abstract A nitrogen-vacancy (NV) center in a diamond enables the access to an electron spin, which is expected to present highly sensitive quantum sensors. Although exploiting a nitrogen nuclear spin improves the sensitivity, manipulating it using a resonant pulse requires a long gate time owing to its small gyromagnetic ratio. Another technique to control nuclear spins is a conditional rotation gate based on dynamical decoupling, which is faster but unavailable for nitrogen spins owing to the lack of transverse hyperfine coupling with the electron spin. In this study, we generated effective transverse coupling by applying a weak off-axis magnetic field. An effective coupling depends on the off-axis field; the conditional rotation gate on the nitrogen-14 spins of an NV center was demonstrated within 4.2 μs under an 1.8% off-axis field and a longitudinal field of approximately 280 mT. We estimated that a population transfer from the electron to nitrogen spins can be implemented with 8.7 μs. Our method is applicable to an ensemble of NV centers, in addition to a single NV center.

Modelling Rabi oscillations for widefield radiofrequency imaging in nitrogen-vacancy centers in diamond

In this paper we study the dynamics of an ensemble of nitrogen-vacancy centers in diamond when its photoluminescence is detected by means of a widefield imaging system. We develop a seven-level model and use it to simulate the widefield detection of nitrogen-vacancy centers Rabi oscillations. The simulation results are compared with experimental measurements showing a good agreement. In particular, we use the model to explain the asymmetric shape of the detected Rabi oscillations due to an incomplete repolarization of the nitrogen-vacancy center during the pulse sequence implemented for the detection of Rabi oscillations.

Robust diamond-embedded microwave antenna for optimizing quantum sensing using nitrogen-vacancy center ensembles

The nitrogen-vacancy (NV) color center in diamond has emerged as a promising candidate for quantum sensing. In this study, we propose a diamond-embedded metal antenna for magnetic detection utilizing NV center ensembles. Our approach involved employing nanofabrication and microwave plasma chemical vapor deposition techniques to fabricate the metal antenna and diamond epilayer. By directly embedding the antenna into the diamond, we effectively minimize external environmental interference, leading to improved device stability and reusability. Moreover, this integration enhances the device's compactness, making it highly suitable for on-chip quantum sensing applications. The innovative antenna design holds great potential for the development of future integrated quantum sensing devices based on NV centers in diamond.

Variance properties of the microwave absorption spectrum of an ensemble of nitrogen vacancy centers in diamond

This work presents an original method based on the variance properties of the microwave absorption spectrum of an ensemble of nitrogen vacancy centers in diamond. The spectrum is measured optically. A compact and simple device is designed to optimize the photon collection. We conduct a quantitative comparison of the ensemble's optical signal in both the visible and near infrared range. Using the enhanced signal-to-noise ratio achieved through the device geometry we perform real-time DC magnetometry at moderate light and microwave powers. Under these conditions, the amplitude of a DC magnetic field can be extracted from the variance of the microwave absorption spectrum in a fast and reproducible manner, without the burden of complex fitting techniques.

Laser writing of preferentially orientated nitrogen-vacancy centers in diamond

Nitrogen-vacancy centers in diamond have gained widespread attention as quantum systems that can be applied in quantum information devices. The excellent properties of quantum devices can be enhanced using preferentially oriented nitrogen-vacancy (NV) centers. However, thus far, orientation control has been achieved only via chemical vapor deposition. In this study, we demonstrate the creation of preferentially oriented NV centers via laser writing. The alignment ratio of ensemble NV centers is biased along the direction parallel to [111], depending on the femtosecond laser polarization, causing an increase of 55 % in contrast to the optically magnetic resonance signal at maximum compared with 25 % in random orientation. Based on time-dependent density-functional theory (TDDFT) simulations and experimental observations, such complex polarization dependence can be attributed to the anisotropy of electron excitation. This technique provides a new optical fabrication method for engineered materials and devices used in quantum technology.

Demonstration of highly sensitive wideband microwave sensing using ensemble nitrogen-vacancy centers

Microwave magnetometry is essential for the advancement of microwave technologies. We demonstrate a broadband microwave sensing protocol using the AC Zeeman effect with ensemble nitrogen-vacancy (NV) centers in diamond. A widefield microscope can visualize the frequency characteristics of the microwave resonator and the spatial distribution of off-resonant microwave amplitude. Furthermore, by combining this method with dynamical decoupling, we achieve the microwave amplitude sensitivity of 5.2 μT/Hz, which is 7.7 times better than 40.2 μT/Hz obtained using the protocol in previous research over a sensing volume of 2.77 μm×2.77 μm×30 nm. Our achievement is a concrete step in adapting ensemble NV centers for wideband and widefield microwave imaging.

Quantum diamond microscope for dynamic imaging of magnetic fields

Wide-field imaging of magnetic signals using ensembles of nitrogen-vacancy (NV) centers in diamond has garnered increasing interest due to its combination of micron-scale resolution, millimeter-scale field of view, and compatibility with diverse samples from across the physical and life sciences. Recently, wide-field NV magnetic imaging based on the Ramsey protocol has achieved uniform and enhanced sensitivity compared to conventional measurements. Here, we integrate the Ramsey-based protocol with spin-bath driving to extend the NV spin dephasing time and improve magnetic sensitivity. We also employ a high-speed camera to enable dynamic wide-field magnetic imaging. We benchmark the utility of this quantum diamond microscope (QDM) by imaging magnetic fields produced from a fabricated wire phantom. Over a 270 × 270 μm2 field of view, a median per-pixel magnetic sensitivity of 4.1(1) nT /Hz is realized with a spatial resolution ≲ 10 μm and sub-millisecond temporal resolution. Importantly, the spatial magnetic noise floor can be reduced to the picotesla scale by time-averaging and signal modulation, which enables imaging of a magnetic-field pattern with a peak-to-peak amplitude difference of about 300 pT. Finally, we discuss potential new applications of this dynamic QDM in studying biomineralization and electrically active cells.

Extending Spin Dephasing Time of Perfectly Aligned Nitrogen‐Vacancy Centers by Mitigating Stress Distribution on Highly Misoriented Chemical‐Vapor‐Deposition Diamond

AbstractExtending the spin‐dephasing time (T2*) of perfectly aligned nitrogen‐vacancy (NV) centers in large‐volume chemical vapor deposition (CVD) diamonds leads to enhanced DC magnetic sensitivity. However, T2* of the NV centers is significantly reduced by the stress distribution in the diamond film as its thickness increases. To overcome this issue, they developed a method to mitigate the stress distribution in the CVD diamond films, leading to a T2* extension of the ensemble NV centers. CVD diamond films of ≈60 µm thickness with perfectly aligned NV centers are formed on (111) diamond substrates with misorientation angles of 2.0°, 3.7°, 5.0°, and 10.0°. The study found that T2* of the ensemble of NV centers increased to approach its value limited only by the electron and nuclear spin bath with increasing the misorientation angle. Microscopic stress imaging revealed that the stress distribution is highly inhomogeneous along the depth direction in the CVD diamond film at low misorientation angles, whereas the inhomogeneity is largely suppressed on highly misoriented substrates. The reduced stress distribution possibly originates from the reduction of the dislocation density in the CVD diamond. This study provides an important method for synthesizing high‐quality diamond materials for use in highly sensitive quantum sensors.

Elimination of zero-field splitting frequency drift of nitrogen vacancy center ensembles in diamond induced by temperature noise

The electron spin state of the NV color center in the diamond is optically polarized and read out by laser. However, laser irradiation introduces additional temperature noise, and the zero-field splitting term in the Hamiltonian becomes unstable. The main objective of this study is to explain and eliminate the influence of temperature noise generated by laser power and to propose a laser pulse shaping for detection. Experimental results show that the additional −2.8 MHz frequency drift introduced by the high-power laser is suppressed, under the condition of achieving the same resonance peak contrast of the high-power laser.

Efficient scheme for implementing a hybrid Toffoli gate with two NV ensembles simultaneously controlling a single superconducting qubit

The Toffoli gate is a three-qubit controlled-controlled-NOT gate, which plays a central role in quantum information processing and quantum computing. Recently, hybrid systems and hybrid quantum gates have attracted much attention. We propose an efficient scheme to implement a hybrid Toffoli gate with two nitrogen-vacancy center ensembles (NV ensembles) as the control qubits and a single superconducting flux qubit as the target qubit. This hybrid Toffoli gate is realized by employing two NV ensembles coupled to a superconducting qutrit. The hybrid Toffoli gate is constructed by a controlled-controlled-phase (CCPHASE) gate sandwiched between two Hadamard gates applied on the target qubit. Since the CCPHASE gate is realized using only a single-step operation and no conventional gate decomposition protocol is applied, the Toffoli-gate implementation is greatly simplified. Because the higher energy level of the flux qutrit is not populated, the decoherence of this level is greatly suppressed. In addition, our hybrid Toffoli gate can be used to generate a hybrid Greenberger–Horne–Zeilinger entangled state of a flux qubit and two NV ensembles. Numerical simulations demonstrate that high-fidelity implementation of a hybrid Toffoli gate is feasible within current experimental technology. This proposal is universal and can be applied to accomplish the same task in a wide range of physical systems.

Controlled Polarized Optical Excitation Method on Ensembles of Nitrogen‐Vacancy Centers in Diamonds

AbstractCrystal axes must be distinguished in vector magnetic measurements of ensemble nitrogen‐vacancy (NV) centers in diamonds. However, achieving crystal axes distinction in confocal systems without a magnetic bias field is challenging. Thus, a controlled polarized optical excitation method to overcome this problem is proposed. The polarization angle of the excitation beam can be adjusted in free space using an optical pen for higher controllable degrees of freedom. Compared to previous optical excitation methods, the proposed method improves the maximum suppression by 19.2% and the maximum excitation by 42.4%. Moreover, the proposed method has a decoupling effect on NV axis resonances with a similar change trend. This method can easily replace existing optical excitation methods in NV measurement systems and is a powerful tool for ensembles of NV centers’ vector measurements without relying on magnetic bias fields.

Hybrid integration of ensemble nitrogen-vacancy centers in single-crystal diamond based on pick-flip-and-place transfer printing

Incorporating color centers in diamond with mature integrated photonics using hybrid integration techniques such as transfer printing provides a promising route toward scalable quantum applications. However, single-crystal diamond nanostructures fabricated using current etching technologies have triangular bottoms that are unsuitable for conventional pick-and-place integration. Herein, we present an alternative approach for deterministically integrating diamond nanostructures on chip. We demonstrate the hybrid integration of a diamond triangular nanobeam containing a nitrogen-vacancy ensemble on an SiO2 chip by picking it up using a weak adhesive film, flipping it, and transferring it to a stronger one. This “pick-flip-and-place” approach provides a flat diamond-chip interface, enabling the high-yield hybrid integration regardless of the shape of diamond nanostructures. Additionally, diamond nanofabrication is facilitated by transfer-printing hard masks for diamond etching. We also show that the integrated diamond nanobeam functions as a nanoscale quantum sensor. Our proposed approach paves the way toward scalable hybrid-diamond quantum photonics.

Charge states of nitrogen-vacancy centers in Fermi level controlled diamond n-i-n junctions

Control of the charge state of the nitrogen-vacancy (NV) center is crucial because of its instability and its transitions between the negative (NV–) and neutral (NV0) NV charge states under laser irradiation In this study, we fabricated an n-i-n junction, with an i-layer sandwiched between two phosphorus-doped n-layers; then, we measured the charge state of NV centers under steady state and laser irradiation in a known band structure where the Fermi energy changes gradually. The steady-state charge state measured by a nondestructive single shot exhibited stable NV– and NV0 signals when the Fermi level was even slightly above and below the transition level, respectively. This result indicates that the charge state can be significantly stabilized through band engineering. Both charge-state populations were observed only when the Fermi level was close to the transition level. Under continuous green laser irradiation, the ratio of NV– measured by the photoluminescence spectra changed gradually with the Fermi level in the depletion layer because of the balance between excitation from the laser and the supply of charge from the band. This outcome agrees reasonably with the calculated bands. Furthermore, we measured the PL spectra of the ensemble NV centers and discovered that their charge state can be well-controlled, as in the single NV center. The charge state of the i-layer at the interface can be stabilized by depositing a thin n-layer on the surface. These results would contribute significantly to improve sensor performance.

The Role of Electrolytes in the Relaxation of Near-Surface Spin Defects in Diamond.

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.