Optically Detected Magnetic Resonance Research Articles

High-SNR Magnetic Field Sensing Using Portable Confocal Magnetometer Probe Based on Nitrogen Vacancy Centers in Diamond

In recent years, nitrogen vacancy (NV) centers have shown great potential for application in quantum sensor research due to their high sensitivity to magnetic fields and excellent spatial resolution. However, in practical applications, it is necessary to eliminate environmental requirements and bulky instruments brought by the optical detection of magnetic resonance (ODMR) measurement method.. In this paper, we propose an efficient portable magnetometer with a miniature confocal system (CSPM) to resist background noise and improve integration. The confocal system can automatically focus, and the volume is limited to 11 cm3. Moreover, a fiber optic flange, an antenna and a homemade integrated photodetector are integrated in the magnetometer to achieve the actual sensitivity of sub-40 nT/Hz1/2. In the experimental process of optimizing system parameters, we discovered the important influence of beam focusing or microwave uniform operation on the detection signal and proposed specific optimization methods, which have guiding significance for future integrated design. Through comparative experiments with an integration scheme that does not use uniform operation, we found that the CSPM reduces the system noise by 4.2 times and that the signal-to-noise ratio (SNR) increases by 6.2 dB.

Integration of Fluorescent, NV-Rich Nanodiamond Particles with AFM Cantilevers by Focused Ion Beam for Hybrid Optical and Micromechanical Devices

In this paper, a novel fabrication technology of atomic force microscopy (AFM) probes integrating cantilever tips with an NV-rich diamond particle is presented. Nanomanipulation techniques combined with the focused electron beam-induced deposition (FEBID) procedure were applied to position the NV-rich diamond particle on an AFM cantilever tip. Ultrasonic treatment of nanodiamond suspension was applied to reduce the size of diamond particles for proper geometry and symmetry. The fabricated AFM probes were tested utilizing measurements of the electrical resistance at highly oriented pyrolytic graphite (HOPG) and compared with a standard AFM cantilever performance. The results showed novel perspectives arising from combining the functionalities of a scanning AFM with optically detected magnetic resonance (ODMR). In particular, it offers enhanced magnetometric sensitivity and the nanometric resolution.

Preferential Placement of Aligned Nitrogen Vacancy Centers in Chemical Vapor Deposition Overgrown Diamond Microstructures

The usefulness of nitrogen vacancy (NV) centers in diamond is augmented by a low defect and impurity density in the surrounding host material, and applications benefit from the ability to control the position of the NV centers. Herein, a process to create NV centers on single‐crystalline diamond microstructures by chemical vapor deposition (CVD) is presented. Pyramidal structures with {111} side facets are formed during the intrinsic overgrowth of dry chemically etched cylindrical pillars on a substrate with {100} surface orientation. A thin nitrogen‐doped epitaxial layer is deposited on top of the pyramids resulting in the creation of NV centers exclusively on the {111} pyramid side faces. Optically detected magnetic resonance (ODMR) and spin echo measurements reveal preferential alignment of the NV centers in a single {111} direction and a time of . The time of the NV centers is limited by the surrounding substitutional nitrogen (P1 center) concentration of . A low density of other paramagnetic spin noise is detected by double‐electron electron resonance (DEER) measurements.

A compact two-dimensional quantum magnetometer module based on the fixed-frequency optical detection of magnetic resonance using nitrogen vacancy centers

In this Letter, we propose an integrated two-dimensional magnetometer module based on nitrogen vacancy centers in diamond. The sensor has a constructed area of 7.12 cm2 and exhibits a magnetic-field sensitivity of approximately 25.12 nT/Hz1/2. By placing anti-microwave shield nets optimizing interference distance, the integrated scheme eliminates the effects of microwave interference on the amplifier. We propose the fixed-frequency optical detection of magnetic resonance, which is used to measure the relation between the magnetic field and the photoluminescence by scanning the magnetic field. Without relying on the lock-in technique, we developed an algorithm for analyzing the magnetic noise based on the PL noise analysis.

High-Contrast Plasmonic-Enhanced Shallow Spin Defects in Hexagonal Boron Nitride for Quantum Sensing.

The recently discovered spin defects in hexagonal boron nitride (hBN), a layered van der Waals material, have great potential in quantum sensing. However, the photoluminescence and the contrast of the optically detected magnetic resonance (ODMR) of hBN spin defects are relatively low so far, which limits their sensitivity. Here we report a record-high ODMR contrast of 46% at room temperature and simultaneous enhancement of the photoluminescence of hBN spin defects by up to 17-fold by the surface plasmon of a gold film microwave waveguide. Our results are obtained with shallow boron vacancy spin defects in hBN nanosheets created by low-energy He+ ion implantation and a gold film microwave waveguide fabricated by photolithography. We also explore the effects of microwave and laser powers on the ODMR and improve the sensitivity of hBN spin defects for magnetic field detection. Our results support the promising potential of hBN spin defects for nanoscale quantum sensing.

Long-Lived Ensembles of Shallow NV– Centers in Flat and Nanostructured Diamonds by Photoconversion

Shallow, negatively charged nitrogen-vacancy centers (NV–) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV0 centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm2). Fluorescence spectroscopy, optically detected magnetic resonance (ODMR), and charge-photoconversion detection are applied to characterize the properties and dynamics of NV– and NV0 centers. We demonstrate that high laser power strongly promotes photoconversion of NV0 to NV– centers. Surprisingly, the excess NV– population is stable over a timescale of 100 ms after switching off the laser, resulting in long-lived enrichment of shallow NV–. The beneficial effect of photoconversion is less marked in nanostructured samples. Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV– centers in diamond.

Optical charge state manipulation of divacancy spins in silicon carbide under resonant excitation

Spin defects in silicon carbide (SiC) have attracted much attentions in various quantum technologies. In this work, we study the optical manipulation of charge state and coherent control of multifold divacancy spins ensemble in SiC under resonant excitation. The results reveal that the resonantly excited divacancy ensemble counts have dozens of enhancements by repumping a higher-energy laser. Moreover, it has a similar optimal repump laser wavelength of around 670 nm for multiple divacancies. On the basis of this, the optically detected magnetic resonance (ODMR) experiment shows that repump lasers with different wavelengths do not affect the ODMR contrast and line width. In addition, the repump lasers also do not change the divacancy spins’ coherence times. The experiments pave the way for using the optimal repump excitation method for SiC-based quantum information processing and quantum sensing.

Optically Enhanced Electric Field Sensing Using Nitrogen-Vacancy Ensembles

Nitrogen-vacancy (NV) centers in diamond have shown promise as inherently localized electric-field sensors, capable of detecting individual charges with nanometer resolution. Working with NV ensembles, we demonstrate that a detailed understanding of the internal electric field environment enables enhanced sensitivity in the detection of external electric fields. We follow this logic along two complementary paths. First, using excitation tuned near the NV's zero-phonon line, we perform optically detected magnetic resonance (ODMR) spectroscopy at cryogenic temperatures in order to precisely measure the NV center's excited-state susceptibility to electric fields. In doing so, we demonstrate that the characteristically observed contrast inversion arises from an interplay between spin-selective optical pumping and the NV centers' local charge distribution. Second, motivated by this understanding, we propose and analyze a novel scheme for optically-enhanced electric-field sensing using NV ensembles; we estimate that our approach should enable order of magnitude improvements in the DC electric-field sensitivity.

Towards ab initio identification of paramagnetic substitutional carbon defects in hexagonal boron nitride acting as quantum bits

Paramagnetic substitutional carbon (${\mathrm{C}}_{\text{B}},{\mathrm{C}}_{\text{N}}$) defects in hexagonal boron nitride are discussed as candidates for quantum bits. Their identification and suitability are approached by means of photoluminescence (PL), charge transitions, electron paramagnetic resonance, and optically detected magnetic resonance (ODMR) spectra. Several clear trends in these are revealed by means of an efficient plane wave periodic supercell ab initio density functional theory approach. In particular, this yields insight into the role of the separation between ${\mathrm{C}}_{\text{B}}$ and ${\mathrm{C}}_{\text{N}}$. In most of the cases, the charge transition between the neutral and a singly charged ground state of a defect is predicted to be experimentally accessible, since the charge transition level position lies within the band gap. A posteriori charge corrections are also discussed. A near-identification of an experimentally isolated single spin center as the neutral ${\mathrm{C}}_{\text{B}}$ point defect was found via comparison of results to recently observed PL and ODMR spectra.

Altering the exciton landscape by removal of specific chlorophylls in monomeric LHCII provides information on the sites of triplet formation and quenching by means of ODMR and EPR spectroscopies

The triplet states populated under illumination in the monomeric light-harvesting complex II (LHCII) were analyzed by EPR and Optically Detected Magnetic Resonance (ODMR) in order to fully characterize the perturbations introduced by site-directed mutations leading to the removal of key chlorophylls. We considered the A2 and A5 mutants, lacking Chls a612(a611) and Chl a603 respectively, since these Chls have been proposed as the sites of formation of triplet states which are subsequently quenched by the luteins. Chls a612 and Chl a603 belong to the two clusters determining the low energy exciton states in the complex. Their removal is expected to significantly alter the excitation energy transfer pathways. On the basis of the TR- and pulse EPR triplet spectra, the two symmetrically related pairs constituted by Chl a612/Lut620 and Chl a603/Lut621 were both possible candidate for triplet-triplet energy transfer (TTET). However, the ODMR results clearly show that only Lut620 is involved in triplet quenching. In the A5 mutant, the Chl a612/Lut620 pair retains this pivotal photoprotective role, while the A2 mutant was found to activate an alternative pathway involving the Chl a603/Lut621pair. These results shows that LHCII is characterized by a robust photoprotective mechanism, able to adapt to the removal of individual chromophores while maintaining a remarkable degree of Chl triplet quenching. Small amounts of unquenched Chl triplet states were also detected. The analysis of the results allowed us to assign the sites of “unquenched” chlorophyll triplets to Chl a610 and Chl a602.

Magnetic Field Mapping Around Individual Magnetic Nanoparticle Agglomerates Using Nitrogen‐Vacancy Centers in Diamond

AbstractA modified diamond–photonics based metrology is proposed to explore the magnetic fields created by agglomerates of magnetic nanoparticles (MNPs). MNPs are promising for environmental and medical applications; those proposed for cancer magnetic hyperthermia treatments are small superparamagnetic <20 nm iron oxide particles. Inside cells, they assemble in larger MNP agglomerates, reaching cross‐sections of several micrometers. Here, these conditions are reproduced and MNP agglomerates immobilized. Optically detected magnetic resonance (ODMR) signals recorded without a bias field in a confocal microscope and scanning across a homogenous shallow layer of fluorescent nitrogen‐vacancy centers in a bulk diamond sample placed in direct contact with the MNP agglomerates are used to determine magnetic fields with a spatial resolution of 500 nm in a lateral direction. This spatial resolution allows determining magnetic field maps around individual MNP agglomerates, for which magnetic fields with strengths ranging from 0.03 mT to maximal 1.2 mT in the direct vicinity of the agglomerates and with detectable fields up to 5 µm away from the agglomerates, are determined. Based on the findings, a pathway to non‐invasively study the micro/nano topology of MNP agglomerates is proposed.

Robust coherent control of solid-state spin qubits using anti-Stokes excitation

Optically addressable solid-state color center spin qubits have become important platforms for quantum information processing, quantum networks and quantum sensing. The readout of color center spin states with optically detected magnetic resonance (ODMR) technology is traditionally based on Stokes excitation, where the energy of the exciting laser is higher than that of the emission photons. Here, we investigate an unconventional approach using anti-Stokes excitation to detect the ODMR signal of silicon vacancy defect spin in silicon carbide, where the exciting laser has lower energy than the emitted photons. Laser power, microwave power and temperature dependence of the anti-Stokes excited ODMR are systematically studied, in which the behavior of ODMR contrast and linewidth is shown to be similar to that of Stokes excitation. However, the ODMR contrast is several times that of the Stokes excitation. Coherent control of silicon vacancy spin under anti-Stokes excitation is then realized at room temperature. The spin coherence properties are the same as those of Stokes excitation, but with a signal contrast that is around three times greater. To illustrate the enhanced spin readout contrast under anti-Stokes excitation, we also provide a theoretical model. The experiments demonstrate that the current anti-Stokes excitation ODMR approach has promising applications in quantum information processing and quantum sensing.

Differential sensitivity to oxygen among the bacteriochlorophylls g in the type-I reaction centers of Heliobacterium modesticaldum.

The type-I, homodimeric photosynthetic reaction center (RC) of Heliobacteria (HbRC) is the only known RC in which bacteriochlorophyll g (BChl g) is found. It is also simpler than other RCs, having the smallest number of protein subunits and bound chromophores of any type-I RC. In the presence of oxygen, BChl g isomerizes to 81-hydroxychlorophyll aF (Chl aF). This naturally occurring process provides a way of altering the chlorophylls and studying the effect of these changes on energy and electron transfer. Transient absorbance difference spectroscopy reveals that triplet-state formation occurs in the antenna chlorophylls of HbRCs but does not provide site-specific information. Here, we report on an extended optically detected magnetic resonance (ODMR) study of the antenna triplet states in HbRCs with differing levels of conversion of BChl g to Chl aF. The data reveal pools of BChl g molecules with different triplet zero-field splitting parameters and different susceptibilities to chemical oxidation. By relating the detailed spectroscopic characteristics derived from the ODMR data to the recently solved crystallographic structure, we have tentatively identified BChl g molecules in which the probability of triplet formation is high and sites at which BChl g conversion is more likely, providing useful information about the fate of the excitation in the complex.

Hyperfine Interactions in the NV-13C Quantum Registers in Diamond Grown from the Azaadamantane Seed.

Nanostructured diamonds hosting optically active paramagnetic color centers (NV, SiV, GeV, etc.) and hyperfine-coupled with them quantum memory 13C nuclear spins situated in diamond lattice are currently of great interest to implement emerging quantum technologies (quantum information processing, quantum sensing and metrology). Current methods of creation such as electronic-nuclear spin systems are inherently probabilistic with respect to mutual location of color center electronic spin and 13C nuclear spins. A new bottom-up approach to fabricate such systems is to synthesize first chemically appropriate diamond-like organic molecules containing desired isotopic constituents in definite positions and then use them as a seed for diamond growth to produce macroscopic diamonds, subsequently creating vacancy-related color centers in them. In particular, diamonds incorporating coupled NV-13C spin systems (quantum registers) with specific mutual arrangements of NV and 13C can be obtained from anisotopic azaadamantane molecule. Here we predict the characteristics of hyperfine interactions (hfi) for the NV-13C systems in diamonds grown from various isotopically substituted azaadamantane molecules differing in 13C position in the seed, as well as the orientation of the NV center in the post-obtained diamond. We used the spatial and hfi data simulated earlier for the H-terminated cluster C510[NV]-H252. The data obtained can be used to identify (and correlate with the seed used) the specific NV-13C spin system by measuring, e.g., the hfi-induced splitting of the mS = ±1 sublevels of the NV center in optically detected magnetic resonance (ODMR) spectra being characteristic for various NV-13C systems.

Wide-Field Dynamic Magnetic Microscopy Using Double-Double Quantum Driving of a Diamond Defect Ensemble

Wide-field magnetometry can be realized by imaging the optically-detected magnetic resonance of diamond nitrogen vacancy (NV) center ensembles. However, NV ensemble inhomogeneities significantly limit the magnetic-field sensitivity of these measurements. We demonstrate a double-double quantum (DDQ) driving technique to facilitate wide-field magnetic imaging of dynamic magnetic fields at a micron scale. DDQ imaging employs four-tone radio frequency pulses to suppress inhomogeneity-induced variations of the NV resonant response. As a proof-of-principle, we use the DDQ technique to image the dc magnetic field produced by individual magnetic-nanoparticles tethered by single DNA molecules to a diamond sensor surface. This demonstrates the efficacy of the diamond NV ensemble system in high-frame-rate magnetic microscopy, as well as single-molecule biophysics applications.

Optically detected flip-flops between different spin ensembles in diamond

We employ the technique of optical detection of magnetic resonance to study dipolar interaction in diamond between nitrogen-vacancy color centers of different crystallographic orientations and substitutional nitrogen defects. We demonstrate optical measurements of resonant spin flips-flips (second Larmor line), and flip-flops between different spin ensembles in diamond. In addition, the strain coupling between the nitrogen-vacancy color centers and bulk acoustic modes is studied using optical detection. Our findings may help optimizing cross polarization protocols, which, in turn, may allow improving the sensitivity of diamond-based detectors.

Preferential coupling of diamond NV centres in step-index fibres.

Diamonds containing the negatively charged nitrogen-vacancy centre are a promising system for room-temperature magnetometry. The combination of nano- and micro-diamond particles with optical fibres provides an option for deploying nitrogen-vacancy magnetometers in harsh and challenging environments. Here we numerically explore the coupling efficiency from nitrogen-vacancy centres within a diamond doped at the core/clad interface across a range of commercially available fibre types so as to inform the design process for a diamond in fibre magnetometers. We determine coupling efficiencies from nitrogen-vacancy centres to the guided modes of a step-index fibre and predict the optically detected magnetic resonance (ODMR) generated by a ensemble of four nitrogen-vacancy centres in this hybrid fibre system. Our results show that the coupling efficiency is enhanced with a high refractive index difference between the fibre core and cladding and depends on the radial position of the nitrogen-vacancy centres in the fibre core. Our ODMR simulations show that due to the preferential coupling of the nitrogen-vacancy emission to the fibre guided modes, certain magnetometry features such as ODMR contrast can be enhanced and lead to improved sensitivity in such diamond-fibre systems, relative to conventional diamond only ensemble geometries.

Optimizing Optical Tweezers Experiments for Magnetic Resonance Sensing with Nanodiamonds

In this Article we explore the requirements for enabling high quality optically detected magnetic resonance (ODMR) spectroscopy in a conventional gradient force optical tweezers using nanodiamonds containing nitrogen-vacancy (NV-) centers. We find that modulation of the infrared (1064 nm) trapping laser during spectroscopic measurements substantially improves the ODMR contrast compared with continuous wave trapping. The work is significant as it allows trapping and quantum sensing protocols to be performed in conditions where signal contrast is substantially reduced. We demonstrate the utility of the technique by resolving NV- spin projections within the ODMR spectrum. Manipulating the orientation of the nanodiamond via the trapping laser polarization, we observe changes in spectral features. Theoretical modeling then allows us to infer the crystallographic orientation of the NV-. This is an essential capability for future magnetic sensing applications of optically trapped nanodiamonds.

Single-channel vector magnetic information detection method based on diamond NV color center* *Project supported by the National Natural Science Foundation of China (Grant Nos. 51635011, 51805493, 51775522, 51727808, and 51922009), the Applied Basic Research Program in Shanxi Province, China (Grant No. 201901D111011(ZD)), the Key Research and Development Program in Shanxi Province, China (Grant No. 201803D121067), the Fund from the Key

A method of detecting the single channel triaxial magnetic field information based on diamond nitrogen-vacancy (NV) color center is introduced. Firstly, the incident angle of the bias magnetic field which can achieve the equal frequency difference optically-detected magnetic resonance (ODMR) spectrum of diamond NV color center is calculated theoretically, and the triaxial magnetic information solution model is also constructed. Secondly, the microwave time-controlled circuit module is designed to generate equal timing and equal frequency difference microwave pulse signals in one channel. Combining with the optical detection magnetic resonance technology, the purpose of sequentially locking and detecting the four formant signals on one side of the diamond NV color center (m s = –1 state signal) is achieved, and the vector magnetic field information detection is accomplished by combining the triaxial magnetic information solution model. The system can obtain magnetic field detection in a range of 0 mT–0.82 mT. The system’s magnetic noise sensitivity is 14.2 nT/Hz1/2, and the deviation angle errors of magnetic field detection θx and θy are 1.3° and 8.2° respectively.

Wide-field fluorescent nanodiamond spin measurements toward real-time large-area intracellular thermometry

Measuring optically detected magnetic resonance (ODMR) of diamond nitrogen vacancy centers significantly depends on the photon detectors used. We study camera-based wide-field ODMR measurements to examine the performance in thermometry by comparing the results to those of the confocal-based ODMR detection. We show that the temperature sensitivity of the camera-based measurements can be as high as that of the confocal detection and that possible artifacts of the ODMR shift are produced owing to the complexity of the camera-based measurements. Although measurements from wide-field ODMR of nanodiamonds in living cells can provide temperature precisions consistent with those of confocal detection, the technique requires the integration of rapid ODMR measurement protocols for better precisions. Our results can aid the development of camera-based real-time large-area spin-based thermometry of living cells.