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Janis Smits

Publications and source records attributed to Janis Smits.

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Optically detected nuclear magnetic resonance of carbon-13 in bulk diamond

Precision measurements based on optically detected nuclear magnetic resonance offer exquisite sensitivity to absolute shifts in spin transition frequencies, with potential applications in fundamental physics experiments and inertial sensing. We investigate 13C nuclear spins in diamond as a candidate system for solid-state implementations, which hold the promise for high-fidelity readout of large numbers of coherent nuclear spins in millitesla or lower magnetic fields. We demonstrate a technique that allows for both optical polarization and readout of large ensembles of ~10^{16} polarized nuclear spins. Our method takes advantage of state-selective Landau-Zener transitions under microwave frequency sweeping, which bidirectionally transfer spin polarization between Nitrogen-Vacancy (NV) electron spins and remote 13C nuclear spins. Using natural isotopic abundance diamonds with nitrogen densities of ~0.5-10 ppm, we perform optically-detected 13C Ramsey spectroscopy and realize a nuclear-spin-dependent fluorescence contrast exceeding 0.5% peak-to-peak. We observe nuclear spin dephasing times T2*~2 ms that only modestly improve with homonuclear dipolar decoupling, indicating that they are limited by the longitudinal spin relaxation of nearby NV electron spins. We study the magnetic field dependence of the optical readout and find comparable contrast and dephasing times for magnetic fields in the range 8-20 mT. Our method can be interpreted as a type of repetitive readout, where each NV center optically reads out the spin state of ~100 nuclei before nuclear spins depolarize.

quant-ph

Earth's field diamond vector magnetometry with isotropic magnetic flux concentrators

Vector magnetometers based on the optically detected magnetic resonance (ODMR) of nitrogen-vacancy centers in diamond are being developed for applications such as navigation and geomagnetism. However, at low magnetic fields, such as that on Earth (~50 {\mu}T), diamond magnetometers suffer from spectral congestion whereby ODMR peaks are not easily resolved. Here, we experimentally investigate a potential solution of using an isotropic, three-dimensional magnetic flux concentrator to amplify Earth's field without altering its direction. The concentrator consists of six ferrite cones, in a face-centered cubic arrangement, centered about a diamond. We vary the direction of a 50 {\mu}T applied field and record and fit the resulting ODMR spectra. By comparing the fitted fields to those of a reference fluxgate magnetometer, we characterize the angular response of the diamond magnetometer and quantify absolute errors in the field magnitude and angle. We find that the enhancement factor is nearly isotropic, with a mean of 19.05 and a standard deviation of 0.16, when weighted by solid angle coverage. Gradient broadening of the ODMR lines is sufficiently small that the spectra are well resolved for nearly all field directions, alleviating spectral congestion. For ~98% of the total 4{\pi} solid angle, Cram\'er-Rao lower bounds for magnetic field estimation uncertainty are within a factor of 2 of those of the fully-resolved case, indicating minimal deadzones. We track the stability of the magnetometer over six hours and observe variations less than or approximately 40 nT/hour, limited by temperature drift. Our study presents a new route for diamond vector magnetometry at Earth's field, with potential applications in geomagnetic surveys, anomaly detection, and navigation.

physics.ins-det

Chemically resolved nuclear magnetic resonance spectroscopy by longitudinal magnetization detection with a diamond magnetometer

Non-inductive magnetometers based on solid-state spins offer a promising solution for small-volume nuclear magnetic resonance (NMR) detection. A remaining challenge is to operate at a sufficiently high magnetic field to resolve chemical shifts at the part-per-billion level. Here, we demonstrate a Ramsey-M_z protocol that uses Ramsey interferometry to convert an analyte's transverse spin precession into a longitudinal magnetization (M_z), which is subsequently modulated and detected with a diamond magnetometer. We record NMR spectra at B0=0.32 T with a fractional spectral resolution of ~350 ppb, limited by the stability of the electromagnet bias field. We perform NMR spectroscopy on a ~1 nL detection volume of ethanol and resolve the chemical shift structure with negligible distortion. Through simulation, we show that the protocol can be extended to fields up to B0=3 T, with minimal spectral distortion, using composite nuclear-spin inversion pulses. For sub-nanoliter analyte volumes, we estimate a resolution of ~1 ppb and concentration sensitivity of ~40 mM s^{1/2} is feasible with improvements to the sensor design. Our results establish diamond magnetometers as high-resolution NMR detectors in the moderate magnetic field regime, with potential applications in metabolomics and pharmaceutical research.

physics.ins-det

The impact of microwave phase noise on diamond quantum sensing

Precision optical measurements of the electron-spin precession of nitrogen-vacancy (NV) centers in diamond form the basis of numerous applications. The most sensitivity-demanding applications, such as femtotesla magnetometry, require the ability to measure changes in GHz spin transition frequencies at the sub-millihertz level, corresponding to a fractional resolution of better than 10^{-12}. Here we study the impact of microwave (MW) phase noise on the response of an NV sensor. Fluctuations of the phase of the MW waveform cause undesired rotations of the NV spin state. These fluctuations are imprinted in the optical readout signal and, left unmitigated, are indistinguishable from magnetic field noise. We show that the phase noise of several common commercial MW generators results in an effective pT s^{1/2}-range noise floor that varies with the MW carrier frequency and the detection frequency of the pulse sequence. The data are described by a frequency domain model incorporating the MW phase noise spectrum and the filter-function response of the sensing protocol. For controlled injection of white and random-walk phase noise, the observed NV magnetic noise floor is described by simple analytic expressions that accurately capture the scaling with pulse sequence length and the number of pi pulses. We outline several strategies to suppress the impact of MW phase noise and implement a version, based on gradiometry, that realizes a >10-fold suppression. Our study highlights an important challenge in the pursuit of sensitive diamond quantum sensors and is applicable to other qubit systems with a large transition frequency.

quant-ph

Super-resolution diamond magnetic microscopy of superparamagnetic nanoparticles

Scanning-probe and wide-field magnetic microscopes based on Nitrogen-Vacancy (NV) centers in diamond have enabled remarkable 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 smaller characteristic NV-nanoparticle distance within nearby sensing voxels. We analyze the magnetic point-spread function and sensitivity as a function of the microscope's spatial resolution and 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 less than 10 mW laser power and can be parallelized by patterned illumination, introduces a new format for nanoscale magnetic imaging.

physics.optics

Nuclear quadrupole resonance spectroscopy with a femtotesla diamond magnetometer

Sensitive Radio-Frequency (RF) magnetometers that can detect oscillating magnetic fields at the femtotesla level are needed for demanding applications such as Nuclear Quadrupole Resonance (NQR) spectroscopy. RF magnetometers based on Nitrogen-Vacancy (NV) centers in diamond have been predicted to offer femtotesla sensitivity, but published experiments have largely been limited to the picotesla level. Here, we demonstrate a femtotesla RF magnetometer based on an NV-doped diamond membrane inserted between two ferrite flux concentrators. The device operates in bias magnetic fields of 2-10 microtesla and provides a ~300-fold amplitude enhancement within the diamond for RF magnetic fields in the 0.07-3.6 MHz range. The magnetometer's sensitivity is ~70 fT s^{1/2} at 0.35 MHz, and the noise floor decreases to below 2 fT after 1 hour of acquisition. We used this sensor to detect the 3.6 MHz NQR signal of 14N in sodium nitrite powder at room temperature. NQR signals are amplified by a resonant RF coil wrapped around the sample, allowing for higher signal-to-noise ratio detection. The diamond RF magnetometer's recovery time after a strong RF pulse is ~35 us, limited by the coil ring-down time. The sodium-nitrite NQR frequency shifts linearly with temperature as -1.00 +/- 0.02 kHz/K, the magnetization dephasing time is T2* = 887 +/- 51 us, and a spin-lock spin-echo pulse sequence extends the signal lifetime to 332 +/- 23 ms, all consistent with coil-based NQR studies. Our results expand the sensitivity frontier of diamond magnetometers to the femtotesla range, with potential applications in security, medical imaging, and materials science.

physics.ins-det

Tunable magnetic field source for magnetic field imaging microscopy

In this work we present a novel, compact, power efficient 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 field concentrators. A Hall probe and NV centers in diamond are used to demonstrate a proof of concept of a proposed magnetic field setup and to characterise 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/$\mu$m or 0.5 $\mu$T/$\mu$m at 222 mT in a 25$\times$25 $\mu$m field of view.

physics.app-ph

NV microscopy of thermally controlled stresses caused by Cr$_2$O$_3$ thin films

Many modern applications, including quantum computing and quantum sensing, use substrate-film interfaces. Particularly, thin films of chromium or titanium and their oxides are commonly used to bind various structures, such as resonators, masks, or microwave antennas, to a diamond surface. Due to different thermal expansions of involved materials, such films and structures could produce significant stresses, which need to be measured or predicted. In this paper, we demonstrate imaging of stresses in the top layer of diamond with deposited structures of Cr$_2$O$_3$ at temperatures 19$^{\circ}$C and 37$^{\circ}$C by using stress-sensitive optically detected magnetic resonances (ODMR) in NV centers. We also calculated stresses in the diamond-film interface by using finite-element analysis and correlated them to measured ODMR frequency shifts. As predicted by the simulation, the measured high-contrast frequency-shift patterns are only due to thermal stresses, whose spin-stress coupling constant along the NV axis is 21$\pm$1 MHz/GPa, that is in agreement with constants previously obtained from single NV centers in diamond cantilever. We demonstrate that NV microscopy is a convenient platform for optically detecting and quantifying spatial distributions of stresses in diamond-based photonic devices with micrometer precision and propose thin films as a means for local application of temperature-controlled stresses. Our results also show that thin film structures produce significant stresses in diamond substrates, which should be accounted for in NV-based applications.

physics.app-ph

Surface magnetic structure investigation of a nanolaminated Mn$_2$GaC thin film using a magnetic field microscope based on Nitrogen-Vacancy centers

This work presents a magnetic field imaging method based on color centers in diamond crystal applied to a thin film of a nanolaminated Mn$_2$GaC MAX phase. Magnetic properties of the surface related structures have been described around the first order transition at 214 K by performing measurements in the temperature range between 200 K and 235 K with the surface features fading out by increasing temperature above the transition temperature. The results presented here demonstrate how Nitrogen-Vacancy center based magnetic microscopy can supplement the traditionally used set of experimental techniques, giving additional information of microscopic scale magnetic field features, and allowing to investigate the temperature dependent magnetic behavior. The additional information acquired in this way is relevant to applications where surface magnetic properties are of essence.

physics.app-ph

Characterization of microscopic ferromagnetic defects in thin films using magnetic microscope based on Nitrogen-Vacancy centres

In this work we present results acquired by applying magnetic field imaging technique based on Nitrogen-Vacancy centres in diamond crystal for characterization of magnetic thin films defects. We used the constructed wide-field magnetic microscope for measurements of two kinds of magnetic defects in thin films. One family of defects under study was a result of non-optimal thin film growth conditions. The magnetic field maps of several regions of the thin films created under very similar conditions to previously published research revealed microscopic impurity islands of ferromagnetic defects, that potentially could disturb the magnetic properties of the surface. The second part of the measurements was dedicated to defects created post deposition - mechanical defects introduced in ferromagnetic thin films. In both cases, the measurements identify the magnetic field amplitude and distribution of the magnetic defects. In addition, the magnetic field maps were correlated with the corresponding optical images. As this method has great potential for quality control of different stages of magnetic thin film manufacturing process and it can rival other widely used measurement techniques, we also propose solutions for the optimization of the device in the perspective of high throughput.

physics.app-ph

Investigation of temperature dependence of magnetic properties of Cr$_2$O$_3$ thin film structure using a magnetic field imaging technique based on Nitrogen-Vacancy centres in diamond crystal

This work presents a magnetic field imaging method based on color centres in diamond crystal applied to thin film structure. To demonstrate the capacity of our device we have used it for characterization of magnetic properties in microscopic scale of Cr$_2$O$_3$ thin film structure above and below N\'eel temperature. The obtained measurement results clearly identify the detection of the magnetic phase transition of Cr$_2$O$_3$ thin film with an unexpected diamagnetic like behaviour at 19$^{\circ}$C (below the N\'eel temperature of Cr$_2$O$_3$). To have better insights in the magnetic fields created by the thin films we present simulations of the magnetic fields near the thin film surface. We also analysed the optically detected magnetic resonance (ODMR) profiles to be sure that the measured property is related only to the shift of the optically detected magnetic resonance. We demonstrate how Nitrogen-Vacancy centre based magnetometry can deliver a convenient platform for research of phase transition dynamics and spatial magnetic field distributions of thin films, that can rival other widely used measurement techniques.

physics.app-ph

Cross-relaxation studies with optically detected magnetic resonances in nitrogen-vacancy centers in diamond in an external magnetic field

In this paper cross-relaxation between nitrogen-vacancy (NV) centers and substitutional nitrogen in a diamond crystal was studied. It was demonstrated that optically detected magnetic resonance signals (ODMR) can be used to measure these signals successfully. The ODMR were detected at axial magnetic field values around 51.2~mT in a diamond sample with a relatively high (200~ppm) nitrogen concentration. We observed transitions that involve magnetic sublevels that are split by the hyperfine interaction. Microwaves in the frequency ranges from 1.3 GHz to 1.6 GHz ($m_S=0\longrightarrow m_S=-1$ NV transitions) and from 4.1 to 4.6 GHz ($m_S=0\longrightarrow m_S=+1$ NV transitions) were used. To understand the cross-relaxation process in more detail and, as a result, reproduce measured signals more accurately, a model was developed that describes the microwave-initiated transitions between hyperfine levels of the NV center that are undergoing anti-crossing and are strongly mixed in the applied magnetic field. Additionally, we simulated the extent to which the microwave radiation used to induce ODMR in the NV center also induced transitions in the substitutional nitrogen via cross-relaxation. The improved understanding of the NV processes in the presence of a magnetic field will be useful for designing NV-diamond-based devices for a wide range of applications from implementation of q-bits to hyperpolarization of large molecules to various quantum technological applications such as field sensors.

quant-ph

Diamond magnetometer enhanced by ferrite flux concentrators

Magnetometers based on nitrogen-vacancy (NV) centers in diamond are promising room-temperature, solid-state sensors. However, their reported sensitivity to magnetic fields at low frequencies (<1 kHz) is presently >10 pT s^{1/2}, precluding potential applications in medical imaging, geoscience, and navigation. Here we show that high-permeability magnetic flux concentrators, which collect magnetic flux from a larger area and concentrate it into the diamond sensor, can be used to improve the sensitivity of diamond magnetometers. By inserting an NV-doped diamond membrane between two ferrite cones in a bowtie configuration, we realize a ~250-fold increase of the magnetic field amplitude within the diamond. We demonstrate a sensitivity of ~0.9 pT s^{1/2} to magnetic fields in the frequency range between 10 and 1000 Hz, using a dual-resonance modulation technique to suppress the effect of thermal shifts of the NV spin levels. This is accomplished using 200 mW of laser power and 20 mW of microwave power. This work introduces a new dimension for diamond quantum sensors by using micro-structured magnetic materials to manipulate magnetic fields.

physics.ins-det

Achromatic varifocal metalens for the visible spectrum

Metasurface optics provide an ultra-thin alternative to conventional refractive lenses. A present challenge is in realizing metasurfaces that exhibit tunable optical properties and achromatic behavior across the visible spectrum. Here, we report the design, fabrication, and characterization of metasurface lenses ("metalenses") that use asymmetric TiO2 nanostructures to induce a polarization-dependent optical response. By rotating the polarization of linearly-polarized input light, the focal length of a 40 micrometer-diameter metalens is tuned from 220-550 micrometers with nearly diffraction-limited performance. We show that imparting a wavelength-dependent polarization rotation on incident light enables achromatic focusing over a wide band of the visible spectrum, 483-620 nm. We use this property to demonstrate varifocal color imaging with white light from a halogen source. Tunable achromatic metalenses may be useful for applications in imaging and display.

physics.optics

Two-dimensional nuclear magnetic resonance spectroscopy with a microfluidic diamond quantum sensor

Quantum sensors based on nitrogen-vacancy centers in diamond have emerged as a promising detection modality for nuclear magnetic resonance (NMR) spectroscopy owing to their micron-scale detection volume and non-inductive based detection. A remaining challenge is to realize sufficiently high spectral resolution and concentration sensitivity for multidimensional NMR analysis of picoliter sample volumes. Here, we address this challenge by spatially separating the polarization and detection phases of the experiment in a microfluidic platform. We realize a spectral resolution of 0.65 +/- 0.05 Hz, an order-of-magnitude improvement over previous diamond NMR studies. We use the platform to perform two-dimensional correlation spectroscopy of liquid analytes within an effective ~20 picoliter detection volume. The use of diamond quantum sensors as in-line microfluidic NMR detectors is a significant step towards applications in mass-limited chemical analysis and single cell biology.

physics.ins-det

Diamond magnetic microscopy of malarial hemozoin nanocrystals

Magnetic microscopy of malarial hemozoin nanocrystals was performed using optically detected magnetic resonance imaging of near-surface diamond nitrogen-vacancy centers. Hemozoin crystals were extracted from $Plasmodium$-$falciparum$-infected human blood cells and studied alongside synthetic hemozoin crystals. The stray magnetic fields produced by individual crystals were imaged at room temperature as a function of applied field up to 350 mT. More than 100 nanocrystals were analyzed, revealing the distribution of their magnetic properties. Most crystals ($96\%$) exhibit a linear dependence of stray field magnitude on applied field, confirming hemozoin's paramagnetic nature. A volume magnetic susceptibility $\chi=3.4\times10^{-4}$ is inferred using a magnetostatic model informed by correlated scanning electron microscopy measurements of crystal dimensions. A small fraction of nanoparticles (4/82 for $Plasmodium$-produced and 1/41 for synthetic) exhibit a saturation behavior consistent with superparamagnetism. Translation of this platform to the study of living malaria-infected cells may shed new light on hemozoin formation dynamics and their interaction with antimalarial drugs.

cond-mat.mes-hall