(2021) Nat. Mater.. Abstract
A plethora of single-photon emitters have been identified in the atomic layers of two-dimensional van der Waals materials. Here, we report on a set of isolated optical emitters embedded in hexagonal boron nitride that exhibit optically detected magnetic resonance. The defect spins show an isotropic ge-factor of ~2 and zero-field splitting below 10 MHz. The photokinetics of one type of defect is compatible with ground-state electron-spin paramagnetism. The narrow and inhomogeneously broadened magnetic resonance spectrum differs significantly from the known spectra of in-plane defects. We determined a hyperfine coupling of ~10 MHz. Its angular dependence indicates an unpaired, out-of-plane delocalized π-orbital electron, probably originating from substitutional impurity atoms. We extracted spin–lattice relaxation times T1 of 13–17 μs with estimated spin coherence times T2 of less than 1 μs. Our results provide further insight into the structure, composition and dynamics of single optically active spin defects in hexagonal boron nitride.
(2021) Nature Materials. Abstract[All authors]
A plethora of single-photon emitters have been identified in the atomic layers of two-dimensional van der Waals materials1,2,3,4,5,6,7,8. Here, we report on a set of isolated optical emitters embedded in hexagonal boron nitride that exhibit optically detected magnetic resonance. The defect spins show an isotropic ge-factor of ~2 and zero-field splitting below 10 MHz. The photokinetics of one type of defect is compatible with ground-state electron-spin paramagnetism. The narrow and inhomogeneously broadened magnetic resonance spectrum differs significantly from the known spectra of in-plane defects. We determined a hyperfine coupling of ~10 MHz. Its angular dependence indicates an unpaired, out-of-plane delocalized π-orbital electron, probably originating from substitutional impurity atoms. We extracted spin–lattice relaxation times T1 of 13–17 μs with estimated spin coherence times T2 of less than 1 μs. Our results provide further insight into the structure, composition and dynamics of single optically active spin defects in hexagonal boron nitride.
(2021) Physical Review Applied. 15, 3, 034066. Abstract
Radical pairs and the dynamics they undergo are prevalent in many chemical and biological systems. Specifically, it has been proposed that the radical-pair mechanism results from a relatively strong hyperfine interaction with its intrinsic nuclear spin environment. While the existence of this mechanism is undisputed, the nanoscale details remain to be experimentally shown. Here, we analyze the role of a quantum sensor in detecting the spin dynamics (non-Markovian) of individual radical pairs in the presence of a weak magnetic field. We show how quantum control methods can be used to set apart the dynamics of the radical-pair mechanism at various stages of the evolution. We expect these findings to have implications to the understanding of the physical mechanism in magnetoreception and other biochemical processes with a microscopic detail.
(2020) Nature Communications. 11, 6405. Abstract[All authors]
Atomic spins for quantum technologies need to be individually addressed and positioned with nanoscale precision. C60 fullerene cages offer a robust packaging for atomic spins, while allowing in-situ physical positioning at the nanoscale. However, achieving single-spin level readout and control of endofullerenes has so far remained elusive. In this work, we demonstrate electron paramagnetic resonance on an encapsulated nitrogen spin (14N@C60) within a C60 matrix using a single near-surface nitrogen vacancy (NV) center in diamond at 4.7 K. Exploiting the strong magnetic dipolar interaction between the NV and endofullerene electronic spins, we demonstrate radio-frequency pulse controlled Rabi oscillations and measure spin-echos on an encapsulated spin. Modeling the results using second-order perturbation theory reveals an enhanced hyperfine interaction and zero-field splitting, possibly caused by surface adsorption on diamond. These results demonstrate the first step towards controlling single endofullerenes, and possibly building large-scale endofullerene quantum machines, which can be scaled using standard positioning or self-assembly methods.
(2020) Nano Letters. 20, 1, p. 463-469 Abstract
Coupled micro- and nanomechanical oscillators are of fundamental and technical interest for emerging quantum technologies. Upon interfacing with long-lived solid-state spins, the coherent manipulation of the quantum hybrid system becomes possible even at ambient conditions. Although the ability of these systems to act as a quantum bus inducing long-range spin-spin interactions has been known, the possibility to coherently couple electron/nuclear spins to the common modes of multiple oscillators and map their mechanical motion to spin-polarization has not been experimentally demonstrated. We here report experiments on interfacing spins to the common modes of a coupled cantilever system and show their correlation by translating ultralow forces induced by radiation from one oscillator to a distant spin. Further, we analyze the coherent spin-spin coupling induced by the common modes and estimate the entanglement generation among distant spins.
(2020) National Science Review. 8, p. nwaa194 Abstract
Nitrogen-vacancy (NV) centers in diamond are promising quantum sensors for their long spin coherence time under ambient conditions. However, their spin resonances are relatively insensitive to non-magnetic parameters such as temperature. A magnetic-nanoparticle-nanodiamond hybrid thermometer, where the temperature change is converted to the magnetic field variation near the Curie temperature, was demonstrated to have enhanced temperature sensitivity (11mK Hz−1/2) [Phys. Rev. X 8, 011042 (2018)], but the sensitivity was limited by the large spectral broadening of ensemble spins in nanodiamonds. To overcome this limitation, here we show an improved design of a hybrid nanothermometer using a single NV center in a diamond nanopillar coupled with a single magnetic nanoparticle of copper-nickel alloy, and demonstrate a temperature sensitivity of 76 μK Hz−1/2. This hybrid design enables detection of 2 millikelvin temperature changes with temporal resolution of 5 milliseconds. The ultra-sensitive nanothermometer offers a new tool to investigate thermal processes in nanoscale systems.
(2017) Scientific Reports. 7, 14758. Abstract[All authors]
Low-dimensional wide bandgap semiconductors open a new playing field in quantum optics using sub-bandgap excitation. In this field, hexagonal boron nitride (h-BN) has been reported to host single quantum emitters (QEs), linking QE density to perimeters. Furthermore, curvature/perimeters in transition metal dichalcogenides (TMDCs) have demonstrated a key role in QE formation. We investigate a curvature-Abundant BN system-quasi one-dimensional BN nanotubes (BNNTs) fabricated via a catalyst-free method. We find that non-Treated BNNT is an abundant source of stable QEs and analyze their emission features down to single nanotubes, comparing dispersed/suspended material. Combining high spatial resolution of a scanning electron microscope, we categorize and pin-point emission origin to a scale of less than 20 nm, giving us a one-To-one validation of emission source with dimensions smaller than the laser excitation wavelength, elucidating nano-Antenna effects. Two emission origins emerge: hybrid/entwined BNNT. By artificially curving h-BN flakes, similar QE spectral features are observed. The impact on emission of solvents used in commercial products and curved regions is also demonstrated. The 'out of the box' availability of QEs in BNNT, lacking processing contamination, is a milestone for unraveling their atomic features. These findings open possibilities for precision engineering of QEs, puts h-BN under a similar 'umbrella' of TMDC's QEs and provides a model explaining QEs spatial localization/formation using electron/ion irradiation and chemical etching.
(2017) Science Advances. 3, 8, e1701116. Abstract[All authors]
Scalable quantum technologies require an unprecedented combination of precision and complexity for designing stable structures of well-controllable quantum systems on the nanoscale. It is a challenging task to find a suitable elementary building block, of which a quantum network can be comprised in a scalable way. We present the working principle of such a basic unit, engineered using molecular chemistry, whose collective control and readout are executed using a nitrogen vacancy (NV) center in diamond. The basic unit we investigate is a synthetic polyproline with electron spins localized on attached molecular side groups separated by a few nanometers. We demonstrate the collective readout and coherent manipulation of very few (
(2017) Review of Scientific Instruments. 88, 1, 013702. Abstract
Magnetic sensing and imaging instruments are important tools in biological and material sciences. There is an increasing demand for attaining higher sensitivity and spatial resolution, with implementations using a single qubit offering potential improvements in both directions. In this article we describe a scanning magnetometer based on the nitrogen-vacancy center in diamond as the sensor. By means of a quantum-assisted readout scheme together with advances in photon collection efficiency, our device exhibits an enhancement in signal to noise ratio of close to an order of magnitude compared to the standard fluorescence readout of the nitrogen-vacancy center. This is demonstrated by comparing non-assisted and assisted methods in a T-1 relaxation time measurement. Published by AIP Publishing.
(2017) Scientific Reports. 7, p. 14758 Abstract
Low-dimensional wide bandgap semiconductors open a new playing field in quantum optics using sub-bandgap excitation. In this field, hexagonal boron nitride (h-BN) has been reported to host single quantum emitters (QEs), linking QE density to perimeters. Furthermore, curvature/perimeters in transition metal dichalcogenides (TMDCs) have demonstrated a key role in QE formation. We investigate a curvature-abundant BN system – quasi one-dimensional BN nanotubes (BNNTs) fabricated via a catalyst-free method. We find that non-treated BNNT is an abundant source of stable QEs and analyze their emission features down to single nanotubes, comparing dispersed/suspended material. Combining high spatial resolution of a scanning electron microscope, we categorize and pin-point emission origin to a scale of less than 20 nm, giving us a one-to-one validation of emission source with dimensions smaller than the laser excitation wavelength, elucidating nano-antenna effects. Two emission origins emerge: hybrid/entwined BNNT. By artificially curving h-BN flakes, similar QE spectral features are observed. The impact on emission of solvents used in commercial products and curved regions is also demonstrated. The ‘out of the box’ availability of QEs in BNNT, lacking processing contamination, is a milestone for unraveling their atomic features. These findings open possibilities for precision engineering of QEs, puts h-BN under a similar ‘umbrella’ of TMDC’s QEs and provides a model explaining QEs spatial localization/formation using electron/ion irradiation and chemical etching.
Structural Attributes and Photodynamics of Visible Spectrum Quantum Emitters in Hexagonal Boron Nitride(2016) Nano Letters. 16, 11, p. 7037-7045 Abstract[All authors]
Newly discovered van der Waals materials like MoS2, WSe2, hexagonal boron nitride (h-BN), and recently C2N have sparked intensive research to unveil the quantum behavior associated with their 2D structure. Of great interest are 2D materials that host single quantum emitters. h-BN, with a band gap of 5.95 eV, has been shown to host single quantum emitters which are stable at room temperature in the UV and visible spectral range. In this paper we investigate correlations between hBN structural features and emitter location from bulk down to the monolayer at room temperature. We demonstrate that chemical etching and ion irradiation can generate emitters in h-BN. We analyze the emitters' spectral features and show that they are dominated by the interaction of their electronic transition with a single Raman active mode of h-BN. Photodynamics analysis reveals diverse rates between the electronic states of the emitter. The emitters show excellent photo stability even under ambient conditions and in monolayers. Comparing the excitation polarization between different emitters unveils a connection between defect orientation and the h-BN hexagonal structure. The sharp spectral features, color diversity, room-temperature stability, long-lived metastable states, ease of fabrication, proximity of the emitters to the environment, outstanding chemical stability, and biocompatibility of hBN provide a completely new class of systems that can be used for sensing and quantum photonics applications.
(2016) Journal of Magnetic Resonance. 269, p. 225-236 Abstract
Different approaches have improved the sensitivity of either electron or nuclear magnetic resonance to the single spin level. For optical detection it has essentially become routine to observe a single electron spin or nuclear spin. Typically, the systems in use are carefully designed to allow for single spin detection and manipulation, and of those systems, diamond spin defects rank very high, being so robust that they can be addressed, read out and coherently controlled even under ambient conditions and in a versatile set of nanostructures. This renders them as a new type of sensor, which has been shown to detect single electron and nuclear spins among other quantities like force, pressure and temperature. Adapting pulse sequences from classic NMR and EPR, and combined with high resolution optical microscopy, proximity to the target sample and nanoscale size, the diamond sensors have the potential to constitute a new class of magnetic resonance detectors with single spin sensitivity. As diamond sensors can be operated under ambient conditions, they offer potential application across a multitude of disciplines. Here we review the different existing techniques for magnetic resonance, with a focus on diamond defect spin sensors, showing their potential as versatile sensors for ultra-sensitive magnetic resonance with nanoscale spatial resolution.
(2015) Nano Letters. 15, 8, p. 4942-4947 Abstract
To study the magnetic dynamics of superparamagnetic nanoparticles, we use scanning probe relaxometry and dephasing of the nitrogen vacancy (NV) center in diamond, characterizing the spin noise of a single 10 nm magnetite particle. Additionally, we show the anisotropy of the NV sensitivity's dependence on the applied decoherence measurement method. By comparing the change in relaxation (T-1) and dephasing (T-2) time in the NV center when scanning a nanoparticle over it, we are able to extract the nanoparticle's diameter and distance from the NV center using an Ornstein- Uhlenbeck model for the nanoparticle's fluctuations. This scanning probe technique can be used in the future to characterize different spin label substitutes for both medical applications and basic magnetic nanoparticle behavior.
(2013) Nature Nanotechnology. 8, 9, p. 639-644 Abstract[All authors]
Superconducting quantum interference devices (SQUIDs) can be used to detect weak magnetic fields and have traditionally been the most sensitive magnetometers available. However, because of their relatively large effective size (on the order of 1 mu m)(1-4), the devices have so far been unable to achieve the level of sensitivity required to detect the field generated by the spin magnetic moment (mu(B)) of a single electron(5,6). Here we show that nanoscale SQUIDs with diameters as small as 46 nm can be fabricated on the apex of a sharp tip. The nano-SQUIDs have an extremely low flux noise of 50 n Phi(0) Hz(-1/2) and a spin sensitivity of down to 0.38 mu(B) Hz(-1/2), which is almost two orders of magnitude better than previous devices(2,3,7,8). They can also operate over a wide range of magnetic fields, providing a sensitivity of 0.6 mu(B) Hz(-1/2) at 1 T. The unique geometry of our nano-SQUIDs makes them well suited to scanning probe microscopy, and we use the devices to image vortices in a type II superconductor, spaced 120 nm apart, and to record magnetic fields due to alternating currents down to 50 nT.
Scanning superconducting quantum Interference device on a tip for magnetic imaging of nanoscale phenomena(2012) Review of Scientific Instruments. 83, 7, Abstract
We describe a new type of scanning probe microscope based on a superconducting quantum interference device (SQUID) that resides on the apex of a sharp tip. The SQUID-on-tip is glued to a quartz tuning fork which allows scanning at a tip-sample separation of a few nm. The magnetic flux sensitivity of the SQUID is 1.8 mu Phi(0)/root Hz and the spatial resolution is about 200 nm, which can be further improved. This combination of high sensitivity, spatial resolution, bandwidth, and the very close proximity to the sample provides a powerful tool for study of dynamic magnetic phenomena on the nanoscale. The potential of the SQUID-on-tip microscope is demonstrated by imaging of the vortex lattice and of the local ac magnetic response in superconductors. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4731656]
(2012) 26Th International Conference On Low Temperature Physics (Lt26), Pts 1-5. 400, Abstract
We present a SQUID of novel design, which is fabricated on the tip of a pulled quartz tube in a simple 3-step evaporation process without need for any additional processing, patterning, or lithography. The resulting devices have SQUID loops with typical diameters in the range 75 - 300 nm. They operate in magnetic fields up to 0.6 T and have flux sensitivity of 1.8 mu Phi(0)/Hz(1/2) and magnetic field sensitivity of 10(-7) T/Hz(1/2), which corresponds to a spin sensitivity of 65 mu B/Hz(1/2) for aluminum SQUIDs. The shape of the tip and the small area of the SQUID loop, together with its high sensitivity, make our device an excellent tool for scanning SQUID microscopy: With the SQUID-on-tip glued to a tine of a quartz tuning fork, we have succeeded in obtaining magnetic images of a patterned niobium film and of vortices in a superconducting film in a magnetic field.[All authors]
(2010) Nano Letters. 10, 3, p. 1046-1049 Abstract
A nanometer-sized superconducting quantum interference device (nanoSQUID) is fabricated on the apex of a sharp quartz tip and integrated into a scanning SQUID microscope, A simple self-aligned fabrication method results in nanoSQUIDs with diameters down to 100 nm with no lithographic processing. An aluminum nanoSQUID with an effective area of 0.034 mu m(2) displays flux sensitivity of 1.8 x 10(-6) Phi(0)/Hz(1/2) and operates in fields as high as 0.6 T. With projected spin sensitivity of 65 mu(B)/Hz(1/2) and high bandwidth, the SQUID on a Lip is a highly promising probe for nanoscale magnetic imaging and spectroscopy.[All authors]
(2009) Physical Review B. 80, 2, Abstract
Using micron-sized thermometers and Hall bars, we report time resolved studies of the local temperature and local magnetization for two types of magnetic avalanches (abrupt spin reversals) in the molecular magnet Mn-12 acetate, corresponding to avalanches of the main slow-relaxing crystalline form and avalanches of the fast-relaxing minor species that exists in all as-grown crystals of this material. An experimental protocol is used that allows the study of each type of avalanche without triggering avalanches in the other, and of both types of avalanches simultaneously. In samples prepared magnetically to enable both types of avalanches, minor species avalanches are found to act as a catalyst for the major species avalanches.
Effect of quantum tunneling on the ignition and propagation of magnetic avalanches in Mn(12) acetate(2007) Physical Review B. 76, 17, Abstract
Using a wire heater to ignite magnetic avalanches in fixed magnetic field applied along the easy axis of single crystals of the molecular magnet Mn(12) acetate, we report fast local measurements of the temperature and time-resolved measurements of the local magnetization as a function of magnetic field. In addition to confirming maxima in the velocity of propagation, we find that avalanches trigger at a threshold temperature which exhibits pronounced minima at resonant magnetic fields, demonstrating that thermally assisted quantum tunneling plays an important role in the ignition as well as the propagation of magnetic avalanches in molecular magnets.