Magnetometry with nitrogen-vacancy (NV) centers in diamond has so far been measured via emission of light from NV centers or via absorption at the singlet transition at 1042 nm. Here, we demonstrate a phenomenon of broadband optical absorption by the NV centers starting in the emission wavelength and reaching up to 1000 nm. The measurements are enabled by a high-finesse cavity, which is used for room-temperature continuous wave pump-probe experiments. The red to infrared probe beam shows the typical optically detected magnetic resonance (ODMR) signal of the NV spin with contrasts up to 42 %. This broadband optical absorption has not yet been reported in terms of NV magnetometry. We argue that the lower level of the absorbing transition could be the energetically lower NV singlet state, based on the increased optical absorption for a resonant microwave field and the spectral behavior. Investigations of the photon-shot-noise-limited sensitivity show improvements with increasing probe wavelength, reaching an optimum of 7.5pT/Hz. The results show significantly improved ODMR contrast compared to emission-based magnetometry. This opens a new detection wavelength regime with coherent laser signal detection for high-sensitivity NV magnetometry.
Nitrogen-vacancy centers (NV) in diamond are promising quantum systems for magnetic field sensing. The sensitivity and the linearity of such a quantum sensor can be greatly improved by using stimulated emission of the NV centers in the concept of laser threshold magnetometry (LTM), which is projected to reach the fT/sqrt(Hz) regime. Previous implementations of NV centers in optical cavities relied on external seed lasers, pulsed operation, or sensing via NVabsorption. In our work, we combine the NV centers with a second gain medium, a laser diode, within the same cavity, achieving self-sustainable continuous-wave lasing. This approach compensates the intrinsic losses of the cavity and the diamond, through a fixed additional gain below the threshold of the laser system. A continuous-wave laser threshold and a linewidth narrowing is observed with increasing pump power on the NV centers of the combined laser system. An improved laser system shows a magnetic field-dependent laser threshold, which is the basis for improved-sensitivity NV magnetometry via LTM.
Diamond is a potential host material for laser applications due to its exceptional thermal properties, ultrawide bandgap, and color centers, which promise gain across the visible spectrum. More recently, coherent laser methods offer improved sensitivity for magnetometry. However, diamond fabrication is difficult in comparison to other crystalline matrices, and many optical loss channels are not yet understood. Here, we demonstrate a continuous-wave laser threshold as a function of the pump intensity on nitrogen-vacancy (NV) color centers. To achieve this, we constructed a laser cavity with both an NV diamond medium and an intracavity antireflection-coated diode laser. This dual-medium approach compensates intrinsic losses of the cavity by providing a fixed additional gain below threshold of the diode laser. We observe a continuous-wave laser threshold of the laser system and linewidth narrowing with increasing green pump power on the NV centers. Our results are a major development toward coherent approaches to magnetometry.
The use of quantum sensors is promising detailed insights into physical phenomena such as magnetism or superconductivity. One example of such quantum sensors is a microscopic diamond tip containing nitrogen vacancy (NV) centers, which is capable of producing correlated measurements of vectorial magnetic fields and the sample topography on the nanoscale. In this study, we present a chemical vapor deposition (CVD) process to produce diamond tips with NV centers by overgrowing microstructured diamond substrates. The resulting diamond tips exhibit a radius of curvature of approximately 10 nm, suitable for use as a probe in an atomic force microscope. The magnetic sensitivity of the CVD-grown diamond tips is characterized with pulsed measurements of the optically detected magnetic resonance, which yield a minimum magnetic sensitivity of 60 mu T Hz-1 . The growth of the diamond microstructures is observed to differ from the commonly used geometric model predicting CVD growth of bulk diamond crystals. We identify an empirical model for the growth behavior of the microstructures by taking into account processes described in the step flow growth model for crystals. Additionally, we demonstrate the applicability of the developed CVD growth process to membrane substrates required for the preparation of magnetometry-capable diamond tips.
A challenge to this day in the development of diamond devices for quantum applications is the laterally defined and closely spaced positioning of nitrogen-vacancy centres with exceptional coherence properties. Here, we demonstrate a maskless, implantation-free method for the controlled in-plane positioning of NV centres using a combination of focused ion beam (FIB) milling, plasma etching and nitrogen-doped diamond growth. The Ga+ ion beam milling resulted in 1 mu m x 1 mu m cavities with depths of up to 450 nm, each cavity exhibiting the four [111]-oriented diamond facets after pure hydrogen plasma treatment and a depth of 700 nm. Low-methane, nitrogen-doped chemical vapour deposition (CVD) overgrowth resulted in in situ formation of oriented NV ensembles, exclusively perpendicular to the {111}-planes.
Widefield magnetometry based on nitrogen-vacancy centers enables high spatial resolution imaging of magnetic field distributions without a need for spatial scanning. In this work, we show nitrogen-vacancy center magnetic imaging of Fe3O4 nanoparticles within the gastrointestinal tract of Drosophila melanogaster larvae. Vector magnetic field imaging based on optically detected magnetic resonance is carried out on dissected larvae intestine organs containing accumulations of externally loaded magnetic nanoparticles. The distribution of the magnetic nanoparticles within the tissue can be clearly deduced from the magnetic stray field measurements. Spatially resolved magnetic imaging requires the nitrogen-vacancy centers to be very close to the sample making the technique particularly interesting for thin tissue samples. This study is a proof of principle showing the capability of nitrogen-vacancy center magnetometry as a technique to detect magnetic nanoparticle distributions in Drosophila melanogaster larvae that can be extended to other biological systems.
Diamond has long been identified as a potential host material for laser applications. This potential arises due to its exceptional thermal properties, ultra-wide bandgap, and color centers which promise gain across the visible spectrum. More recently, coherent laser methods offer new approaches to magnetometry. However, diamond fabrication is difficult in comparison to other crystalline matrices, and many optical loss channels are not yet understood. Here, we demonstrate the first continuous-wave nitrogen-vacancy (NV) color center laser system. To achieve this, we constructed a laser cavity with both, an NV-diamond medium and an intra-cavity anti-reflection coated diode laser. This dual-medium approach compensates intrinsic losses of the cavity by providing a fixed additional gain below threshold of the diode laser. We observe the first clear continuous-wave laser threshold in the output of the laser system as well as linewidth narrowing with increasing green pump power on the NV centers. Our results are a major development towards coherent approaches to magnetometry.
The use of diamond colour centres such as the nitrogen-vacancy (NV) centre is increasingly enabling quantum sensing and computing applications. Novel concepts like cavity coupling and readout, laser-threshold magnetometry and multi-pass geometries allow significantly improved sensitivity and performance via increased signals and strong light fields. Enabling material properties for these techniques and their further improvements are low optical material losses via optical absorption of signal light and low birefringence. Here, we study systematically the behaviour of absorption around 700 nm and birefringence with increasing nitrogen- and NV-doping, as well as their behaviour during NV creation via diamond growth, electron beam irradiation and annealing treatments. Absorption correlates with increased nitrogen doping yet substitutional nitrogen does not seem to be the direct absorber. Birefringence reduces with increasing nitrogen doping. We identify multiple crystal defect concentrations via absorption spectroscopy and their changes during the material processing steps and thus identify potential causes of absorption and birefringence as well as strategies to fabricate chemical vapour deposition diamonds with high NV density yet low absorption and low birefringence. This article is part of the Theo Murphy meeting issue ‘Diamond for quantum applications’.
Negatively charged nitrogen-vacancy (NV) centers in diamond are promising magnetic field quantum sensors. Laser threshold magnetometry theory predicts improved NV center ensemble sensitivity via increased signal strength and magnetic field contrast. Here, we experimentally demonstrate laser threshold magnetometry. We use a macroscopic high-finesse laser cavity containing a highly NV-doped and low absorbing diamond gain medium that is pumped at 532 nm and resonantly seeded at 710 nm. This enables a 64% signal power amplification by stimulated emission. We test the magnetic field dependency of the amplification and thus demonstrate magnetic field-dependent stimulated emission from an NV center ensemble. This emission shows an ultrahigh contrast of 33% and a maximum output power in the milliwatt regime. The coherent readout of NV centers pave the way for novel cavity and laser applications of quantum defects and diamond NV magnetic field sensors with substantially improved sensitivity for the health, research, and mining sectors.
The nitrogen-vacancy (NV) center in diamond is a promising quantum system for magnetometry applications exhibiting optical readout of minute energy shifts in its spin sub-levels. Key material requirements for NV ensembles are a high NV − concentration, a long spin coherence time and a stable charge state. However, these are interdependent and can be difficult to optimize during diamond growth and subsequent NV creation. In this work, we systematically investigate the NV center formation and properties in bulk chemical vapor deposition (CVD) diamond. The nitrogen flow during growth is varied by over four orders of magnitude, resulting in a broad range of single substitutional nitrogen concentrations of 0.2–20 parts per million. For a fixed nitrogen concentration, we optimize electron-irradiation fluences with two different accelerated electron energies, and we study defect formation via optical characterizations. We discuss a general approach to determine the optimal irradiation conditions, for which an enhanced NV concentration and an optimum of NV charge states can both be satisfied. We achieve spin–spin coherence times T 2 ranging from 45.5 to 549 μ s for CVD diamonds containing 168 to 1 parts per billion NV − centers, respectively. This study shows a pathway to engineer properties of NV-doped CVD diamonds for improved sensitivity.
Single substitutional nitrogen atoms Ns0 are the prerequisite to create nitrogen-vacancy (NV) centers in diamonds. They not only serve as the electron donors to create the desired NV− center and provide charge stability against photo-ionisation but also are the main source of decoherence. Therefore, precise and quick determination of Ns0 concentration is a key advantage to a multitude of NV-related research in terms of material improvement as well as applications. Here, we present a method to determine the Ns0 concentration based on absorption spectroscopy in the UV-Visible range and fitting the 270 nm absorption band. UV-Visible spectroscopy has experimental simplicity and widespread availability that bear advantages over established methods. It allows a rapid determination of Ns0 densities, even for large numbers of samples. Our method shows further advantages in determining low concentrations as well as the ability to measure locally, which is highly relevant for diamonds with largely varying Ns0 concentrations in a single crystal. A cross-check with electron paramagnetic resonance shows high reliability of our method and yields the absorption cross section of the 270 nm absorption band σ=1.96±0.15 cm−1 ppm−1 (in common logarithm) or σe=4.51±0.35 cm−1 ppm−1 (in natural logarithm), which serves as a reference to determine Ns0 concentrations and makes our method applicable for others without the need for a known Ns0-reference sample and calibration. We provide a rapid, practical, and replicable pathway that is independent of the machine used and can be widely implemented as a standard characterization method for the determination of Ns0 concentrations.
Encapsulins, a prokaryotic class of self-assembling protein nanocompartments, are being re-engineered to serve as ‘nanoreactors’ for the augmentation or creation of key biochemical reactions. However, approaches that allow encapsulin nanoreactors to be functionally activated with spatial and temporal precision is lacking. We report the construction of a light-responsive encapsulin nanoreactor for “on-demand” production of reactive oxygen species (ROS). Herein, encapsulins were loaded with the fluorescent flavoprotein mini-Singlet Oxygen Generator (miniSOG), a biological photosensitizer that is activated by blue-light to generate ROS, primarily singlet oxygen ( 1 O 2 ). We established that the nanocompartments stably encased miniSOG, and in response to blue-light were able to mediate the photoconversion of molecular oxygen into ROS. Using an in vitro model of lung cancer, ROS generated by the nanoreactor was shown to trigger photosensitized oxidation reactions that exerted a toxic effect on tumour cells, suggesting utility in photodynamic therapy. This encapsulin nanoreactor thus represents a platform for the light-controlled initiation and/or modulation of ROS-driven processes in biomedicine and biotechnology.
We present a set of experiments in which the backscattering spectra of 4 μm single TiO2 particles are probed with circularly polarized vortex beams. The experiment is carried out with a tunable laser at λ = 760 - 810nm. We observe that the use of vortex beams enables us to tailor the backscattering in different ways. Given a certain backscattering of a particle (induced by a Gaussian beam or a plane wave), we observe that vortex beams can tune it and sharpen it. Moreover, we also observe that the level of conservation of helicty can be increased thanks to the use of vortex beams. We explain the mechanisms that give rise to these effects using Mie Theory. Our method of backscattering control can be experimentally implemented in most of microscopy set-ups. In addition, if brought to its limits, the method can be used to excite single multipolar modes from spheres. We believe that our method could find application in the levitation of particles or the excitation of whispering gallery modes.
Laser-threshold magetometry using the negatively charged nitrogen-vacancy (NV-) centre in diamond as a gain medium has been proposed as a technique to dramatically enhance the sensitivity of room-temperature magnetometry. We experimentally explore a diamond-loaded open tunable fibre-cavity system as a potential contender for the realization of lasing with NV- centres. We observe amplification of the transmission of a cavity-resonant seed laser at 721 nm when the cavity is pumped at 532 nm, and attribute this to stimulated emission. Changes in the intensity of spontaneously emitted photons accompany the amplification, and a qualitative model including stimulated emission and ionisation dynamics of the NV- centre captures the dynamics in the experiment very well. These results highlight important considerations in the realization of an NV- laser in diamond.
We study the engineering of quantum magnetic sensor using laser generated from diamond nitrogen-vacancy (NV) centres in fibre cavity. The projected sensitivity of such a sensor is of the order of pT / Hz $^{1/2}$.
Lens-axicon doublets have been used to produce Bessel-Gaussian beams, a narrow non-diffracting beam of relatively constant width. One problem of using Bessel-Gaussian beams is that there is a compromise between achieving a long effective focal length with a small central core radius and distributing the beam intensity between the central core and the off-axis rings. Here, we explore the advantage of tuning the lens-axicon separation, which allows us to have an additional degree of freedom to tailor the beam profile. Moreover, the separation between the lens and the axicon reduces the spherical aberrations in the beam profile, which can then be modeled within the paraxial regime. We study the detrimental effects of the spherical aberrations and provide several options to minimize them. We examine both sharp and shallow axicons used in combination with different converging lenses. We perform a series of detailed experiments to image the structure of the beam through the Bessel region. The spatial light distribution of the lens-axicon system is analyzed by using high dynamic range imaging and complemented with consistent theoretical calculations within the paraxial regime.
Over the past decade, exciton-polaritons in semiconductor microcavities have attracted a great deal of interest as driven-dissipative quantum fluids [1]. They offer themselves as a versatile platform for performing Hamiltonian simulations with light as well as for experimentally realizing nontrivial out-of-equilibrium phase transitions.
Summary form only given. Magnetic sensing with lasing from negatively charged nitorgen-vacancy (NV) centres in diamond is predicted to reach fT/√Hz regime even at room temperature [1]. Stimulated emission from NV centres has already been explored as a stepping stone towards such a laser magnetometer [2, 3, 4]. Here we report the observation of amplification on the cavity transmission of an open fibre cavity formed between a fibre-mirror and a macroscopic mirror, loaded with a high NV density diamond sample. On adding green laser light to optically pump the NV centres, we observe amplification on the transmitted seed wavelength close to 720 nm up to a factor around 3.
Measuring photon autocorrelations via a Hanbury-Brown and Twiss (HBT) setup is a widely used experimental technique in quantum optics and is the base for quantum characterizations via Hong-Ou-Mandel interferometry, Bell inequality tests or quantum state tomography. The most common use for HBT measurements is the demonstration of single-photon emission from a quantum emitter. In order to make a definite statement and analyze the coincidence histograms obtained in the experiment, the temporal position of the zero delay time (ZDT) must be accurately known. In many cases, determining the ZDT requires tedious calibration measurements using light sources with known non-trivial photon correlations. Here we report on a non-invasive technique for measuring the ZDT in HBT setups based on avalanche photodiodes (APDs). The technique relies on the deliberate enhancement of optical crosstalk between the APDs. It can be used with any conventional laser source and therefore means a significant improvement for the easy calibration of the ZDT in HBT setups. (C) 2019 Elsevier Ltd. All rights reserved.
Chiral resolution using non-functionalized mesoporous particles is demonstrated for a variety of enantiomeric pairs. This is achieved through the use of supramolecular templated silica materials prepared with guanosine monophosphate (NGM-1) and folic acid (NFM-1) which enable direct chiral transcription onto the surface of the mesopores after solvent extraction and post calcination of the template. The chiral selectivity and kinetics of the mesoporous materials are measured by circular dichroism (CD) spectroscopy on adsorbed molecules with different affinities for the pore surface. NGM-1 and NFM-1 have opposite enantiomeric selectivity for enantiomeric pairs. These results significantly increase the potential of mesoporous materials for chiral separation and enantiomeric catalysis.