Impact of Thickness-Dependent Nanophotonic Effects on the Optical Response of Color Centers in Hexagonal Boron Nitride.

Among a broad diversity of color centers hosted in layered van der Waals materials, the negatively charged boron vacancy (VB-) center in hexagonal boron nitride (hBN) is garnering considerable attention for the development of quantum sensing units on a two-dimensional platform. In this work, we investigate how the optical response of an ensemble of VB- centers evolves with the hBN thickness in a range of a few to hundreds of nanometers. We show that the photoluminescence intensity features a nontrivial evolution with thickness, which is quantitatively reproduced by numerical calculations taking into account thickness-dependent variations of the absorption, radiative lifetime, and radiation pattern of VB- centers. Besides providing an important resource to optimize the performances of quantum sensing units based on VB- centers in hBN, the thickness-dependent nanophotonic effects discussed in this work generally apply to any type of color center embedded in a van der Waals material.

Microwave Remote Sensing with Hybrid Quantum Receiver.

Detecting a microwave signal that is emitted or reflected by distant targets is a powerful tool in fundamental science and industrial technology. Solid-state spins provide an opportunity to realize quantum-enhanced remote sensing under ambient conditions. However, the weak interaction between the free-space signal and atomic size sensor limits the sensitivity. This hinders the realization of practical quantum remote sensing. Here, we demonstrate active microwave remote sensing with a diamond-based hybrid quantum receiver by combining electromagnetic field localization at nanoscale with quantum spin manipulation. A method of differential spin refocusing (DSR) is developed to overcome the challenge of reducing the impact of inhomogeneities in spin-signal interaction, while the strength of interaction is enhanced by more than 3 orders with nanostructure. It improves the coherent interaction time of quantum receiver by 30-fold, substantially enhancing the sensitivity and stability. By detecting the reflected microwave with picotesla sensitivity, diamond remote sensing monitors the real-time status of a centimeter-sized target at 2 m distance. Our method is general to various solid-state spins. The results will expand the applications of solid-state spin quantum sensors in areas ranging from medical imaging to resource survey.

Theoretical investigation of decoherence channels in athermal phonon sensors.

The creation and evolution of nonequilibrium phonons is central in applications ranging from cosmological particle searches to decoherence processes in qubits. However, the fundamental understanding of decoherence pathways for athermal phonon distributions in solid-state systems remains an open question. Using first-principles calculations, we investigate the primary decay channels of athermal phonons in two technologically relevant semiconductors - Si and GaAs. We quantify the contributions of anharmonic, isotopic, and interfacial scattering in these materials. From this, we construct a model to estimate the thermal power in a readout scheme as a function of time. We discuss the implication of our results on noise limitations in current phonon sensor designs and strategies for improving coherence in next-generation phonon sensors. .

Optical Tweezers Assembled Nanodiamond Quantum Sensors.

Here we show that gradient force optical tweezers can be used to mediate the self-assembly of nanodiamonds into superstructures, which can serve as optically trapped nanoscale quantum probes with superior magnetic resonance sensing capabilities. Enhanced fluorescence rates from nitrogen-vacancy NV- defect centers enable rapid acquisition of optically detected magnetic resonance (ODMR), and shape-induced forces can improve both positioning accuracy and orientation control. The use of confocal imaging can isolate the signal from individual nanodiamonds within the assembly, thereby retaining the desirable properties of a single crystal probe. The improvements afforded by the use nanodiamond assemblies has the potential to resolve dynamic changes through, for example, real-time monitoring of the ODMR contrast.

Charge and Spin Dynamics and Destabilization of Shallow Nitrogen-Vacancy Centers under UV and Blue Excitation.

Shallow nitrogen-vacancy (NV) centers in diamond offer opportunities to study photochemical reactions, including photogeneration of radical pairs, at the single-molecule regime. A prerequisite is a detailed understanding of charge and spin dynamics of NVs exposed to the short-wavelength light required to excite chemical species. Here, we investigate the charge and spin dynamics of shallow NVs under 445 and 375 nm illumination. With blue excitation, charge-state preparation is power-dependent, and modest spin initialization fidelity is observed. Under UV excitation, charge-state preparation is power-independent and no spin polarization is observed. Aging of NVs under prolonged UV exposure manifests in a reduced charge stability and spin contrast. We attribute this aging to modified local charge environments of near-surface NVs and identify distinct electronic traps only accessible at short wavelengths. Finally, we evaluate the prospects of NVs to probe photogenerated radical pairs based on measured sensitivities and outline possible sensing schemes.

Operando Decoding Ion-Conductive Switch in Stimuli-Responsive Hydrogel by Nanodiamond-Based Quantum Sensing.

Thermal-responsive hydrogels are developed as ion-conductive switchs for energy storage devices, however, the molecule mechanism of switch on/off remains unclear. Here, poly(N-isopropylacrylamide-co-acrylamide) hydrogel is synthesized as a model material and nanodiamond (ND) based quantum sensing for phase change study is developed. First, micro-scale phase separation with cross-linked mesh structure after sol-gel transition is visualized in situ and water molecules are trapped by polymer chains and on a chemically "frozen" state. Then, the nano-scale inhomogeneous distributions of viscosity, thermal conductivity and ionic mobility in hydrogel at high temperature are observed by measuring the rotation, translation and zero-field splitting of NDs. Besides, the ionic mobility of hydrogel is found to be dependent not only on temperature but also on polymer concentration. These observations suggested that the physical "wall" induced by inhomogeneous phase separation at microscopic scale blocked the ion conduction pathways, providing a potential intrinsic explanation for ion migration shut-down of ionic hydrogels at high temperature.

Recent Advances in Transparent Electrodes and Their Multimodal Sensing Applications.

This review examines the recent advancements in transparent electrodes and their crucial role in multimodal sensing technologies. Transparent electrodes, notable for their optical transparency and electrical conductivity, are revolutionizing sensors by enabling the simultaneous detection of diverse physical, chemical, and biological signals. Materials like graphene, carbon nanotubes, and conductive polymers, which offer a balance between optical transparency, electrical conductivity, and mechanical flexibility, are at the forefront of this development. These electrodes are integral in various applications, from healthcare to solar cell technologies, enhancing sensor performance in complex environments. The paper addresses challenges in applying these electrodes, such as the need for mechanical flexibility, high optoelectronic performance, and biocompatibility. It explores new materials and innovative techniques to overcome these hurdles, aiming to broaden the capabilities of multimodal sensing devices. The review provides a comparative analysis of different transparent electrode materials, discussing their applications and the ongoing development of novel electrode systems for multimodal sensing. This exploration offers insights into future advancements in transparent electrodes, highlighting their transformative potential in bioelectronics and multimodal sensing technologies.

Quantum illumination and quantum radar: a brief overview.

Quantum illumination (QI) and quantum radar have emerged as potentially groundbreaking technologies, leveraging the principles of quantum mechanics to revolutionise the field of remote sensing and target detection. The protocol, particularly in the context of quantum radar, has been subject to a great deal of aspirational conjecture as well as criticism with respect to its realistic potential. In this review, we present a broad overview of the field of quantum target detection focusing on QI and its potential as an underlying scheme for a quantum radar operating at microwave frequencies. We provide context for the field by considering its historical development and fundamental principles. Our aim is to provide a balanced discussion on the state of theoretical and experimental progress towards realising a working QI-based quantum radar, and draw conclusions about its current outlook and future directions.

Spatially Resolved Quantum Sensing with High-Density Bubble-Printed Nanodiamonds.

Nitrogen-vacancy (NV-) centers in nanodiamonds have emerged as a versatile platform for a wide range of applications, including bioimaging, photonics, and quantum sensing. However, the widespread adoption of nanodiamonds in practical applications has been hindered by the challenges associated with patterning them into high-resolution features with sufficient throughput. In this work, we overcome these limitations by introducing a direct laser-writing bubble printing technique that enables the precise fabrication of two-dimensional nanodiamond patterns. The printed nanodiamonds exhibit a high packing density and strong photoluminescence emission, as well as robust optically detected magnetic resonance (ODMR) signals. We further harness the spatially resolved ODMR of the nanodiamond patterns to demonstrate the mapping of two-dimensional temperature gradients using high frame rate widefield lock-in fluorescence imaging. This capability paves the way for integrating nanodiamond-based quantum sensors into practical devices and systems, opening new possibilities for applications involving high-resolution thermal imaging and biosensing.

Microcontroller-Optimized Measurement Electronics for Coherent Control Applications of NV Centers.

Long coherence times at room temperature make the NV center a promising candidate for quantum sensors and quantum computers. The necessary coherent control of the electron spin triplet in the ground state requires microwave π pulses in the nanosecond range, obtained from the Rabi oscillation of the mS spin states of the magnetic resonances of the NV centers. Laboratory equipment has a high temporal resolution for these measurements but is expensive and, therefore, uninteresting for fields such as education. In this work, we present measurement electronics for NV centers that are optimized for microcontrollers. It is shown that the Rabi frequency is linear to the output of the digital-to-analog converter (DAC) and is used to adapt the time length π of the electron spin flip, to the limited pulse width resolution of the microcontroller. This was achieved by breaking down the most relevant functions of conventional laboratory devices and replacing them with commercially available integrated components. The result is a cost-effective handheld setup for coherent control applications of NV centers.

Low frequency signal detection via correlated Ramsey measurements.

The low frequency region of the spectrum is a challenging regime for quantum probes. We support the idea that, in this regime, performing Ramsey measurements carefully controlling the time at which each measurement is initiated is an excellent signal detection strategy. We use the Fisher information to demonstrate a high quality performance in the low frequency regime, compared to more elaborated measurement sequences, and to optimize the correlated Ramsey sequence according to any given experimental parameters, showing that correlated Ramsey rivals with state-of-the-art protocols, and can even outperform commonly employed sequences such as dynamical decoupling in the detection of low frequency signals. Contrary to typical quantum detection protocols for oscillating signals, which require adjusting the time separation between pulses to match the half period of the target signal, and consequently see their scope limited to signals whose period is shorter than the characteristic decoherence time of the probe, or to those protocols whose target is primarily static signals, the time-tagged correlated Ramsey sequence simultaneously tracks the amplitude and the phase information of the target signal, regardless of its frequency, which crucially permits correlating measurements in post-processing, leading to efficient spectral reconstruction.

Sensing at the Nanoscale Using Nitrogen-Vacancy Centers in Diamond: A Model for a Quantum Pressure Sensor.

The sensing of stress under harsh environmental conditions with high resolution has critical importance for a range of applications including earth's subsurface scanning, geological CO2 storage monitoring, and mineral and resource recovery. Using a first-principles density functional theory (DFT) approach combined with the theoretical modelling of the low-energy Hamiltonian, here, we investigate a novel approach to detect unprecedented levels of pressure by taking advantage of the solid-state electronic spin of nitrogen-vacancy (NV) centers in diamond. We computationally explore the effect of strain on the defect band edges and band gaps by varying the lattice parameters of a diamond supercell hosting a single NV center. A low-energy Hamiltonian is developed that includes the effect of stress on the energy level of a ±1 spin manifold at the ground state. By quantifying the energy level shift and split, we predict pressure sensing of up to 0.3 MPa/Hz using the experimentally measured spin dephasing time. We show the superiority of the quantum sensing approach over traditional optical sensing techniques by discussing our results from DFT and theoretical modelling for the frequency shift per unit pressure. Importantly, we propose a quantum manometer that could be useful to measure earth's subsurface vibrations as well as for pressure detection and monitoring in high-temperature superconductivity studies and in material sciences. Our results open avenues for the development of a sensing technology with high sensitivity and resolution under extreme pressure limits that potentially has a wider applicability than the existing pressure sensing technologies.

Observation of magnetic amplification using dark spins.

Quantum amplification enables the enhancement of weak signals and is of great importance for precision measurements, such as biomedical science and tests of fundamental symmetries. Here, we observe a previously unexplored magnetic amplification using dark noble-gas nuclear spins in the absence of pump light. Such dark spins exhibit remarkable coherence lasting up to 6 min and the resilience against the perturbations caused by overlapping alkali-metal gas. We demonstrate that the observed phenomenon, referred to as "dark spin amplification," significantly magnifies magnetic field signals by at least three orders of magnitude. As an immediate application, we showcase an ultrasensitive magnetometer capable of measuring subfemtotesla fields in a single 500-s measurement. Our approach is generic and can be applied to a wide range of noble-gas isotopes, and we discuss promising optimizations that could further improve the current signal amplification up to [Formula: see text] with [Formula: see text]Ne, [Formula: see text] with [Formula: see text]Xe, and [Formula: see text] with [Formula: see text]He. This work unlocks opportunities in precision measurements, including searches for ultralight dark matter with sensitivity well beyond the supernova-observation constraints.

Room Temperature Relaxometry of Single Nitrogen Vacancy Centers in Proximity to α-RuCl3 Nanoflakes.

Nitrogen vacancy (NV) center-based magnetometry has been proven to be a versatile sensor for various classes of magnetic materials in broad temperature and frequency ranges. Here, we use the longitudinal relaxation time T1 of single NV centers to investigate the spin dynamics of nanometer-thin flakes of α-RuCl3 at room temperature. We observe a significant reduction in the T1 in the presence of α-RuCl3 in the proximity of NVs, which we attribute to paramagnetic spin noise confined in the 2D hexagonal planes. Furthermore, the T1 time exhibits a monotonic increase with an applied magnetic field. We associate this trend with the alteration of the spin and charge noise in α-RuCl3 under an external magnetic field. These findings suggest that the influence of the spin dynamics of α-RuCl3 on the T1 of the NV center can be used to gain information about the material itself and the technique to be used on other 2D materials.

High Spatial Resolution 2D Imaging of Current Density and Pressure for Graphene Devices under High Pressure Using Nitrogen-Vacancy Centers in Diamond.

Current density imaging is helpful for discovering interesting electronic phenomena and understanding carrier dynamics, and by combining pressure distributions, several pressure-induced novel physics may be comprehended. In this work, noninvasive, high-resolution two-dimensional images of the current density and pressure gradient for graphene ribbon and hBN-graphene-hBN devices are explored using nitrogen-vacancy (NV) centers in diamond under high pressure. The two-dimensional vector current density is reconstructed by the vector magnetic field mapped by the near-surface NV center layer in the diamond. The current density images accurately and clearly reproduce the complicated structure and current flow of graphene under high pressure. Additionally, the spatial distribution of the pressure is simultaneously mapped, rationalizing the nonuniformity of the current density under high pressure. The current method opens a significant new avenue to investigate electronic transport and conductance variations in two-dimensional materials and electrical devices under high pressure as well as for nondestructive evaluation of semiconductor circuits.

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.

Quantum Mimicry With Inorganic Chemistry.

Quantum objects, such as atoms, spins, and subatomic particles, have important properties due to their unique physical properties that could be useful for many different applications, ranging from quantum information processing to magnetic resonance imaging. Molecular species also exhibit quantum properties, and these properties are fundamentally tunable by synthetic design, unlike ions isolated in a quadrupolar trap, for example. In this comment, we collect multiple, distinct, scientific efforts into an emergent field that is devoted to designing molecules that mimic the quantum properties of objects like trapped atoms or defects in solids. Mimicry is endemic in inorganic chemistry and featured heavily in the research interests of groups across the world. We describe a new field of using inorganic chemistry to design molecules that mimic the quantum properties (e.g. the lifetime of spin superpositions, or the resonant frequencies thereof) of other quantum objects, "quantum mimicry." In this comment, we describe the philosophical design strategies and recent exciting results from application of these strategies.

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 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 narrower optical point-spread function and the shallow depth of NV centers. We analyze the magnetic nanoparticle images and sensitivity as a function of the microscope's spatial resolution and show that the signal-to-noise ratio for nanoparticle detection does not degrade as the spatial resolution improves. We 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 <10 mW laser power and can be parallelized by patterned illumination, introduces a promising format for nanoscale magnetic imaging.

Quantum Sensing of Free Radical Generation in Mitochondria of Single Heart Muscle Cells during Hypoxia and Reoxygenation.

Cells are damaged during hypoxia (blood supply deprivation) and reoxygenation (oxygen return). This damage occurs in conditions such as cardiovascular diseases, cancer, and organ transplantation, potentially harming the tissue and organs. The role of free radicals in cellular metabolic reprogramming under hypoxia is under debate, but their measurement is challenging due to their short lifespan and limited diffusion range. In this study, we employed a quantum sensing technique to measure the real-time production of free radicals at the subcellular level. We utilize fluorescent nanodiamonds (FNDs) that exhibit changes in their optical properties based on the surrounding magnetic noise. This way, we were able to detect the presence of free radicals. To specifically monitor radical generation near mitochondria, we coated the FNDs with an antibody targeting voltage-dependent anion channel 2 (anti-VDAC2), which is located in the outer membrane of mitochondria. We observed a significant increase in the radical load on the mitochondrial membrane when cells were exposed to hypoxia. Subsequently, during reoxygenation, the levels of radicals gradually decreased back to the normoxia state. Overall, by applying a quantum sensing technique, the connections among hypoxia, free radicals, and the cellular redox status has been revealed.

Scanning Spin Probe Based on Magnonic Vortex Quantum Cavities.

Performing nanoscale scanning electron paramagnetic resonance (EPR) requires three essential ingredients: First, a static magnetic field together with field gradients to Zeeman split the electronic energy levels with spatial resolution; second, a radio frequency (rf) magnetic field capable of inducing spin transitions; finally, a sensitive detection method to quantify the energy absorbed by spins. This is usually achieved by combining externally applied magnetic fields with inductive coils or cavities, fluorescent defects, or scanning probes. Here, we theoretically propose the realization of an EPR scanning sensor merging all three characteristics into a single device: the vortex core stabilized in ferromagnetic thin-film discs. On one hand, the vortex ground state generates a significant static magnetic field and field gradients. On the other hand, the precessional motion of the vortex core around its equilibrium position produces a circularly polarized oscillating magnetic field, which is enough to produce spin transitions. Finally, the spin-magnon coupling broadens the vortex gyrotropic frequency, suggesting a direct measure of the presence of unpaired electrons. Moreover, the vortex core can be displaced by simply using external magnetic fields of a few mT, enabling EPR scanning microscopy with large spatial resolution. Our numerical simulations show that, by using low damping magnets, it is theoretically possible to detect single spins located on the disc's surface. Vortex nanocavities could also attain strong coupling to individual spin molecular qubits with potential applications to mediate qubit-qubit interactions or to implement qubit readout protocols.