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The reconstruction of electrical current densities from magnetic field measurements is an important technique with applications in materials science, circuit design, quality control, plasma physics, and biology. Analytic reconstruction methods exist for planar currents, but break down in the presence of high spatial frequency noise or large standoff distance, restricting the types of systems that can be studied. Here, we demonstrate the use of a deep convolutional neural network for current density reconstruction from two-dimensional (2D) images of vector magnetic fields acquired by a quantum diamond microscope (QDM) utilizing a surface layer of Nitrogen Vacancy (NV) centers in diamond. Trained network performance significantly exceeds analytic reconstruction for data with high noise or large standoff distances. This machine learning technique can perform quality inversions on lower SNR data, reducing the data collection time by a factor of about 400 and permitting reconstructions of weaker and three-dimensional current sources.

The quantum diamond microscope (QDM) is a recently developed technology for near-field imaging of magnetic fields with micron-scale spatial resolution. In the present work, we integrate a QDM with a narrowband measurement protocol and a lock-in camera; and demonstrate imaging of radiofrequency (RF) magnetic field patterns produced by microcoils, with spectral resolution $\approx1$\u2009Hz. This RF-QDM provides multi-frequency imaging with a central detection frequency that is easily tunable over the MHz-scale, allowing spatial discrimination of both crowded spectral peaks and spectrally well-separated signals. The present instrument has spatial resolution $\approx2\,\mathrm{\mu m}$, field-of-view $\approx300\times300\,\mathrm{\mu m^2}$, and per-pixel sensitivity to narrowband fields $\sim{1}\,$nT$\cdot$Hz$^{-1/2}$. Spatial noise can be reduced to the picotesla scale by signal averaging and/or spatial binning. The RF-QDM enables simultaneous imaging of the amplitude, frequency, and phase of narrowband magnetic field patterns at the micron-scale, with potential applications in real-space NMR imaging, AC susceptibility mapping, impedance tomography, analysis of electronic circuits, and spatial eddy-current-based inspection.

The second "Mineral Detection of Neutrinos and Dark Matter" (MDvDM'24) meeting was held January 8-11, 2024 in Arlington, VA, USA, hosted by Virginia Tech's Center for Neutrino Physics. This document collects contributions from this workshop, providing an overview of activities in the field. MDvDM'24 was the second topical workshop dedicated to the emerging field of mineral detection of neutrinos and dark matter, following a meeting hosted by IFPU in Trieste, Italy in October 2022. Mineral detectors have been proposed for a wide variety of applications, including searching for dark matter, measuring various fluxes of astrophysical neutrinos over gigayear timescales, monitoring nuclear reactors, and nuclear disarmament protocols; both as paleo-detectors using natural minerals that could have recorded the traces of nuclear recoils for timescales as long as a billion years and as detectors recording nuclear recoil events on laboratory timescales using natural or artificial minerals. Contributions to this proceedings discuss the vast physics potential, the progress in experimental studies, and the numerous challenges lying ahead on the path towards mineral detection. These include a better understanding of the formation and annealing of recoil defects in crystals; identifying the best classes of minerals and, for paleo-detectors, understanding their geology; modeling and control of the relevant backgrounds; developing, combining, and scaling up imaging and data analysis techniques; and many others. During the last years, MDvDM has grown rapidly and gained attention. Small-scale experimental efforts focused on establishing various microscopic readout techniques are underway at institutions in North America, Europe and Asia. We are looking ahead to an exciting future full of challenges to overcome, surprises to be encountered, and discoveries lying ahead of us.

Nitrogen-vacancy (NV) centers in diamond are a leading modality for magnetic sensing and imaging under ambient conditions. However, these sensors suffer from degraded performance due to paramagnetic impurities and regions of stress in the diamond crystal lattice. This work demonstrates a quantum diamond microscope (QDM) for simultaneous mapping and spatial correlation of key properties of a millimeter-scale NV-diamond sensor chip, including: NV ensemble photoluminescence (PL) amplitude, spin-lattice relaxation time (T$_1$), and homogeneous and inhomogeneous spin coherence lifetimes (T$_2$ and T$_2^*$), as well as lattice stress/strain, birefringence magnitude, and birefringence angle of the diamond crystal.

The nitrogen vacancy (NV) center in diamond is an increasingly popular quantum sensor for microscopy of electrical current, magnetization, and spins. However, efficient NV-sample integration with a robust, high-quality interface remains an outstanding challenge to realize scalable, high-throughput microscopy. In this work, we characterize a diamond micro-chip (DMC) containing a (111)-oriented NV ensemble; and demonstrate its utility for high-resolution quantum microscopy. We perform strain imaging of the DMC and find minimal detrimental strain variation across a field-of-view of tens of micrometer. We find good ensemble NV spin coherence and optical properties in the DMC, suitable for sensitive magnetometry. We then use the DMC to demonstrate wide-field microscopy of electrical current, and show that diffraction-limited quantum microscopy can be achieved. We also demonstrate the deterministic transfer of DMCs with multiple materials of interest for next-generation electronics and spintronics. Lastly, we develop a polymer-based technique for DMC placement. This work establishes the DMC's potential to expand the application of NV quantum microscopy in materials, device, geological, biomedical, and chemical sciences.

The field of nanoscale magnetic resonance imaging (NanoMRI) was started 30 years ago. It was motivated by the desire to image single molecules and molecular assemblies, such as proteins and virus particles, with near-atomic spatial resolution and on a length scale of 100 nm. Over the years, the NanoMRI field has also expanded to include the goal of useful high-resolution nuclear magnetic resonance (NMR) spectroscopy of molecules under ambient conditions, including samples up to the micron-scale. The realization of these goals requires the development of spin detection techniques that are many orders of magnitude more sensitive than conventional NMR and MRI, capable of detecting and controlling nanoscale ensembles of spins. Over the years, a number of different technical approaches to NanoMRI have emerged, each possessing a distinct set of capabilities for basic and applied areas of science. The goal of this roadmap article is to report the current state of the art in NanoMRI technologies, outline the areas where they are poised to have impact, identify the challenges that lie ahead, and propose methods to meet these challenges. This roadmap also shows how developments in NanoMRI techniques can lead to breakthroughs in emerging quantum science and technology applications.

Nitrogen vacancy (NV) centers in diamond enable nuclear magnetic resonance (NMR) spectroscopy of samples at the nano- and micron scales. However, at typical tesla-scale NMR magnetic field strengths, NV-NMR protocols become difficult to implement due to the challenge of driving fast NV pulse sequences sensitive to nuclear Larmor frequencies above a few megahertz. We perform simulations and theoretical analysis of the experimental viability of NV-NMR at tesla-scale magnetic fields using a new measurement protocol called DRACAERIS (Double Rewound ACquisition Amplitude Encoded Radio Induced Signal). DRACAERIS detects the NMR sample's longitudinal magnetization at a much lower driven Rabi frequency, more suitable technically for NV detection. We discuss how pulse errors, finite pulse lengths, and nuclear spin-spin couplings affect the resulting NMR spectra. We find that DRACAERIS is less susceptible to pulse imperfections and off-resonance effects than previous protocols for longitudinal magnetization detection. We also identify reasonable parameters for experimental implementation.

This paper presents a method for hardware trojan detection in integrated circuits. Unsupervised deep learning is used to classify wide field-of-view (4x4 mm$^2$), high spatial resolution magnetic field images taken using a Quantum Diamond Microscope (QDM). QDM magnetic imaging is enhanced using quantum control techniques and improved diamond material to increase magnetic field sensitivity by a factor of 4 and measurement speed by a factor of 16 over previous demonstrations. These upgrades facilitate the first demonstration of QDM magnetic field measurement for hardware trojan detection. Unsupervised convolutional neural networks and clustering are used to infer trojan presence from unlabeled data sets of 600x600 pixel magnetic field images without human bias. This analysis is shown to be more accurate than principal component analysis for distinguishing between field programmable gate arrays configured with trojan free and trojan inserted logic. This framework is tested on a set of scalable trojans that we developed and measured with the QDM. Scalable and TrustHub trojans are detectable down to a minimum trojan trigger size of 0.5% of the total logic. The trojan detection framework can be used for golden-chip free detection, since knowledge of the chips' identities is only used to evaluate detection accuracy

Next-generation dark matter (DM) detectors searching for weakly interacting massive particles (WIMPs) will be sensitive to coherent scattering from solar neutrinos, demanding an efficient background-signal discrimination tool. Directional detectors improve sensitivity to WIMP DM despite the irreducible neutrino background. Wide-bandgap semiconductors offer a path to directional detection in a high-density target material. A detector of this type operates in a hybrid mode. The WIMP or neutrino-induced nuclear recoil is detected using real-time charge, phonon, or photon collection. The directional signal, however, is imprinted as a durable sub-micron damage track in the lattice structure. This directional signal can be read out by a variety of atomic physics techniques, from point defect quantum sensing to x-ray microscopy. In this white paper, we present the detector principle and review the status of the experimental techniques required for directional readout of nuclear recoil tracks. Specifically, we focus on diamond as a target material; it is both a leading platform for emerging quantum technologies and a promising component of next-generation semiconductor electronics. Based on the development and demonstration of directional readout in diamond over the next decade, a future WIMP detector will leverage or motivate advances in multiple disciplines towards precision dark matter and neutrino physics.

The adoption of 3D packaging technology necessitates the development of new approaches to failure electronic device analysis. To that end, our team is developing a tool called the quantum diamond microscope (QDM) that leverages an ensemble of nitrogen vacancy (NV) centers in diamond, achieving vector magnetic imaging with a wide field-of-view and high spatial resolution under ambient conditions. Here, we present the QDM measurement of 2D current distributions in an 8-nm flip chip IC and 3D current distributions in a multi-layer PCB. Magnetic field emanations from the C4 bumps in the flip chip dominate the QDM measurements, but these prove to be useful for image registration and can be subtracted to resolve adjacent current traces in the die at the micron scale. Vias in 3D ICs display only Bx and By magnetic fields due to their vertical orientation and are difficult to detect with magnetometers that only measure the Bz component (orthogonal to the IC surface). Using the multi-layer PCB, we show that the QDM's ability to simultaneously measure Bx, By, and Bz is advantageous for resolving magnetic fields from vias as current passes between layers. We also show how spacing between conducting layers is determined by magnetic field images and how it agrees with the design specifications of the PCB. In our initial efforts to provide further z-depth information for current sources in complex 3D circuits, we show how magnetic field images of individual layers can be subtracted from the magnetic field image of the total structure. This allows for isolation of signal layers and can be used to map embedded current paths via solution of the 2D magnetic inverse. In addition, the paper also discusses the use of neural networks to identify 2D current distributions and its potential for analyzing 3D structures.

$^{31}$P NMR and MRI are commonly used to study organophosphates that are central to cellular energy metabolism. In some molecules of interest, such as adenosine diphosphate (ADP) and nicotinamide adenine dinucleotide (NAD), pairs of coupled $^{31}$P nuclei in the diphosphate moiety should enable the creation of nuclear spin singlet states, which may be long-lived and can be selectively detected via quantum filters. Here, we show that $^{31}$P singlet states can be created on ADP and NAD, but their lifetimes are shorter than T$_{1}$ and are strongly sensitive to pH. Nevertheless, the singlet states were used with a quantum filter to successfully isolate the $^{31}$P NMR spectra of those molecules from the adenosine triphosphate (ATP) background signal.

Crystal strain variation imposes significant limitations on many quantum sensing and information applications for solid-state defect qubits in diamond. Thus, precision measurement and control of diamond crystal strain is a key challenge. Here, we report diamond strain measurements with a unique set of capabilities, including micron-scale spatial resolution, millimeter-scale field-of-view, and a two order-of-magnitude improvement in volume-normalized sensitivity over previous work [1], reaching $5(2) \times 10^{-8}/\sqrt{\rm{Hz}\cdot\rm{\mu m}^3}$ (with spin-strain coupling coefficients representing the dominant systematic uncertainty). We use strain-sensitive spin-state interferometry on ensembles of nitrogen vacancy (NV) color centers in single-crystal CVD bulk diamond with low strain gradients. This quantum interferometry technique provides insensitivity to magnetic-field inhomogeneity from the electronic and nuclear spin bath, thereby enabling long NV ensemble electronic spin dephasing times and enhanced strain sensitivity. We demonstrate the strain-sensitive measurement protocol first on a scanning confocal laser microscope, providing quantitative measurement of sensitivity as well as three-dimensional strain mapping; and second on a wide-field imaging quantum diamond microscope (QDM). Our strain microscopy technique enables fast, sensitive characterization for diamond material engineering and nanofabrication; as well as diamond-based sensing of strains applied externally, as in diamond anvil cells or embedded diamond stress sensors, or internally, as by crystal damage due to particle-induced nuclear recoils.

Understanding nano- and micro-scale crystal strain in CVD diamond is crucial to the advancement of diamond quantum technologies. In particular, the presence of such strain and its characterization present a challenge to diamond-based quantum sensing and information applications -- as well as for future dark matter detectors where directional information of incoming particles is encoded in crystal strain. Here, we exploit nanofocused scanning X-ray diffraction microscopy to quantitatively measure crystal deformation from defects in diamond with high spatial and strain resolution. Combining information from multiple Bragg angles allows stereoscopic three-dimensional modeling of strain feature geometry; the diffraction results are validated via comparison to optical measurements of the strain tensor based on spin-state-dependent spectroscopy of ensembles of nitrogen vacancy (NV) centers in the diamond. Our results demonstrate both strain and spatial resolution sufficient for directional detection of dark matter via X-ray measurement of crystal strain, and provide a promising tool for diamond growth analysis and improvement of defect-based sensing.

A subset of QuantISED Sensor PIs met virtually on May 26, 2020 to discuss a response to a charge by the DOE Office of High Energy Physics. In this document, we summarize the QuantISED sensor community discussion, including a consideration of HEP science enabled by quantum sensors, describing the distinction between Quantum 1.0 and Quantum 2.0, and discussing synergies/complementarity with the new DOE NQI centers and with research supported by other SC offices. Quantum 2.0 advances in sensor technology offer many opportunities and new approaches for HEP experiments. The DOE HEP QuantISED program could support a portfolio of small experiments based on these advances. QuantISED experiments could use sensor technologies that exemplify Quantum 2.0 breakthroughs. They would strive to achieve new HEP science results, while possibly spinning off other domain science applications or serving as pathfinders for future HEP science targets. QuantISED experiments should be led by a DOE laboratory, to take advantage of laboratory technical resources, infrastructure, and expertise in the safe and efficient construction, operation, and review of experiments. The QuantISED PIs emphasized that the quest for HEP science results under the QuantISED program is distinct from the ongoing DOE HEP programs on the energy, intensity, and cosmic frontiers. There is robust evidence for the existence of particles and phenomena beyond the Standard Model, including dark matter, dark energy, quantum gravity, and new physics responsible for neutrino masses, cosmic inflation, and the cosmic preference for matter over antimatter. Where is this physics and how do we find it? The QuantISED program can exploit new capabilities provided by quantum technology to probe these kinds of science questions in new ways and over a broader range of science parameters than can be achieved with conventional techniques.

We introduce a double quantum (DQ) 4-Ramsey measurement protocol that enables wide-field magnetic imaging using nitrogen vacancy (NV) centers in diamond, with enhanced homogeneity of the magnetic sensitivity relative to conventional single quantum (SQ) techniques. The DQ 4-Ramsey protocol employs microwave-phase alternation across four consecutive Ramsey (4-Ramsey) measurements to isolate the desired DQ magnetic signal from any residual SQ signal induced by microwave pulse errors. In a demonstration experiment employing a 1-$\mu$m-thick NV layer in a macroscopic diamond chip, the DQ 4-Ramsey protocol provides volume-normalized DC magnetic sensitivity of $\eta^\text{V}=34\,$nTHz$^{-1/2} \mu$m$^{3/2}$ across a $125\,\mu$m$ \,\times\,125\,\mu $m field of view, with about 5$\times$ less spatial variation in sensitivity across the field of view compared to a SQ measurement. The improved robustness and magnetic sensitivity homogeneity of the DQ 4-Ramsey protocol enable imaging of dynamic, broadband magnetic sources such as integrated circuits and electrically-active cells.

Optically-probed nitrogen-vacancy (NV) quantum defects in diamond can detect nuclear magnetic resonance (NMR) signals with high-spectral resolution from micron-scale sample volumes of about 10 picoliters. However, a key challenge for NV-NMR is detecting samples at millimolar concentrations. Here, we demonstrate an improvement in NV-NMR proton concentration sensitivity of about $10^5$ over thermal polarization by hyperpolarizing sample proton spins through signal amplification by reversible exchange (SABRE), enabling micron-scale NMR of small molecule sample concentrations as low as 1 millimolar in picoliter volumes. The SABRE-enhanced NV-NMR technique may enable detection and chemical analysis of low concentration molecules and their dynamics in complex micron-scale systems such as single-cells.

We provide an overview of the experimental techniques, measurement modalities, and diverse applications of the Quantum Diamond Microscope (QDM). The QDM employs a dense layer of fluorescent nitrogen-vacancy (NV) color centers near the surface of a transparent diamond chip on which a sample of interest is placed. NV electronic spins are coherently probed with microwaves and optically initialized and read out to provide spatially resolved maps of local magnetic fields. NV fluorescence is measured simultaneously across the diamond surface, resulting in a wide-field, two-dimensional magnetic field image with adjustable spatial pixel size set by the parameters of the imaging system. NV measurement protocols are tailored for imaging of broadband and narrowband fields, from DC to GHz frequencies. Here we summarize the physical principles common to diverse implementations of the QDM and review example applications of the technology in geoscience, biology, and materials science.

We present a micrometer-resolution millimeter-field-of-view stress imaging method for diamonds containing a thin surface layer of nitrogen vacancy (NV) centers. In this method, we reconstruct stress tensor elements over a two-dimensional field of view from NV optically-detected magnetic resonance (ODMR) spectra. We use this technique to study how stress inhomogeneity affects NV magnetometry performance, and show how NV stress imaging is a useful and direct way to assess these effects. This new tool for mapping stress in diamond will aid optimization of NV-diamond sensing, with wide-ranging applications in the physical and life sciences.

Nitrogen-vacancy (NV) quantum defects in diamond are sensitive detectors of magnetic fields. Due to their atomic size and optical readout capability, they have been used for magnetic resonance spectroscopy of nanoscale samples on diamond surfaces. Here we present a protocol for fabricating NV-diamond chips and for constructing and operating a simple, low-cost quantum diamond spectrometer for performing nuclear magnetic resonance (NMR) and electron spin resonance (ESR) spectroscopy in nanoscale volumes. The instrument is based on a commercially-available diamond chip, with an ion-implanted NV-ensemble at a depth of ~ 10 nm below the diamond surface. The spectrometer operates at low magnetic fields (~ 300 G) and requires standard optical and microwave components for NV spin preparation, manipulation and readout. We demonstrate the utility of this device for nanoscale proton and fluorine NMR spectroscopy, as well as for the detection of transition metals via ESR noise spectroscopy. We estimate that the full protocol requires 2-3 months to implement, depending on the availability of equipment, diamond substrates, and user experience.

Nuclear magnetic resonance (NMR) spectroscopy is a widely used tool for chemical analysis and molecular structure identification. Because it typically relies on the weak magnetic fields produced by a small thermal nuclear spin polarization, NMR suffers from poor molecule-number sensitivity compared to other analytical techniques. Recently, a new class of NMR sensors based on optically-probed nitrogen-vacancy (NV) quantum defects in diamond have allowed molecular spectroscopy from sample volumes several orders of magnitude smaller than the most sensitive inductive detectors. To date, however, NV-NMR spectrometers have only been able to observe signals from pure, highly concentrated samples. To overcome this limitation, we introduce a technique that combines picoliter-scale NV-NMR with fully integrated Overhauser dynamic nuclear polarization (DNP) to perform high-resolution spectroscopy on a variety of small molecules in dilute solution, with femtomole sensitivity. Our technique advances mass-limited NMR spectroscopy for drug and natural product discovery, catalysis research, and single cell studies.

We demonstrate a broad, flat, visible supercontinuum spectrum that is generated by a dispersion-engineered tapered photonic crystal fiber pumped by a 1 GHz repetition rate turn-key Ti:sapphire laser outputting $\sim$ 30 fs pulses at 800 nm. At a pulse energy of 100 pJ, we obtain an output spectrum that is flat to within 3 dB over the range 490-690 nm with a blue tail extending below 450 nm. The mode-locked laser combined with the photonic crystal fiber forms a simple visible frequency comb system that is extremely well-suited to the precise calibration of astrophysical spectrographs, among other applications.

We demonstrate a vector magnetometer that simultaneously measures all Cartesian components of a dynamic magnetic field using an ensemble of nitrogen-vacancy (NV) centers in a single-crystal diamond. Optical NV-diamond measurements provide high-sensitivity, broadband magnetometry under ambient or extreme physical conditions; and the fixed crystallographic axes inherent to this solid-state system enable vector sensing free from heading errors. In the present device, multi-channel lock-in detection extracts the magnetic-field-dependent spin resonance shifts of NVs oriented along all four tetrahedral diamond axes from the optical signal measured on a single detector. The sensor operates from near DC up to a $12.5$ kHz measurement bandwidth; and simultaneously achieves $\sim\!50$ pT/$\sqrt{\text{Hz}}$ magnetic field sensitivity for each Cartesian component, which is to date the highest demonstrated sensitivity of a full vector magnetometer employing solid-state spins. Compared to optimized devices interrogating the four NV orientations sequentially, the simultaneous vector magnetometer enables a $4\times$ measurement speedup. This technique can be extended to pulsed-type sensing protocols and parallel wide-field magnetic imaging.

Point source localization is a problem of persistent interest in optical imaging. In particular, a number of widely used biological microscopy techniques rely on precise three-dimensional localization of single fluorophores. As emitter depth localization is more challenging than lateral localization, considerable effort has been spent on engineering the response of the microscope in a way that reveals increased depth information. Here we consider the theoretical limits of such approaches by deriving the quantum Cramér-Rao bound (QCRB). We show that existing methods for depth localization with single-objective detection exceed the QCRB by a factor $>\sqrt{2}$, and propose an interferometer arrangement that approaches the bound. We also show that for detection with two opposed objectives, established interferometric measurement techniques globally reach the QCRB.

The practical implementation of many quantum technologies relies on the development of robust and bright single photon sources that operate at room temperature. The negatively charged silicon-vacancy (SiV-) color center in diamond is a possible candidate for such a single photon source. However, due to the high refraction index mismatch to air, color centers in diamond typically exhibit low photon out-coupling. An additional shortcoming is due to the random localization of native defects in the diamond sample. Here we demonstrate deterministic implantation of Si ions with high conversion efficiency to single SiV- centers, targeted to fabricated nanowires. The co-localization of single SiV- centers with the nanostructures yields a ten times higher light coupling efficiency than for single SiV- centers in bulk diamond. This enhanced photon out-coupling, together with the intrinsic scalability of the SiV- creation method, enables a new class of devices for integrated photonics and quantum science.

Diamond-based magnetic field sensors have attracted great interest in recent years. In particular, wide-field magnetic imaging using nitrogen-vacancy (NV) centers in diamond has been previously demonstrated in condensed matter, biological, and paleomagnetic applications. Vector magnetic imaging with NV ensembles typically requires an applied field (>10 G) to separate the contributions from four crystallographic orientations, hindering studies of magnetic samples that require measurement in low or independently specified bias fields. Here we decompose the NV ensemble magnetic resonance spectrum without such a bias field by modulating the collected light at the microscope's Fourier plane. In addition to enabling vector magnetic imaging at arbitrarily low fields, our method can be used to extend the dynamic range at a given bias field. As demonstrated here, optically-detected diamond magnetometry stands to benefit from Fourier optical approaches, which have already found widespread utility in other branches of photonics.

Using a turn-key Ti:sapphire femtosecond laser frequency comb, an off-the-shelf supercontinuum device, and Fabry-Perot mode filters, we report the generation of a 16 GHz frequency comb spanning a 90 nm band about a center wavelength of 566 nm. The light from this astro-comb is used to calibrate the HARPS-N astrophysical spectrograph for precision radial velocity measurements. The comb-calibrated spectrograph achieves a stability of $\sim$ 1 cm/s within half an hour of averaging time. We also use the astro-comb as a reference for measurements of solar spectra obtained with a compact telescope, and as a tool to study intrapixel sensitivity variations on the CCD of the spectrograph.

Magnetic resonance imaging (MRI) is a widely used biomedical imaging modality that derives much of its contrast from microscale magnetic field gradients in biological tissues. However, the connection between these sub-voxel field patterns and MRI contrast has not been studied experimentally. Here, we describe a new method to map subcellular magnetic fields in mammalian cells and tissues using nitrogen vacancy diamond magnetometry and connect these maps to voxel-scale MRI contrast, providing insights for in vivo imaging and contrast agent design.

Zircon crystals offer a unique combination of suitability for high-precision radiometric dating and high resistance to alteration. Paleomagnetic experiments on ancient zircons may potentially constrain the earliest geodynamo, which holds broad implications for the early Earth interior and atmosphere. However, the ability of zircons to record accurately the geomagnetic field has not been fully demonstrated. Here we conduct thermal and room temperature alternating field (AF) paleointensity experiments on 767.1 thousand year old (ka) zircons from the Bishop Tuff, California. The rapid emplacement of these zircons in a well-characterized magnetic field provides a high-fidelity test of the zircons intrinsic paleomagnetic recording accuracy. Successful dual heating experiments on nine zircons measured using a superconducting quantum interference device (SQUID) microscope yield a mean paleointensity of 46.2 +/- 18.8 microtesla (1sigma), which agrees closely with high-precision results from Bishop Tuff whole rock (43.0 +/- 3.2 microtesla). High-resolution quantum diamond magnetic mapping, electron microscopy, and X-ray tomography indicate that the bulk of the remanent magnetization in Bishop Tuff zircons is carried by Fe oxides associated with apatite inclusions, which would be susceptible to destruction via metamorphism and aqueous alteration in older zircons. As such, while zircons can reliably record the geomagnetic field, robust zircon-derived paleomagnetic results require careful characterization of the ferromagnetic carrier and demonstration of their occurrence in primary inclusions. We further conclude that a combination of quantum diamond magnetometry and high-resolution imaging can provide detailed, direct characterization of the ferromagnetic mineralogy of geological samples.

A key challenge for neuroscience is noninvasive, label-free sensing of action potential (AP) dynamics in whole organisms with single-neuron resolution. Here, we present a new approach to this problem: using nitrogen-vacancy (NV) quantum defects in diamond to measure the time-dependent magnetic fields produced by single-neuron APs. Our technique has a unique combination of features: (i) it is noninvasive, as the light that probes the NV sensors stays within the biocompatible diamond chip and does not enter the organism, enabling activity monitoring over extended periods; (ii) it is label-free and should be widely applicable to most organisms; (iii) it provides high spatial and temporal resolution, allowing precise measurement of the AP waveforms and conduction velocities of individual neurons; (iv) it directly determines AP propagation direction through the inherent sensitivity of NVs to the associated AP magnetic field vector; (v) it is applicable to neurons located within optically opaque tissue or whole organisms, through which magnetic fields pass largely unperturbed; and (vi) it is easy-to-use, scalable, and can be integrated with existing techniques such as wide-field and superresolution imaging. We demonstrate our method using excised single neurons from two invertebrate species, marine worm and squid; and then by single-neuron AP magnetic sensing exterior to whole, live, opaque marine worms for extended periods with no adverse effect. The results lay the groundwork for real-time, noninvasive 3D magnetic mapping of functional neuronal networks, ultimately with synapse-scale (~10 nm) resolution and circuit-scale (~1 cm) field-of-view.

We probe small scalar coupling differences via the coherent interactions between two nuclear spin singlet states in organic molecules. We show that the spin-lock induced crossing (SLIC) technique enables the coherent transfer of singlet order between one spin pair and another. The transfer is mediated by the difference in cis and trans vicinal J couplings among the spins. By measuring the transfer rate, we calculate a J coupling difference of $8 \pm 2$ mHz in phenylalanine-glycine-glycine and $2.57 \pm 0.04$ Hz in glutamate. We also characterize a coherence between two singlet states in glutamate, which may enable the creation of a long-lived quantum memory.

We demonstrate an all-optical method for magnetic sensing of individual molecules in ambient conditions at room temperature. Our approach is based on shallow nitrogen-vacancy (NV) centers near the surface of a diamond crystal, which we use to detect single paramagnetic molecules covalently attached to the diamond surface. The manipulation and readout of the NV centers is all-optical and provides a sensitive probe of the magnetic field fluctuations stemming from the dynamics of the electronic spins of the attached molecules. As a specific example, we demonstrate detection of a single paramagnetic molecule containing a gadolinium (Gd$^{3+}$) ion. We confirm single-molecule resolution using optical fluorescence and atomic force microscopy to co-localize one NV center and one Gd$^{3+}$-containing molecule. Possible applications include nanoscale and in vivo magnetic spectroscopy and imaging of individual molecules.

We introduce a broadly applicable technique to create nuclear spin singlet states in organic molecules and other many-atom systems. We employ a novel pulse sequence to produce a spin-lock induced crossing (SLIC) of the spin singlet and triplet energy levels, which enables triplet/singlet polarization transfer and singlet state preparation. We demonstrate the utility of the SLIC method by producing a long-lived nuclear spin singlet state on two strongly-coupled proton pairs in the tripeptide molecule phenylalanine-glycine-glycine dissolved in D2O, and by using SLIC to measure the J-couplings, chemical shift differences, and singlet lifetimes of the proton pairs. We show that SLIC is more efficient at creating nearly-equivalent nuclear spin singlet states than previous pulse sequence techniques, especially when triplet/singlet polarization transfer occurs on the same timescale as spin-lattice relaxation.

Correlative light and electron microscopy promises to combine molecular specificity with nanoscale imaging resolution. However, there are substantial technical challenges including reliable co-registration of optical and electron images, and rapid optical signal degradation under electron beam irradiation. Here, we introduce a new approach to solve these problems: multi-color imaging of stable optical cathodoluminescence emitted in a scanning electron microscope by nanoparticles with controllable surface chemistry. We demonstrate well-correlated cathodoluminescence and secondary electron images using three species of semiconductor nanoparticles that contain defects providing stable, spectrally-distinguishable cathodoluminescence. We also demonstrate reliable surface functionalization of the particles. The results pave the way for the use of such nanoparticles for targeted labeling of surfaces to provide nanoscale mapping of molecular composition, indicated by cathodoluminescence color, simultaneously acquired with structural electron images in a single instrument.

We measure the lifetime of long-lived nuclear spin singlet states as a function of the strength of the RF spin-locking field and present a simple theoretical model that agrees well with our measurements, including the low-RF-power regime. We also measure the lifetime of a long-lived coherence between singlet and triplet states that does not require a spin-locking field for preservation. Our results indicate that for many molecules, singlet states can be created using weak RF spin-locking fields: more than two orders of magnitude lower RF power than in previous studies. Our findings suggest that in many biomolecules, singlets and related states with enhanced lifetimes might be achievable in vivo with safe levels of RF power.

We demonstrate that Michelson-Morley tests, which detect direction-dependent anisotropies in the speed of light, can also be used to place limits upon isotropic deviations of the vacuum speed of light from $c$, as described by the photon sector Standard Model Extension (SME) parameter $\tilde{\kappa}_{tr}$. A shift in the speed of light that is isotropic in one inertial frame implies anisotropic shifts in others. Using observer Lorentz covariance, we derive the time-dependent variations in the relative resonance frequencies of a pair of electromagnetic resonators that would be generated by such a shift in the rest frame of the Sun. A new analysis of a recent experimental test of relativity using this result constrains $\tilde{\kappa}_{tr}$ with a precision of $7.4\times10^{-9}$. This represents the first constraint on $\tilde{\kappa}_{tr}$ by a Michelson-Morley experiment and the first analysis of a single experiment to simultaneously set limits on all nine non-birefringent terms in the photon sector of the SME.

Improved wavelength calibrators for high-resolution astrophysical spectrographs will be essential for precision radial velocity (RV) detection of Earth-like exoplanets and direct observation of cosmological deceleration. The astro-comb is a combination of an octave-spanning femtosecond laser frequency comb and a Fabry-Pérot cavity used to achieve calibrator line spacings that can be resolved by an astrophysical spectrograph. Systematic spectral shifts associated with the cavity can be 0.1-1 MHz, corresponding to RV errors of 10-100 cm/s, due to the dispersive properties of the cavity mirrors over broad spectral widths. Although these systematic shifts are very stable, their correction is crucial to high accuracy astrophysical spectroscopy. Here, we demonstrate an \emphin-situ technique to determine the systematic shifts of astro-comb lines due to finite Fabry-Pérot cavity dispersion. The technique is practical for implementation at a telescope-based spectrograph to enable wavelength calibration accuracy better than 10 cm/s.

We propose and analyze a new approach to generate a broadband astro-comb by spectral broadening of a narrowband astro-comb inside a highly nonlinear optical fiber. Numerical modeling shows that cascaded four-wave-mixing dramatically degrades the input comb's side-mode suppression and causes side-mode amplitude asymmetry. These two detrimental effects can systematically shift the center-of-gravity of astro-comb spectral lines as measured by an astrophysical spectrograph with resolution \approx100,000; and thus lead to wavelength calibration inaccuracy and instability. Our simulations indicate that this performance penalty, as a result of nonlinear spectral broadening, can be compensated by using a filtering cavity configured for double-pass. As an explicit example, we present a design based on an Yb-fiber source comb (with 1 GHz repetition rate) that is filtered by double-passing through a low finesse cavity (finesse = 208), and subsequent spectrally broadened in a 2-cm, SF6-glass photonic crystal fiber. Spanning more than 300 nm with 16 GHz line spacing, the resulting astro-comb is predicted to provide 1 cm/s (~10 kHz) radial velocity calibration accuracy for an astrophysical spectrograph. Such extreme performance will be necessary for the search for and characterization of Earth-like extra-solar planets, and in direct measurements of the change of the rate of cosmological expansion.

We present a joint theoretical and experimental characterization of the coherent population trapping (CPT) resonance excited on the D1 line of 87Rb atoms by bichromatic linearly polarized laser light. We observe high-contrast transmission resonances (up to 25%), which makes this excitation scheme promising for miniature all-optical atomic clock applications. We also demonstrate cancellation of the first-order light shift by proper choice of the frequencies and relative intensities of the two laser field components. Our theoretical predictions are in good agreement with the experimental results.

We discuss the feasibility of negative refraction with reduced absorption in coherently driven atomic media. Coherent coupling of an electric and a magnetic dipole transition by laser fields induces magneto-electric cross-coupling and negative refraction at dipole densities which are considerably smaller than necessary to achieve a negative permeability. At the same time the absorption gets minimized due to destructive quantum interference and the ratio of negative refraction index to absorption becomes orders of magnitude larger than in systems without coherent cross-coupling. The proposed scheme allows for a fine-tuning of the refractive index. We derive a generalized expression for the impedance of a medium with magneto-electric cross coupling and show that impedance matching to vacuum can easily be achieved. Finally we discuss the tensorial properties of the medium response and derive expressions for the dependence of the refractive index on the propagation direction.

We show that a characteristic two photon lineshape asymmetry arises in coherent population trapping (CPT) and three photon (N) resonances because both resonances are simultaneously induced by modulation sidebands in the interrogating laser light. The N resonance is a three-photon resonance in which a two-photon Raman excitation is combined with a resonant optical pumping field. This joint CPT and N resonance can be the dominant source of lineshape distortion, with direct relevance for the operation of miniaturized atomic frequency standards. We present the results of both an experimental study and theoretical treatment of the asymmetry of the joint CPT and N resonance under conditions typical to the operation of an N resonance clock.

Space-based experiments today can uniquely address important questions related to the fundamental laws of Nature. In particular, high-accuracy physics experiments in space can test relativistic gravity and probe the physics beyond the Standard Model; they can perform direct detection of gravitational waves and are naturally suited for precision investigations in cosmology and astroparticle physics. In addition, atomic physics has recently shown substantial progress in the development of optical clocks and atom interferometers. If placed in space, these instruments could turn into powerful high-resolution quantum sensors greatly benefiting fundamental physics. We discuss the current status of space-based research in fundamental physics, its discovery potential, and its importance for modern science. We offer a set of recommendations to be considered by the upcoming National Academy of Sciences' Decadal Survey in Astronomy and Astrophysics. In our opinion, the Decadal Survey should include space-based research in fundamental physics as one of its focus areas. We recommend establishing an Astronomy and Astrophysics Advisory Committee's interagency ``Fundamental Physics Task Force'' to assess the status of both ground- and space-based efforts in the field, to identify the most important objectives, and to suggest the best ways to organize the work of several federal agencies involved. We also recommend establishing a new NASA-led interagency program in fundamental physics that will consolidate new technologies, prepare key instruments for future space missions, and build a strong scientific and engineering community. Our goal is to expand NASA's science objectives in space by including ``laboratory research in fundamental physics'' as an element in agency's ongoing space research efforts.

The human lung and its functions are extremely sensitive to orientation and posture, and debate continues as to the role of gravity and the surrounding anatomy in determining lung function and heterogeneity of perfusion and ventilation. However, study of these effects is difficult. The conventional high-field magnets used for most hyperpolarized 3He MRI of the human lung, and most other common radiological imaging modalities including PET and CT, restrict subjects to lying horizontally, minimizing most gravitational effects. In this paper, we briefly review the motivation for posture-dependent studies of human lung function, and present initial imaging results of human lungs in the supine and vertical body orientations using inhaled hyperpolarized 3He gas and an open-access MRI instrument. The open geometry of this MRI system features a "walk-in" capability that permits subjects to be imaged in vertical and horizontal positions, and potentially allows for complete rotation of the orientation of the imaging subject in a two-dimensional plane. Initial results include two-dimensional lung images acquired with ~ 4 mm in-plane resolution and three-dimensional images with ~ 1.5 cm slice thickness. Effects of posture variation are observed.

We demonstrate slow and stored light in Rb vapor with a combination of desirable features: minimal loss and distortion of the pulse shape, and large fractional delay (> 10). This behavior is enabled by: (i) a group index that can be controllably varied during light pulse propagation; and (ii) controllable gain integrated into the medium to compensate for pulse loss. Any medium with the above two characteristics should be able to realize similarly high-performance slow light.

We report an experimental comparison of three-photon-absorption resonances (known as "N-resonances") for the D_1 and D_2 optical transitions of thermal 87Rb vapor. We find that the D_2 N-resonance has better contrast, a broader linewidth, and a more symmetric lineshape than the D_1 N-resonance. Taken together, these factors imply superior performance for frequency standards operating on alkali D_2 N-resonances, in contrast to coherent population trapping (CPT) resonances for which the D_2 transition provides poorer frequency standard performance than the D_1 transition.

We demonstrate that first-order light-shifts can be cancelled for an all-optical, three-photon-absorption resonance ("N-resonance") on the D1 transition of Rb87. This light-shift cancellation enables improved frequency stability for an N-resonance clock. For example, using a table-top apparatus designed for N-resonance spectroscopy, we measured a short-term fractional frequency stability (Allan deviation) 1.5e-11 tau^(-1/2) for observation times 1s< tau < 50s. Further improvements in frequency stability should be possible with an apparatus designed as a dedicated N-resonance clock.

We report an experimental study of an all-optical three-photon-absorption resonance (known as a "N-resonance") and discuss its potential application as an alternative to atomic clocks based on coherent population trapping (CPT). We present measurements of the N-resonance contrast, width and light-shift for the D1 line of 87Rb with varying buffer gases, and find good agreement with an analytical model of this novel resonance. The results suggest that N-resonances are promising for atomic clock applications.

We investigate systematic errors associated with a common modulation technique used for phase sensitive detection of a coherent population trapping (CPT) resonance. In particular, we show that modification of the CPT resonance lineshape due to the presence of off-resonant fields leads to frequency shifts which may limit the stability of CPT-based atomic clocks. We also demonstrate that an alternative demodulation technique greatly reduces these effects.

The human lung and its functions are extremely sensitive to gravity, however the conventional high-field magnets used for most laser-polarized 3He MRI of the human lung restrict subjects to lying horizontally. Imaging of human lungs using inhaled laser-polarized 3He gas is demonstrated in an open-access very-low-magnetic-field (< 5 mT) MRI instrument. This prototype device employs a simple, low-cost electromagnet, with an open geometry that allows variation of the orientation of the imaging subject in a two-dimensional plane. As a demonstration, two-dimensional lung images were acquired with 4 mm in-plane resolution from a subject in two orientations: lying supine, and sitting in a vertical position with one arm raised. Experience with this prototype device will guide optimization of a second-generation very-low-field imager to enable studies of human pulmonary physiology as a function of subject orientation.

A search for an annual variation of a daily sidereal modulation of the frequency difference between co-located ${}^{129}$Xe and ${}^{3}$He Zeeman masers sets a stringent limit on boost-dependent Lorentz and CPT violation involving the neutron, consistent with no effect at the level of 150 nHz. In the framework of the general Standard-Model Extension, the present result provides the first clean test for the fermion sector of the symmetry of spacetime under boost transformations at a level of $10^{-27}$ GeV.

We present details from a recent test of Lorentz and CPT symmetry using hydrogen masers. We have placed a new limit on Lorentz and CPT violation of the proton in terms of a recent standard model extension by placing a bound on sidereal variation of the F = 1 Zeeman frequency in hydrogen. Here, the theoretical standard model extension is reviewed. The operating principles of the maser and the double resonance technique used to measure the Zeeman frequency are discussed. The characterization of systematic effects is described, and the method of data analysis is presented. We compare our result to other recent experiments, and discuss potential steps to improve our measurement.

Using a novel NMR scheme we observed persistence in 1-D gas diffusion. Analytical approximations and numerical simulations have indicated that for an initially random array of spins undergoing diffusion, the probability p(t) that the average spin magnetization in a given region has not changed sign (i.e., ``persists'') up to time t follows a power law t^-\theta, where \theta depends on the dimensionality of the system. Using laser-polarized ^129Xe gas, we prepared an initial ``quasirandom'' 1D array of spin magnetization and then monitored the ensemble's evolution due to diffusion using real-time NMR imaging. Our measurements are consistent with analytical and numerical predictions of \theta ≈0.12.

We present a new measurement constraining Lorentz and CPT violation of the proton using a hydrogen maser double resonance technique. A search for hydrogen Zeeman frequency variations with a period of the sidereal day (23.93 h) sets a clean limit on violation of Lorentz and CPT symmetry of the proton at the 10^-27 GeV level.

We compared the frequency shift of the 21Ne Zeeman resonance induced by polarized Rb vapor to the shift induced in the 3He Zeeman resonance. The 3He/Rb shift has recently been measured with high precision, permitting the conversion of our differential measurement to an absolute value for the 21Ne/Rb shift. We report a value of K = 31.8 +/- 2.8 for the Rb/21Ne enhancement factor at a temperature of 124.8 +/- 1.9 C. We propose high-precision differential contact shift measurements, the absolute accuracy of which would be limited by the error in the 3He contact shift.

We present two new measurements constraining Lorentz and CPT violation using the Xe-129 / He-3 Zeeman maser and atomic hydrogen masers. Experimental investigations of Lorentz and CPT symmetry provide important tests of the framework of the standard model of particle physics and theories of gravity. The two-species Xe-129 / He-3 Zeeman maser bounds violations of CPT and Lorentz symmetry of the neutron at the 10^-31 GeV level. Measurements with atomic hydrogen masers provide a clean limit of CPT and Lorentz symmetry violation of the proton at the 10^-27 GeV level.

We present two new measurements constraining Lorentz and CPT violation using the Xe-129 / He-3 Zeeman maser and atomic hydrogen masers. Experimental investigations of Lorentz and CPT symmetry provide important tests of the framework of the standard model of particle physics and theories of gravity. The two-species Xe-129 / He-3 Zeeman maser bounds violations of CPT and Lorentz symmetry of the neutron at the 10^-31 GeV level. Measurements with atomic hydrogen masers provide a clean limit of CPT and Lorentz symmetry violation of the proton at the 10^-27 GeV level.

We use the dressed atom formalism to calculate the frequency shift in a hydrogen maser induced by applied radiation near the Zeeman frequency, and find excellent agreement with a previous calculation made in the bare atom basis. The maser oscillates on the Delta_F = 1, Delta_m_F = 0 hyperfine transition, while the applied field is swept through the F = 1, Delta_m_F = \pm 1 Zeeman resonance. We determine the effect of the applied field on the Zeeman levels using the dressed atom picture, and then calculate the maser frequency shift by coupling the dressed states to the microwave cavity. Qualitatively, the dressed-atom analysis gives a new and simpler physical interpretation of this double resonance process, which has applications in precision hydrogen Zeeman spectroscopy, e.g., in fundamental symmetry tests.

A search for sidereal variations in the frequency difference between co-located 129-Xe and 3-He Zeeman masers sets the most stringent limit to date on leading-order Lorentz and CPT violation involving the neutron, consistent with no effect at the level of 10^-31 GeV.