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.

Spin Hyperpolarization in Modern Magnetic Resonance.

Magnetic resonance techniques are successfully utilized in a broad range of scientific disciplines and in various practical applications, with medical magnetic resonance imaging being the most widely known example. Currently, both fundamental and applied magnetic resonance are enjoying a major boost owing to the rapidly developing field of spin hyperpolarization. Hyperpolarization techniques are able to enhance signal intensities in magnetic resonance by several orders of magnitude, and thus to largely overcome its major disadvantage of relatively low sensitivity. This provides new impetus for existing applications of magnetic resonance and opens the gates to exciting new possibilities. In this review, we provide a unified picture of the many methods and techniques that fall under the umbrella term "hyperpolarization" but are currently seldom perceived as integral parts of the same field. Specifically, before delving into the individual techniques, we provide a detailed analysis of the underlying principles of spin hyperpolarization. We attempt to uncover and classify the origins of hyperpolarization, to establish its sources and the specific mechanisms that enable the flow of polarization from a source to the target spins. We then give a more detailed analysis of individual hyperpolarization techniques: the mechanisms by which they work, fundamental and technical requirements, characteristic applications, unresolved issues, and possible future directions. We are seeing a continuous growth of activity in the field of spin hyperpolarization, and we expect the field to flourish as new and improved hyperpolarization techniques are implemented. Some key areas for development are in prolonging polarization lifetimes, making hyperpolarization techniques more generally applicable to chemical/biological systems, reducing the technical and equipment requirements, and creating more efficient excitation and detection schemes. We hope this review will facilitate the sharing of knowledge between subfields within the broad topic of hyperpolarization, to help overcome existing challenges in magnetic resonance and enable novel applications.

Near-zero-field microwave-free magnetometry with nitrogen-vacancy centers in nanodiamonds.

We study the fluorescence of nanodiamond ensembles as a function of static external magnetic field and observe characteristic dip features close to the zero field with potential for magnetometry applications. We analyze the dependence of the feature's width and the contrast of the feature on the size of the diamond (in the range 30 nm-3000 nm) and on the strength of a bias magnetic field applied transversely to the field being scanned. We also perform optically detected magnetic resonance (ODMR) measurements to quantify the strain splitting of the zero-field ODMR resonance across various nanodiamond sizes and compare it with the width and contrast measurements of the zero-field fluorescence features for both nanodiamonds and bulk samples. The observed properties provide compelling evidence of cross-relaxation effects in the NV system occurring close to zero magnetic fields. Finally, the potential of this technique for use in practical magnetometry is discussed.

Rapid hyperpolarization and purification of the metabolite fumarate in aqueous solution.

Hyperpolarized fumarate is a promising biosensor for carbon-13 magnetic resonance metabolic imaging. Such molecular imaging applications require nuclear hyperpolarization to attain sufficient signal strength. Dissolution dynamic nuclear polarization is the current state-of-the-art methodology for hyperpolarizing fumarate, but this is expensive and relatively slow. Alternatively, this important biomolecule can be hyperpolarized in a cheap and convenient manner using parahydrogen-induced polarization. However, this process requires a chemical reaction, and the resulting solutions are contaminated with the catalyst, unreacted reagents, and reaction side-product molecules, and are hence unsuitable for use in vivo. In this work we show that the hyperpolarized fumarate can be purified from these contaminants by acid precipitation as a pure solid, and later redissolved to a desired concentration in a clean aqueous solvent. Significant advances in the reaction conditions and reactor equipment allow for formation of hyperpolarized fumarate at 13C polarization levels of 30-45%.

Zero- to Ultralow-Field Nuclear Magnetic Resonance Enhanced with Dissolution Dynamic Nuclear Polarization.

Zero- to ultralow-field nuclear magnetic resonance is a modality of magnetic resonance experiment which does not require strong superconducting magnets. Contrary to conventional high-field nuclear magnetic resonance, it has the advantage of allowing high-resolution detection of nuclear magnetism through metal as well as within heterogeneous media. To achieve high sensitivity, it is common to couple zero-field nuclear magnetic resonance with hyperpolarization techniques. To date, the most common technique is parahydrogen-induced polarization, which is only compatible with a small number of compounds. In this article, we establish dissolution dynamic nuclear polarization as a versatile method to enhance signals in zero-field nuclear magnetic resonance experiments on sample mixtures of [13C]sodium formate, [1-13C]glycine, and [2-13C]sodium acetate, and our technique is immediately extendable to a broad range of molecules with >1 s relaxation times. We find signal enhancements of up to 11,000 compared with thermal prepolarization in a 2 T permanent magnet. To increase the signal in future experiments, we investigate the relaxation effects of the TEMPOL radicals used for the hyperpolarization process at zero- and ultralow-fields.

Enzymatic Reactions Observed with Zero- and Low-Field Nuclear Magnetic Resonance.

We demonstrate that enzyme-catalyzed reactions can be observed in zero- and low-field NMR experiments by combining recent advances in parahydrogen-based hyperpolarization methods with state-of-the-art magnetometry. Specifically, we investigated two model biological processes: the conversion of fumarate into malate, which is used in vivo as a marker of cell necrosis, and the conversion of pyruvate into lactate, which is the most widely studied metabolic process in hyperpolarization-enhanced imaging. In addition to this, we constructed a microfluidic zero-field NMR setup to perform experiments on microliter-scale samples of [1-13C]fumarate in a lab-on-a-chip device. Zero- to ultralow-field (ZULF) NMR has two key advantages over high-field NMR: the signals can pass through conductive materials (e.g., metals), and line broadening from sample heterogeneity is negligible. To date, the use of ZULF NMR for process monitoring has been limited to studying hydrogenation reactions. In this work, we demonstrate this emerging analytical technique for more general reaction monitoring and compare zero- vs low-field detection.

Diamond-optic enhanced photon collection efficiency for sensing with nitrogen-vacancy centers.

We present a design to increase the amount of collected fluorescence emitted by nitrogen-vacancy color centers in diamond used for quantum-sensing. An improvement was measured in collected fluorescence when comparing oppositely faced emitting surfaces by a factor of 3.8(1). This matches ray-tracing simulation results. This design therefore improves on the shot noise limited sensitivity in optical readout-based measurements of, for instance, magnetic and electric fields, pressure, temperature, and rotations.

Heading-Error-Free Optical Atomic Magnetometry in the Earth-Field Range.

We demonstrate an alignment-based ^{87}Rb magnetometer that is immune to nonlinear Zeeman (NLZ) splitting, addressing an important problem in alkali-metal atomic magnetometry. In our scheme, there is a single magnetic resonance peak and well-separated hyperfine transition frequencies, making the magnetometer insensitive or even immune to NLZ-related heading errors. It is shown that the magnetometer can be implemented for practical measurements in geomagnetic environments, and the photon-shot-noise-limited sensitivity reaches 9 fT/sqrt[Hz] at 5 µT and remains at tens of fT/sqrt[Hz] at 50 µT at room temperature.

Search for Ultralight Dark Matter with Spectroscopy of Radio-Frequency Atomic Transitions.

The effects of scalar and pseudoscalar ultralight bosonic dark matter (UBDM) were searched for by comparing the frequency of a quartz oscillator to that of a hyperfine-structure transition in ^{87}Rb, and an electronic transition in ^{164}Dy. We constrain linear interactions between a scalar UBDM field and standard-model (SM) fields for an underlying UBDM particle mass in the range 1×10^{-17}-8.3×10^{-13} eV and quadratic interactions between a pseudoscalar UBDM field and SM fields in the range 5×10^{-18}-4.1×10^{-13} eV. Within regions of the respective ranges, our constraints on linear interactions significantly improve on results from previous, direct searches for oscillations in atomic parameters, while constraints on quadratic interactions surpass limits imposed by such direct searches as well as by astrophysical observations.

Constraints on Spin-Spin Velocity-Dependent Interactions.

The existence of exotic spin-dependent forces may shine light on new physics beyond the standard model. We utilize two iron shielded SmCo_{5} electron-spin sources and two optically pumped magnetometers to search for exotic long-range spin-spin velocity-dependent force. The orientations of spin sources and magnetometers are optimized such that the exotic force is enhanced and common-mode noise is effectively subtracted. We set direct limit on proton-electron interaction in the force range from 1 cm to 1 km. Our experiment represents more than 10 orders of magnitude improvement than previous works.

Ultrasensitive Atomic Comagnetometer with Enhanced Nuclear Spin Coherence.

Achieving high energy resolution in spin systems is important for fundamental physics research and precision measurements, with alkali-noble-gas comagnetometers being among the best available sensors. We found a new relaxation mechanism in such devices, the gradient of the Fermi-contact-interaction field that dominates the relaxation of hyperpolarized nuclear spins. We report on precise control over spin distribution, demonstrating a tenfold increase of nuclear spin hyperpolarization and transverse coherence time with optimal hybrid optical pumping. Operating in the self-compensation regime, our ^{21}Ne-Rb-K comagnetometer achieves an ultrahigh inertial rotation sensitivity of 3×10^{-8} rad/s/Hz^{1/2} in the frequency range from 0.2 to 1.0 Hz, which is equivalent to the energy resolution of 3.1×10^{-23} eV/Hz^{1/2}. We propose to use this comagnetometer to search for exotic spin-dependent interactions involving proton and neutron spins. The projected sensitivity surpasses the previous experimental and astrophysical limits by more than 4 orders of magnitude.

Sensitive magnetometry reveals inhomogeneities in charge storage and weak transient internal currents in Li-ion cells.

The ever-increasing demand for high-capacity rechargeable batteries highlights the need for sensitive and accurate diagnostic technology for determining the state of a cell, for identifying and localizing defects, and for sensing capacity loss mechanisms. Here, we leverage atomic magnetometry to map the weak induced magnetic fields around Li-ion battery cells in a magnetically shielded environment. The ability to rapidly measure cells nondestructively allows testing even commercial cells in their actual operating conditions, as a function of state of charge. These measurements provide maps of the magnetic susceptibility of the cell, which follow trends characteristic for the battery materials under study upon discharge. In particular, hot spots of charge storage are identified. In addition, the measurements reveal the capability to measure transient internal current effects, at a level of µA, which are shown to be dependent upon the state of charge. These effects highlight noncontact battery characterization opportunities. The diagnostic power of this technique could be used for the assessment of cells in research, quality control, or during operation, and could help uncover details of charge storage and failure processes in cells.

Floquet Spin Amplification.

Detection of weak electromagnetic waves and hypothetical particles aided by quantum amplification is important for fundamental physics and applications. However, demonstrations of quantum amplification are still limited; in particular, the physics of quantum amplification is not fully explored in periodically driven (Floquet) systems, which are generally defined by time-periodic Hamiltonians and enable observation of many exotic quantum phenomena such as time crystals. Here we investigate the magnetic-field signal amplification by periodically driven ^{129}Xe spins and observe signal amplification at frequencies of transitions between Floquet spin states. This "Floquet amplification" allows us to simultaneously enhance and measure multiple magnetic fields with at least one order of magnitude improvement, offering the capability of femtotesla-level measurements. Our findings extend the physics of quantum amplification to Floquet spin systems and can be generalized to a wide variety of existing amplifiers, enabling a previously unexplored class of "Floquet spin amplifiers".

Improved Bounds on Ultralight Scalar Dark Matter in the Radio-Frequency Range.

We present a search for fundamental constant oscillations in the range 20 kHz-100 MHz that may arise within models for ultralight dark matter (UDM). Using two independent optical-spectroscopy apparatuses, we achieve up to ×1000 greater sensitivity in the search relative to previous work [D. Antypas et al., Phys. Rev. Lett. 123, 141102 (2019).PRLTAO0031-900710.1103/PhysRevLett.123.141102]. We report no observation of UDM and thus constrain respective couplings to electrons and photons within the investigated UDM particle mass range 8×10^{-11}-4×10^{-7} eV. The constraints significantly exceed previously set bounds from atomic spectroscopy and, as we show, may surpass in future experiments those provided by equivalence-principle (EP) experiments in a specific case regarding the combination of UDM couplings probed by the EP experiments.

Limits on Axions and Axionlike Particles within the Axion Window Using a Spin-Based Amplifier.

Searches for the axion and axionlike particles may hold the key to unlocking some of the deepest puzzles about our Universe, such as dark matter and dark energy. Here, we use the recently demonstrated spin-based amplifier to constrain such hypothetical particles within the well-motivated "axion window" (10 µeV-1 meV) through searching for an exotic dipole-dipole interaction between polarized electron and neutron spins. The key ingredient is the use of hyperpolarized long-lived ^{129}Xe nuclear spins as an amplifier for the pseudomagnetic field generated by the exotic interaction. Using such a spin sensor, we obtain a direct upper bound on the product of coupling constants g_{p}^{e}g_{p}^{n}. The spin-based amplifier technique can be extended to searches for a wide variety of hypothetical particles beyond the standard model.

Zero- to Ultralow-Field NMR Spectroscopy of Small Biomolecules.

Nuclear magnetic resonance (NMR) spectroscopy is a well-established analytical technique used to study chemicals and their transformations. However, high-field NMR spectroscopy necessitates advanced infrastructure, and even cryogen-free benchtop NMR spectrometers cannot be readily assembled from commercially available components. We demonstrate construction of a portable zero-field NMR spectrometer employing a commercially available magnetometer and investigate its applications in analytical chemistry. In particular, J-spectra of small representative biomolecules [13C]-formic acid, [1-13C]-glycine, [2,3-13C]-fumarate, and [1-13C]-d-glucose were acquired, and an approach relying on the presence of a transverse magnetic field during the detection was investigated for relaxometry purposes. We found that the water relaxation time strongly depends on the concentration of dissolved d-glucose in the range of 1-10 mM suggesting opportunities for indirect assessment of glucose concentration in aqueous solutions. Extending analytical capabilities of zero-field NMR to aqueous solutions of simple biomolecules (amino acids, sugars, and metabolites) and relaxation studies of aqueous solutions of glucose highlights the analytical potential of noninvasive and portable ZULF NMR sensors for applications outside of research laboratories.

Intensity-correlated spiking of infrared and ultraviolet emission from sodium vapors.

Temporal spiking of directional infrared and ultraviolet cooperative emission from sodium vapors excited to the $4D_{5/2}$ level with a continuous-wave resonant laser pump is analyzed. Mirrorless lasing at 2207 and 2338 nm on cascade population-inverted transitions and radiation at 330 nm generated due to four-wave mixing demonstrate a high degree of intensity correlation.

Surpassing the Energy Resolution Limit with Ferromagnetic Torque Sensors.

We discuss the fundamental noise limitations of a ferromagnetic torque sensor based on a levitated magnet in the tipping regime. We evaluate the optimal magnetic field resolution taking into account the thermomechanical noise and the mechanical detection noise at the standard quantum limit. We find that the energy resolution limit, pointed out in recent literature as a relevant benchmark for most classes of magnetometers, can be surpassed by many orders of magnitude. Moreover, similarly to the case of a ferromagnetic gyroscope, it is also possible to surpass the standard quantum limit for magnetometry with independent spins, arising from spin-projection noise. Our finding indicates that magnetomechanical systems optimized for magnetometry can achieve a magnetic field resolution per unit volume several orders of magnitude better than any conventional magnetometer. We discuss possible implications, focusing on fundamental physics problems such as the search for exotic interactions beyond the standard model.

Stand-Off Magnetometry with Directional Emission from Sodium Vapors.

Stand-off magnetometry allows measuring magnetic field at a distance, and can be employed in geophysical research, hazardous environment monitoring, and security applications. Stand-off magnetometry based on resonant scattering from atoms or molecules is often limited by the scarce amounts of detected light. The situation would be dramatically improved if the light emitted by excited atoms were to propagate towards the excitation light source in a directional manner. Here, we demonstrate that this is possible by means of mirrorless lasing. In a tabletop experiment, we detect free-precession signals of ground-state sodium spins under the influence of an external magnetic field by measuring backward-directed light. This method enables scalar magnetometry in the Earth field range, that can be extended to long-range remote sensing.

Search for Axionlike Dark Matter Using Solid-State Nuclear Magnetic Resonance.

We report the results of an experimental search for ultralight axionlike dark matter in the mass range 162-166 neV. The detection scheme of our Cosmic Axion Spin Precession Experiment is based on a precision measurement of ^{207}Pb solid-state nuclear magnetic resonance in a polarized ferroelectric crystal. Axionlike dark matter can exert an oscillating torque on ^{207}Pb nuclear spins via the electric dipole moment coupling g_{d} or via the gradient coupling g_{aNN}. We calibrate the detector and characterize the excitation spectrum and relaxation parameters of the nuclear spin ensemble with pulsed magnetic resonance measurements in a 4.4 T magnetic field. We sweep the magnetic field near this value and search for axionlike dark matter with Compton frequency within a 1 MHz band centered at 39.65 MHz. Our measurements place the upper bounds |g_{d}|<9.5×10^{-4} GeV^{-2} and |g_{aNN}|<2.8×10^{-1} GeV^{-1} (95% confidence level) in this frequency range. The constraint on g_{d} corresponds to an upper bound of 1.0×10^{-21} e cm on the amplitude of oscillations of the neutron electric dipole moment and 4.3×10^{-6} on the amplitude of oscillations of CP-violating θ parameter of quantum chromodynamics. Our results demonstrate the feasibility of using solid-state nuclear magnetic resonance to search for axionlike dark matter in the neV mass range.