Search for Dark-Matter-Induced Oscillations of Fundamental Constants Using Molecular Spectroscopy.

A possible implication of an ultralight dark matter field interacting with the standard model degrees of freedom is oscillations of fundamental constants. Here, we establish direct experimental bounds on the coupling of an oscillating ultralight dark matter field to the up, down, and strange quarks and to the gluons, for oscillation frequencies between 10 and 10^{8} Hz. We employ spectroscopic experiments that take advantage of the dependence of molecular transition frequencies on the nuclear masses. Our results apply to previously unexplored frequency bands and improve on existing bounds at frequencies >5 MHz. We also improve on the bounds for coupling to the electromagnetic field and the electron field, in particular spectral windows. We identify a sector of ultralight dark matter and standard model coupling space where the bounds from equivalence principle tests may be challenged by next-generation experiments of the present kind.

Precision Determination of Isotope Shifts in Ytterbium and Implications for New Physics.

We report measurements of isotope shifts for the five spinless Yb isotopes on the 6s^{2} ^{1}S_{0}→5d6s ^{1}D_{2} transition using Doppler-free two-photon spectroscopy. We combine these data with existing measurements on two transitions in Yb^{+} [Counts et al. Phys. Rev. Lett. 125, 123002 (2020)PRLTAO0031-900710.1103/PhysRevLett.125.123002], where deviation from King-plot linearity showed hints of a new bosonic force carrier at the 3σ level. The combined data strongly reduce the significance of the new-physics signal. We show that the observed nonlinearity in the joint Yb/Yb^{+} King-plot analysis can be accounted for by the deformation of the Yb nuclei.

Emergent hydrodynamics in a strongly interacting dipolar spin ensemble.

Conventional wisdom holds that macroscopic classical phenomena naturally emerge from microscopic quantum laws1-7. However, despite this mantra, building direct connections between these two descriptions has remained an enduring scientific challenge. In particular, it is difficult to quantitatively predict the emergent 'classical' properties of a system (for example, diffusivity, viscosity and compressibility) from a generic microscopic quantum Hamiltonian7-14. Here we introduce a hybrid solid-state spin platform, where the underlying disordered, dipolar quantum Hamiltonian gives rise to the emergence of unconventional spin diffusion at nanometre length scales. In particular, the combination of positional disorder and on-site random fields leads to diffusive dynamics that are Fickian yet non-Gaussian15-20. Finally, by tuning the underlying parameters within the spin Hamiltonian via a combination of static and driven fields, we demonstrate direct control over the emergent spin diffusion coefficient. Our work enables the investigation of hydrodynamics in many-body quantum spin systems.

Singlet-Contrast Magnetic Resonance Imaging: Unlocking Hyperpolarization with Metabolism*.

Hyperpolarization-enhanced magnetic resonance imaging can be used to study biomolecular processes in the body, but typically requires nuclei such as 13 C, 15 N, or 129 Xe due to their long spin-polarization lifetimes and the absence of a proton-background signal from water and fat in the images. Here we present a novel type of 1 H imaging, in which hyperpolarized spin order is locked in a nonmagnetic long-lived correlated (singlet) state, and is only liberated for imaging by a specific biochemical reaction. In this work we produce hyperpolarized fumarate via chemical reaction of a precursor molecule with para-enriched hydrogen gas, and the proton singlet order in fumarate is released as antiphase NMR signals by enzymatic conversion to malate in D2 O. Using this model system we show two pulse sequences to rephase the NMR signals for imaging and suppress the background signals from water. The hyperpolarization-enhanced 1 H-imaging modality presented here can allow for hyperpolarized imaging without the need for low-abundance, low-sensitivity heteronuclei.

Scalar Dark Matter in the Radio-Frequency Band: Atomic-Spectroscopy Search Results.

Among the prominent candidates for dark matter are bosonic fields with small scalar couplings to the standard-model particles. Several techniques are employed to search for such couplings, and the current best constraints are derived from tests of gravity or atomic probes. In experiments employing atoms, observables would arise from expected dark-matter-induced oscillations in the fundamental constants of nature. These studies are primarily sensitive to underlying particle masses below 10^{-14} eV. We present a method to search for fast oscillations of fundamental constants using atomic spectroscopy in cesium vapor. We demonstrate sensitivity to scalar interactions of dark matter associated with a particle mass in the range 8×10^{-11} to 4×10^{-7} eV. In this range our experiment yields constraints on such interactions, which within the framework of an astronomical-size dark matter structure are comparable with, or better than, those provided by experiments probing deviations from the law of gravity.

Direct limits on the interaction of antiprotons with axion-like dark matter.

Astrophysical observations indicate that there is roughly five times more dark matter in the Universe than ordinary baryonic matter1, and an even larger amount of the Universe's energy content is attributed to dark energy2. However, the microscopic properties of these dark components remain unknown. Moreover, even ordinary matter-which accounts for five per cent of the energy density of the Universe-has yet to be understood, given that the standard model of particle physics lacks any consistent explanation for the predominance of matter over antimatter3. Here we present a direct search for interactions of antimatter with dark matter and place direct constraints on the interaction of ultralight axion-like particles (dark-matter candidates) with antiprotons. If antiprotons have a stronger coupling to these particles than protons do, such a matter-antimatter asymmetric coupling could provide a link between dark matter and the baryon asymmetry in the Universe. We analyse spin-flip resonance data in the frequency domain acquired with a single antiproton in a Penning trap4 to search for spin-precession effects from ultralight axions, which have a characteristic frequency governed by the mass of the underlying particle. Our analysis constrains the axion-antiproton interaction parameter to values greater than 0.1 to 0.6 gigaelectronvolts in the mass range from 2 × 10-23 to 4 × 10-17 electronvolts, improving the sensitivity by up to five orders of magnitude compared with astrophysical antiproton bounds. In addition, we derive limits on six combinations of previously unconstrained Lorentz- and CPT-violating terms of the non-minimal standard model extension5.

Polychromatic, continuous-wave mirrorless lasing from monochromatic pumping of cesium vapor.

We report on the studies of simultaneous continuous-wave mirrorless lasing on multiple optical transitions, realized by pumping hot cesium (Cs) vapor with laser light resonant with the 6S1/2→8P3/2 transition. The multiplicity of the decay paths for the excited atoms to their ground state is responsible for the emergence of lasing in a number of transitions, observed here in at least seven wavelengths in the infrared and at two wavelengths in the blue. We study the properties of the fields generated in the Cs vapor such as optical power, directionality, and optical linewidth.

System for control of polarization state of light and generation of light with continuously rotating linear polarization.

We present a technique for generating light in an arbitrary polarization state. The technique is based on interference of two orthogonally polarized light beams, whose amplitudes and phases are controlled with a Mach-Zehnder inteferometer with acousto-optic modulators (AOMs) placed in each arm. We demonstrate that via control over amplitudes, phases, and frequencies of acoustic waves driving the AOMs, any polarization state can be synthesized. In particular, we demonstrate generation of linearly polarized light, whose polarization plane continuously rotates at a rate from 1 kHz to 1 MHz. Such light finds applications in science (e.g., investigations of Bloch-Siegert effect) and technology (optically pumped magnetometers).

Imaging the Local Charge Environment of Nitrogen-Vacancy Centers in Diamond.

Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields, and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at a low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning more than two orders of magnitude. Motivated by this understanding, we propose and implement a novel method for the nanoscale localization of individual charges within the diamond lattice; our approach relies upon the fact that the charge induces a NV dark state which depends on the electric field orientation.

A method for measurement of spin-spin couplings with sub-mHz precision using zero- to ultralow-field nuclear magnetic resonance.

We present a method which allows for the extraction of physical quantities directly from zero- to ultralow-field nuclear magnetic resonance (ZULF NMR) data. A numerical density matrix evolution is used to simulate ZULF NMR spectra of several molecules in order to fit experimental data. The method is utilized to determine the indirect spin-spin couplings (J-couplings) in these systems, which is achieved with precision of 10-2-10-4Hz. The simulated and measured spectra are compared to earlier research. Agreement and improved precision are achieved for most of the J-coupling estimates. The availability of fast, flexible fitting method for ZULF NMR enables a new generation of precision-measurement experiments for spin-dependent interactions and physics beyond the Standard Model.

Solution nuclear magnetic resonance spectroscopy on a nanostructured diamond chip.

Sensors using nitrogen-vacancy centers in diamond are a promising tool for small-volume nuclear magnetic resonance (NMR) spectroscopy, but the limited sensitivity remains a challenge. Here we show nearly two orders of magnitude improvement in concentration sensitivity over previous nitrogen-vacancy and picoliter NMR studies. We demonstrate NMR spectroscopy of picoliter-volume solutions using a nanostructured diamond chip with dense, high-aspect-ratio nanogratings, enhancing the surface area by 15 times. The nanograting sidewalls are doped with nitrogen-vacancies located a few nanometers from the diamond surface to detect the NMR spectrum of roughly 1 pl of fluid lying within adjacent nanograting grooves. We perform 1H and 19F nuclear magnetic resonance spectroscopy at room temperature in magnetic fields below 50 mT. Using a solution of CsF in glycerol, we determine that 4 ± 2 × 1012 19F spins in a 1 pl volume can be detected with a signal-to-noise ratio of 3 in 1 s of integration.Nitrogen vacancy (NV) centres in diamond can be used for NMR spectroscopy, but increased sensitivity is needed to avoid long measurement times. Kehayias et al. present a nanostructured diamond grating with a high density of NV centres, enabling NMR spectroscopy of picoliter-volume solutions.

Dichroic atomic vapor laser lock with multi-gigahertz stabilization range.

A dichroic atomic vapor laser lock (DAVLL) system exploiting buffer-gas-filled millimeter-scale vapor cells is presented. This system offers similar stability as achievable with conventional DAVLL system using bulk vapor cells, but has several important advantages. In addition to its compactness, it may provide continuous stabilization in a multi-gigahertz range around the optical transition. This range may be controlled either by changing the temperature of the vapor or by application of a buffer gas under an appropriate pressure. In particular, we experimentally demonstrate the ability of the system to lock the laser frequency between two hyperfine components of the (85)Rb ground state or as far as 16 GHz away from the closest optical transition.

Raman and nuclear magnetic resonance investigation of alkali metal vapor interaction with alkene-based anti-relaxation coating.

The use of anti-relaxation coatings in alkali vapor cells yields substantial performance improvements compared to a bare glass surface by reducing the probability of spin relaxation in wall collisions by several orders of magnitude. Some of the most effective anti-relaxation coating materials are alpha-olefins, which (as in the case of more traditional paraffin coatings) must undergo a curing period after cell manufacturing in order to achieve the desired behavior. Until now, however, it has been unclear what physicochemical processes occur during cell curing, and how they may affect relevant cell properties. We present the results of nondestructive Raman-spectroscopy and magnetic-resonance investigations of the influence of alkali metal vapor (Cs or K) on an alpha-olefin, 1-nonadecene coating the inner surface of a glass cell. It was found that during the curing process, the alkali metal catalyzes migration of the carbon-carbon double bond, yielding a mixture of cis- and trans-2-nonadecene.

Detection of nanoscale electron spin resonance spectra demonstrated using nitrogen-vacancy centre probes in diamond.

Electron spin resonance (ESR) describes a suite of techniques for characterizing electronic systems with applications in physics, chemistry, and biology. However, the requirement for large electron spin ensembles in conventional ESR techniques limits their spatial resolution. Here we present a method for measuring ESR spectra of nanoscale electronic environments by measuring the longitudinal relaxation time of a single-spin probe as it is systematically tuned into resonance with the target electronic system. As a proof of concept, we extracted the spectral distribution for the P1 electronic spin bath in diamond by using an ensemble of nitrogen-vacancy centres, and demonstrated excellent agreement with theoretical expectations. As the response of each nitrogen-vacancy spin in this experiment is dominated by a single P1 spin at a mean distance of 2.7 nm, the application of this technique to the single nitrogen-vacancy case will enable nanoscale ESR spectroscopy of atomic and molecular spin systems.

Search for the Effect of Massive Bodies on Atomic Spectra and Constraints on Yukawa-Type Interactions of Scalar Particles.

We propose a new method to search for hypothetical scalar particles that have feeble interactions with standard-model particles. In the presence of massive bodies, these interactions produce a nonzero Yukawa-type scalar-field magnitude. Using radio-frequency spectroscopy data of atomic dysprosium, as well as atomic clock spectroscopy data, we constrain the Yukawa-type interactions of a scalar field with the photon, electron, and nucleons for a range of scalar-particle masses corresponding to length scales >10 cm. In the limit as the scalar-particle mass m_{ϕ}→0, our derived limits on the Yukawa-type interaction parameters are Λ_{γ}≳8×10^{19} GeV, Λ_{e}≳1.3×10^{19} GeV, and Λ_{N}≳6×10^{20} GeV. Our measurements also constrain combinations of interaction parameters, which cannot otherwise be probed with traditional anomalous-force measurements. We suggest further measurements to improve on the current level of sensitivity.

Photoelectric detection of electron spin resonance of nitrogen-vacancy centres in diamond.

The readout of negatively charged nitrogen-vacancy centre electron spins is essential for applications in quantum computation, metrology and sensing. Conventional readout protocols are based on the detection of photons emitted from nitrogen-vacancy centres, a process limited by the efficiency of photon collection. We report on an alternative principle for detecting the magnetic resonance of nitrogen-vacancy centres, allowing the direct photoelectric readout of nitrogen-vacancy centres spin state in an all-diamond device. The photocurrent detection of magnetic resonance scheme is based on the detection of charge carriers promoted to the conduction band of diamond by two-photon ionization of nitrogen-vacancy centres. The optical and photoelectric detection of magnetic resonance are compared, by performing both types of measurements simultaneously. The minima detected in the measured photocurrent at resonant microwave frequencies are attributed to the spin-dependent ionization dynamics of nitrogen-vacancy, originating from spin-selective non-radiative transitions to the metastable singlet state.

Zero-field nuclear magnetic resonance spectroscopy of viscous liquids.

We report zero-field NMR measurements of a viscous organic liquid, ethylene glycol. Zero-field spectra were taken showing resolved scalar spin-spin coupling (J-coupling) for ethylene glycol at different temperatures and water contents. Molecular dynamics strongly affects the resonance linewidth, which closely follows viscosity. Quantum chemical calculations have been used to obtain the relative stability and coupling constants of all ethylene glycol conformers. The results show the potential of zero-field NMR as a probe of molecular structure and dynamics in a wide range of environments, including viscous fluids.

Limiting P-odd interactions of cosmic fields with electrons, protons, and neutrons.

We propose methods for extracting limits on the strength of P-odd interactions of pseudoscalar and pseudovector cosmic fields with electrons, protons, and neutrons, by exploiting the static and dynamic parity-nonconserving amplitudes and electric dipole moments they induce in atoms. Candidates for such fields are dark matter (including axions) and dark energy, as well as several more exotic sources described by Lorentz-violating standard model extensions. Atomic calculations are performed for H, Li, Na, K, Rb, Cs, Ba(+), Tl, Dy, Fr, and Ra(+). From these calculations and existing measurements in Dy, Cs, and Tl, we constrain the interaction strengths of the parity-violating static pseudovector cosmic field to be 7 × 10(-15) GeV with an electron, and 3 × 10(-8) GeV with a proton.

All-optical vector atomic magnetometer.

We demonstrate an all-optical magnetometer capable of measuring the magnitude and direction of a magnetic field using nonlinear magneto-optical rotation in cesium vapor. Vector capability is added by effective modulation of the field along orthogonal axes and subsequent demodulation of the magnetic-resonance frequency. This modulation is provided by the ac Stark shift induced by circularly polarized laser beams. The sensor exhibits a demonstrated rms noise floor of ∼65 fT/√[Hz] in measurement of the field magnitude and 0.5 mrad/√[Hz] in the field direction; elimination of technical noise would improve these sensitivities to 12 fT/√[Hz] and 10 µrad/√[Hz], respectively. Applications for this all-optical vector magnetometer would include magnetically sensitive fundamental physics experiments, such as the search for a permanent electric dipole moment of the neutron.

Cavity-enhanced room-temperature magnetometry using absorption by nitrogen-vacancy centers in diamond.

We demonstrate a cavity-enhanced room-temperature magnetic field sensor based on nitrogen-vacancy centers in diamond. Magnetic resonance is detected using absorption of light resonant with the 1042 nm spin-singlet transition. The diamond is placed in an external optical cavity to enhance the absorption, and significant absorption is observed even at room temperature. We demonstrate a magnetic field sensitivity of 2.5 nT/Hz, and project a photon shot-noise-limited sensitivity of 70 pT/Hz for a few mW of infrared light, and a quantum projection-noise-limited sensitivity of 250 fT/Hz for the sensing volume of ∼90 µm×90 µm×200 µm.