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Alkali-metal-noble-gas comagnetometers are precision probes well-suited for tests of fundamental physics and inertial rotation sensing, combining high sensitivity of the spin-exchange-relaxation free (SERF) magnetometers with inherent suppression of magnetic field noise. Past versions of the device utilizing continuous-wave optical pumping are sensitive to a single axis perpendicular to the plane spanned by the orthogonal pump and probe laser beams. These devices are susceptible to light shifts in the alkali atoms, and to power and beam pointing fluctuations of both the probe and pump lasers, the latter of which is a dominant source of $1/f$ noise. In this work, we model and implement a new approach to alkali-metal-noble-gas comagnetometers using pulsed optical pumping. After each pump laser pulse, an off-resonance probe beam measures the precession of noble-gas-spins-coupled alkali spins via optical rotation in the dark, thus eliminating effects from pump laser light shift and power fluctuations. Performing non-linear fitting on the sinusoidal transient signal with a proper phase enables separate and simultaneous measurement of signals along two orthogonal axes in the plane perpendicular to the pump beam. Effects from beam pointing fluctuations of the probe beam in the pump-probe plane is fundamentally eliminated, and signal response to pump beam pointing fluctuations is suppressed by compensation from noble-gas nuclear spins., Comment: 12 pages, 11 figures

Rydberg atoms have large transition electric dipole moments and high sensitivity to electric fields. We describe a new method for microwave field sensing in a vapor cell consisting of separate excitation, quantum evolution between two Rydberg levels in the dark and state-dependent detection with probe laser transmission. Using microwave pulse techniques we study homogeneous and inhomogeneous relaxation of the coherence between Rydberg levels and demonstrate detection of a 10 GHz signal with electric field sensitivity of 10 nV/cm/Hz$^{1/2}$., Comment: 5 pages, 4 figures

We present a vector atomic magnetometer based on applying a fast-rotating magnetic field to a pulsed $^{87}$Rb scalar atomic magnetometer. This method enables simultaneous measurements of the total magnetic field and two polar angles relative to the plane of magnetic field rotation. Using two channels in a gradiometer mode, it provides simultaneous measurements of the total field gradient with a sensitivity of 35 $\mathrm{fT/\sqrt{Hz}}$ (0.7 part per billion), as well as two polar angles with resolutions of 6 $\mathrm{nrad/\sqrt{Hz}}$ at 50 $\mu$T Earth field strength. The noise spectrums of these measurements are flat down to 1 Hz and 0.1 Hz, respectively. Crucially, this approach avoids several metrological difficulties associated with vector magnetometers and gradiometers. We detail the fundamental, systematic, and practical limits of such vector magnetometers. Notably, we provide a comprehensive study of the systematic effects of vector atomic magnetometers. We introduce a new concept of dynamic heading error and investigate several other systematic effects. A unique peak-altering fast rotating field modulation is proposed to cancel out these systematics. Additionally, we derive fundamental limits on the sensitivity of such sensors and demonstrate that the vector sensitivity of the sensor can approach its scalar sensitivity while retaining the accuracy and metrological advantages of scalar sensors. This high-dynamic-range vector magnetometer, with ultrahigh resolution and inherent calibration, is suitable for a wide array of applications., Comment: 10 pages

Ultralight axion-like particles can contribute to the dark matter near the Sun, leading to a distinct, stochastic signature in terrestrial experiments. We search for such particles through their neutron-spin coupling by re-analyzing approximately 40 days of data from a K-$^3$He co-magnetometer with a new frequency-domain likelihood-based formalism that properly accounts for stochastic effects over all axion coherence times relative to the experimental time span. Assuming that axions make up all of the dark matter in the Sun's vicinity, we find a median 95% upper limit on the neutron-spin coupling of $2.4 \times 10^{-10}$ GeV$^{{-1}}$ for axion masses from 0.4 to 4 feV, which is about five orders of magnitude more stringent than previous laboratory bounds in that mass range. Although several peaks in the experiment's magnetic power spectrum suggest the rejection of a white-noise null hypothesis, further analysis of their lineshapes yields no positive evidence for a dark matter axion., Comment: 25 pages, 15 figures

Indirect spin-spin interactions between nuclei bound in a molecule are well-known in nuclear magnetic resonance, but such interactions between unbound atoms are less well studied and are often assumed to be zero. We present the first precision calculation of this interaction between 129Xe and 3He nuclei in a gas. Relativistic, state-of-the-art electronic structure theory is used to compute the scalar coupling constant J(R) and the interatomic potential energy function, V(R), as functions of the Xe-He internuclear distance R. Using virial expansion we find the nuclear spin enhancement factor kappa = -0.0105 +/- 0.0015 in excellent agreement with recent experiments. This interaction is particularly important for precision measurements using nuclear spin co-magnetometers., Comment: 5 pages, 3 figures, 1 table

We report the results of a new search for long range spin-dependent interactions using a Rb -$^{21}$Ne atomic comagnetometer and a rotatable electron spin source based on a SmCo$_{5}$ magnet with an iron flux return. By looking for signal correlations with the orientation of the spin source we set new constrains on the product of the pseudoscalar electron and neutron couplings $g^e_p g^n_p/\hbar c<1.7\times10^{-14}$ and on the product of their axial couplings $g^e_A g^n_A/\hbar c<5\times10^{-42}$ to a new particle with a mass of less than about $1~\mu$eV. Our measurements improve by about 2 orders of magnitude previous constraints on such spin-dependent interactions., Comment: 4 pages, 4 figures

Very light particles with CP-violating couplings to ordinary matter, such as axions or axion-like particles, can mediate long-range forces between polarized and unpolarized fermions. We describe a new experimental search for such forces between unpolarized nucleons in two 250 kg Pb weights and polarized neutrons and electrons in a $^3$He-K co-magnetometer located about 15 cm away. We place improved constrains on the products of scalar and pseudoscalar coupling constants, $g^n_p g^N_s < 4.2\times10^{-30}$ and $g^e_p g^N_s < 1.7\times10^{-30}$ (95% CL) for axion-like particle masses less than $10^{-6}$ eV, which represents an order of magnitude improvement over the best previous neutron laboratory limit.

Atomic co-magnetometers are widely used in precision measurements searching for spin interactions beyond the Standard Model. We describe a new $^3$He-$^{129}$Xe co-magnetometer probed by Rb atoms and use it to identify two general classes of systematic effects in gas co-magnetometers, one associated with diffusion in second-order magnetic field gradients and another due to temperature gradients. We also develop a general and practical approach for calculating spin relaxation and frequency shifts due to arbitrary magnetic field gradients and confirm it experimentally., Comment: 5 pages, 4 figures

A cosmic scalar field evolving very slowly in time can account for the observed dark energy of the Universe. Unlike a cosmological constant, an evolving scalar field also has local spatial gradients due to gravity. If the scalar field has a minimal derivative coupling to electromagnetism, it will cause modifications of Maxwell's equations. In particular, in the presence of a scalar field gradient generated by Earth's gravity, regions with a magnetic field appear to be electrically charged and regions with a static electric field appear to contain electric currents. We propose experiments to detect such effects with sensitivity exceeding current limits on scalar field interactions from measurements of cosmological birefringence. If the scalar field has derivative couplings to fermions, it would also generate observable effects in precision spin precession experiments., Comment: 5 pages, 3 figures (added two more scenarios to detect interaction, plus references)

A comparison between existing measurements and calculations of the scalar spin-spin interaction (J-coupling) in deuterated molecular hydrogen (HD) yields stringent constraints on anomalous spin-dependent potentials between nucleons at the atomic scale (${\rm \sim 1 \AA}$). The dimensionless coupling constant $g_P^pg_P^{N}/4\pi$ associated with exchange of pseudoscalar (axion-like) bosons between nucleons is constrained to be less than $5\times 10^{-7}$ for boson masses in the range of $5 {\rm keV}$. This represents improvement by a factor of about 100 over constraints placed by measurements of the dipole-dipole interaction in molecular ${\rm H_2}$. The dimensionless coupling constant $g_A^pg_A^N/4 \pi$ associated with exchange of a heretofore undiscovered axial-vector boson between nucleons is constrained to be $g_A^pg_A^N/4 \pi < 2 \times 10^{-19}$ for bosons of mass $\lesssim 1000 {\rm eV}$, improving constraints at this distance scale by a factor of 100 for proton-proton couplings and more than 8 orders of magnitude for neutron-proton couplings. This limit is also a factor of 100 more stringent than recent constraints obtained for axial-vector couplings between electrons and nucleons obtained from comparison of measurements and calculations of hyperfine structure., Comment: 4 pages 2 figures

Nuclear spin optical rotation (NSOR) is a recently developed technique for detection of nuclear magnetic resonance via rotation of light polarization, instead of the usual long-range magnetic fields. NSOR signals depend on hyperfine interactions with virtual optical excitations, giving new information about the nuclear chemical environment. We use a multi-pass optical cell to perform first precision measurements of NSOR signals for a range of organic liquids and find clear distinction between proton signals for different compounds, in agreement with our earlier predictions. Detailed first principles quantum-mechanical NSOR calculations are found to be in good agreement with the measurements., Comment: 4 pages

We discuss nuclear spin comagnetometers based on ultra-low-field nuclear magnetic resonance in mixtures of miscible solvents, each rich in a different nuclear spin. In one version thereof, Larmor precession of protons and ${\rm ^{19}F}$ nuclei in a mixture of thermally polarized pentane and hexafluorobenzene is monitored via a sensitive alkali-vapor magnetometer. We realize transverse relaxation times in excess of 20 s and suppression of magnetic field fluctuations by a factor of 3400. We estimate it should be possible to achieve single-shot sensitivity of about $5\times{\rm 10^{-9} Hz}$, or about $5\times 10^{-11} {\rm Hz}$ in $\approx 1$ day of integration. In a second version, spin precession of protons and ${\rm ^{129}Xe}$ nuclei in a mixture of pentane and hyperpolarized liquid xenon is monitored using superconducting quantum interference devices. Application to spin-gravity experiments, electric dipole moment experiments, and sensitive gyroscopes is discussed., Comment: 5 pages 5 figures

Scalar couplings between covalently bound nuclear spins are a ubiquitous feature in nuclear magnetic resonance (NMR) experiments, imparting valuable information to NMR spectra regarding molecular structure and conformation. Such couplings arise due to a second-order hyperfine interaction, and, in principle, the same mechanism should lead to scalar couplings between nuclear spins in unbound van der Waals complexes. Here, we report the first observation of scalar couplings between nuclei in van der Waals molecules. Our measurements are performed in a solution of hyperpolarized ${\rm ^{129}Xe}$ and pentane, using superconducting quantum interference devices to detect NMR in 10 mG fields, and are in good agreement with calculations based on density functional theory. van der Waals forces play an important role in many physical phenomena, and hence the techniques presented here may provide a new method for probing such interactions., Comment: 7 pages, 4 figures

Electric dipole moments (EDMs) of elementary particles and atoms probe violations of T and P symmetries and consequently of CP if CPT is an exact symmetry. We point out that EDMs can also serve as sensitive probes of CPT-odd, CP-even interactions, that are not constrained by any other existing experiments. Analyzing models with spontaneously broken Lorentz invariance, we calculate EDMs in terms of the leading CPT-odd operators to show that experimental sensitivity probes the scale of CPT breaking as high as 10^{12}GeV., Comment: 4 pages, typos corrected

An experimental nuclear-spin gyroscope is based on an alkali-metal/noblegas co-magnetometer, which automatically cancels the effects of magnetic fields. Whereas the performances of prior nuclear-spin gyroscopes are limited by sensitivity to magnetic fields, this gyroscope is insensitive to magnetic fields and to other external perturbations. In addition, relative to prior nuclear-spin gyroscopes, this one exhibits greater sensitivity to rotation. There is commercial interest in development of small, highly sensitive gyroscopes. The present experimental device could be a prototype for development of nuclear spin gyroscopes suitable for navigation. In comparison with fiber-optic gyroscopes, these gyroscopes would draw less power and would be smaller, lighter, more sensitive, and less costly.