Search

Atomic spectroscopy can be used to search for new bosons that carry exotic forces between elementary fermions. A comparison of a recent precise measurement [Bullis \textit{et al.}, Phys. Rev. Lett. \textbf{130}, 203001 (2023)] of the hyperfine splitting of the 2S$_{1/2}$ electronic levels of hydrogen and up-to-date bound-state quantum electrodynamics theory yields improved constraints on electron-proton exotic interactions of the dimensionless coupling strengths $g_pg_p$ and $g_Ag_A$, corresponding to the exchange of a pseudoscalar (axionlike) or axial-vector boson, respectively., Comment: 2 pages, 2 figures

While it is possible to estimate the dark matter density at the Sun distance from the galactic center, this does not give information on actual dark matter density in the Solar system. There can be considerable local enhancement of dark matter density in the vicinity of gravitating centers, including the Sun, the Earth, as well as other planets in the solar system. Generic mechanisms for the formation of such halos were recently elucidated. In this work, we studies the possible halo dark matter overdensities and corresponding dark matter masses allowed for various objects in the solar system. We explore spacecraft missions to detect such halos with instruments such as quantum clocks, atomic and molecular spectrometers designed to search for fast (tens of hertz to gigahertz) oscillations of fundamental constants, highly sensitive comagnetometers, and other quantum sensors and sensor networks., Comment: 9 pages, 4 figures

Axion-like particles (ALPs) arise from well-motivated extensions to the Standard Model and could account for dark matter. ALP dark matter would manifest as a nearly monochromatic field oscillating at an (as of yet) unknown frequency. The frequency depends on the ALP mass, which could plausibly range from $10^{-22}$ eV/$c^2$ to $10$ eV/$c^2$. We report on a direct search for ALP dark matter through the ALP-nucleon interaction by interfering the signals of two atomic K-Rb-$^3$He comagnetometers, with one situated in Mainz, Germany, and the other in Krak\'ow, Poland. We use the ALP dark matter's spatiotemporal coherence properties assuming the standard halo model of dark matter in the Milky Way to improve the sensitivity and exclude spurious candidates. The search extends over nine orders of magnitude in ALP mass. In this range, no significant evidence of an ALP signal is found. We thus place new upper limits on the ALP-neutron and ALP-proton couplings of $g_{aNN}<10^{-5}$ GeV$^{-1}$ and $g_{aPP}<5 \times 10^{-4}$ GeV$^{-1}$ at a mass of $10^{-22}$ eV/$c^2$ and extending to a mass of $10^{-15}$ eV/$c^2$ where the upper limits reach below $g_{aNN}<10^{-9}$ GeV$^{-1}$ and $g_{aPP}<10^{-7}$ GeV$^{-1}$, respectively. For both neutron and proton couplings, this work is an improvement of up to four orders of magnitude compared to previous laboratory constraints.

We report the first experimental demonstration of stimulated Raman adiabatic passage (STIRAP) in nuclear-spin transitions of $^{14}$N within nitrogen-vacancy (NV) color centers in diamond. It is shown that the STIRAP technique suppresses the occupation of the intermediate state, which is a crucial factor for improvements in quantum sensing technology. Building on that advantage, we develop and implement a generalized version of the Ramsey interferometric scheme, employing half-STIRAP pulses to perform the necessary quantum-state manipulation with high fidelity. The enhanced robustness of the STIRAP-based Ramsey scheme to variations in the pulse parameters is experimentally demonstrated, showing good agreement with theoretical predictions. Our results pave the way for improving the long-term stability of diamond-based sensors, such as gyroscopes and frequency standards., Comment: 11 pages, 7 figures

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 features width and contrast of the feature on the size of the diamond (in the range 30 nm to 3 um) 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., Comment: 9 pages, 5 figures

A quantum limit on the measurement of magnetic field has been recently pointed out, stating that the so-called Energy Resolution $E_\mathrm{R}$ is bounded to $E_\mathrm{R} \gtrsim \hbar$. This limit holds indeed true for the vast majority of existing quantum magnetometers, including SQUIDs, solid state spins and optically pumped atomic magnetometers. However, it can be surpassed by highly correlated spin systems, as recently demonstrated with a single-domain spinor Bose-Einstein Condensate. Here we show that similar and potentially much better resolution can be achieved with a hard ferromagnet levitated above a superconductor at cryogenic temperature. We demonstrate $E_\mathrm{R}=\left( 0.064 \pm 0.010 \right) \, \hbar$ and anticipate that $E_\mathrm{R}<10^{-3} \, \hbar$ is within reach with near-future improvements. This finding opens the way to new applications in condensed matter, biophysics and fundamental science. In particular, we propose an experiment to search for axionlike dark matter and project a sensitivity orders of magnitude better than in previous searches., Comment: 26 pages, 8 figures (including Supplementary Information)

This paper presents a new technique to study the adsorption and desorption of ions and electrons on insulating surfaces in the presence of strong electric fields in cryoliquids. The experimental design consists of a compact cryostat coupled with a sensitive electro-optical Kerr device to monitor the stability of the electric fields. The behavior of nitrogen and helium ions on a poly(methyl methacrylate) (PMMA) surface was compared to a PMMA surface coated with a mixture of deuterated polystyrene and deuterated polybutadiene. Ion accumulation and removal on these surfaces were unambiguously observed. Within the precision of the data, both surfaces behave similarly for the physisorbed ions. The setup was also used to measure the (quasi-)static dielectric constant of PMMA at T = 70 K. The impact of the ion adsorption on the search for a neutron permanent electric dipole moment in a cryogenic environment, like the nEDM@SNS experiment, is discussed.

A wide-field magnetometer utilizing nitrogen-vacancy (NV) centers in diamond that does not require microwaves is demonstrated. It is designed for applications where microwaves need to be avoided, such as magnetic imaging of biological or conductive samples. The system exploits a magnetically sensitive feature of NV centers near the ground state level anticrossing (GSLAC). An applied test field from a wire was mapped over an imaging area of $\approx 500 \times 470\,{\mu}\text{m}^2$. Analysis of the GSLAC lineshape allows to extract vector information of the applied field. The device allows micrometer-scale magnetic imaging at a spatial resolution dominated by the thickness of the NV layer (here $50\,{\mu}\text{m}$). For a pixel size of $4\,{\mu}\text{m} \times 3.8\,{\mu}\text{m}$ the estimated sensitivity is $4.8\,{\mu}\text{T}/\sqrt{\text{Hz}}$. Two modalities for visualizing the magnetic fields, static and temporal, are presented along with a discussion of technical limitations and future extensions of the method., Comment: 8 pages,6 figures

Experiments aimed at detecting ultralight dark matter typically rely on resonant effects, which are sensitive to the dark matter mass that matches the resonance frequency. In this study, we investigate the nucleon couplings of ultralight axion dark matter using a magnetometer operating in a nuclear magnetic resonance (NMR) mode. Our approach involves the use of a $^{21}$Ne spin-based sensor, which features the lowest nuclear magnetic moment among noble-gas spins. This configuration allows us to achieve an ultrahigh sensitivity of 0.73 fT/Hz$^{1/2}$ at around 5 Hz, corresponding to energy resolution of approximately 1.5$\times 10^{-23}\,\rm{eV/Hz^{1/2}}$. Our analysis reveals that under certain conditions it is beneficial to scan the frequency with steps significantly larger than the resonance width. The analytical results are in agreement with experimental data and the scan strategy is potentially applicable to other resonant searches. Further, our study establishes stringent constraints on axion-like particles (ALP) in the 4.5--15.5 Hz Compton-frequency range coupling to neutrons and protons, improving on prior work by several-fold. Within a band around 4.6--6.6 Hz and around 7.5 Hz, our laboratory findings surpass astrophysical limits derived from neutron-star cooling. Hence, we demonstrate an accelerated resonance search for ultralight dark matter, achieving an approximately 30-fold increase in scanning step while maintaining competitive sensitivity., Comment: 13 pages, 11 figures, accepted by Communications Physics

Sensitive magnetometers have been applied in a wide range of research fields, including geophysical exploration, bio-magnetic field detection, ultralow-field nuclear magnetic resonance, etc. Commonly, magnetometers are directly placed at the position where the magnetic field is to be measured. However, in some situations, for example in near space or harsh environments, near nuclear reactors or particle accelerators, it is hard to place a magnetometer directly there. If the magnetic field can be detected remotely, i.e., via stand-off detection, this problem can be solved. As optical magnetometers are based on optical readout, they are naturally promising for stand-off detection. We review various approaches to optical stand-off magnetometry proposed and developed over the years, culminating in recent results on measuring magnetic fields in the mesosphere using laser guide stars, magnetometry with mirrorless-lasing readout, and proposals for satellite-assisted interrogation of atmospheric sodium., Comment: 68 pages, 19 figures

We propose and demonstrate a general method to calibrate the frequency-dependent response of self-compensating noble-gas-alkali-metal comagnetometers to arbitrary spin perturbations. This includes magnetic and nonmagnetic perturbations like rotations and exotic spin interactions. The method is based on a fit of the magnetic field response to an analytical model. The frequency-dependent response of the comagnetometer to arbitrary spin perturbations can be inferred using the fit parameters. We demonstrate the effectiveness of this method by comparing the inferred rotation response to an experimental measurement of the rotation response. Our results show that experiments relying on zero-frequency calibration of the comagnetometer response can over- or under-estimate the comagnetometer sensitivity by orders of magnitude over a wide frequency range. Moreover, this discrepancy accumulates over time as operational parameters tend to drift during comagnetometer operation. The demonstrated calibration protocol enables accurate prediction and control of comagnetometer sensitivity to, for example, ultralight bosonic dark-matter fields coupling to electron or nuclear spins as well as accurate monitoring and control of the relevant system parameters.

The sensitivity and accessible mass range of magnetic resonance searches for axionlike dark matter depends on the homogeneity of applied magnetic fields. Optimizing homogeneity through shimming requires exploring a large parameter space which can be prohibitively time consuming. We have automated the process of tuning the shim-coil currents by employing an algorithm based on Bayesian optimization. This method is especially suited for applications where the duration of a single optimization step prohibits exploring the parameter space extensively or when there is no prior information on the optimal operation point. Using the Cosmic Axion Spin Precession Experiment (CASPEr)-gradient low-field apparatus, we show that for our setup this method converges after approximately 30 iterations to a sub-10 parts-per-million field homogeneity which is desirable for our dark matter search.

Galactic dark matter may consist of axionlike particles (ALPs) that can be described as an "ultralight bosonic field" oscillating at the ALP Compton frequency. The ALP field can be searched for using nuclear magnetic resonance (NMR), where resonant precession of spins of a polarized sample can be sensitively detected. The ALP mass to which the experiment is sensitive is scanned by sweeping the bias magnetic field. The scanning either results in detection of ALP dark matter or rules out ALP dark matter with sufficiently strong couplings to nuclear spins over the range of ALP masses corresponding to the covered span of Larmor frequencies. In this work, scanning strategies are analyzed with the goal of optimizing the parameter-space coverage via a proper choice of experimental parameters (e.g., the effective transverse relaxation time).

Quantum sensing is a fundamental building block of modern technology that employs quantum resources and creates new opportunities for precision measurements. However, previous methods usually have a common assumption that detection noise levels should be below the intrinsic sensitivity provided by quantum resources. Here we report the first demonstration of Fano resonance between coupled alkali-metal and noble gases through rapid spin-exchange collisions. The Fano resonance gives rise to two intriguing phenomena: spin amplification and deamplification, which serve as crucial resources for enhanced sensing. Further we develop a novel scheme of quantum sensing enhanced by amplification and deamplification, with relaxed requirements on the detection noise. The coupled systems of alkali-metal and noble gases act as amplifiers or de-amplifiers, enabling to extract small signals above the detection noise before final detection. We demonstrate magnetic-field measurement about 54 decibels below the photon-shot noise, which outperforms the state-of-the-art squeezed-light technology and realizes femtotesla-level sensitivity. Our work opens new avenues to applications in searches for ultralight dark matter with sensitivity well beyond the supernova-observation constraints., Comment: 7 pages, 4 figures

As promising quantum sensors, nitrogen-vacancy (NV) centers in diamond have been widely used in frontier studies in condensed matter physics, material sciences, and life sciences. In practical applications, weak laser excitation is favorable as it reduces the side effects of laser irradiation, for example, phototoxicity and heating. Here we report a combined theoretical and experimental study of optically detected magnetic resonance (ODMR) of NV-center ensembles under weak 532-nm laser excitation. In this regime, both the width and splitting of ODMR spectra decrease with increasing laser power. This power dependence is reproduced with a model considering laser-induced charge neutralization of NV--N+ pairs, which alters the local electric field environment. These results are important for understanding and designing NV-based quantum sensing in light-sensitive applications.

Mirrorless lasing has been a topic of particular interest for about a decade due to promising new horizons for quantum science and applications. In this work, we review first-principles theory that describes this phenomenon, and discuss degenerate mirrorless lasing in a vapor of Rb atoms, the mechanisms of amplification of light generated in the medium with population inversion between magnetic sublevels within the $D_2$ line, and challenges associated with experimental realization.

The combination of a powerful and broadly applicable nuclear hyperpolarization technique with emerging (near-)zero-field modalities offer novel opportunities in a broad range of nuclear magnetic resonance spectroscopy and imaging applications, including biomedical diagnostics, monitoring catalytic reactions within metal reactors and many others. These are discussed along with a roadmap for future developments., Comment: 12 pages, 5 figures

As-yet undiscovered light bosons may constitute all or part of the dark matter (DM) of our Universe, and are expected to have (weak) self-interactions. We show that the quartic self-interactions generically induce the capture of dark matter from the surrounding halo by external gravitational potentials such as those of stars, including the Sun. This leads to the subsequent formation of dark matter bound states supported by such external potentials, resembling gravitational atoms (e.g. a solar halo around our own Sun). Their growth is governed by the ratio $\xi_{\rm foc} \equiv \lambda_{\rm dB}/R_\star$ between the de Broglie wavelength of the incoming DM waves, $\lambda_{\rm dB}$, and the radius of the ground state $R_\star$. For $\xi_{\rm foc}\lesssim 1$, the gravitational atom grows to an (underdense) steady state that balances the capture of particles and the inverse (stripping) process. For $\xi_{\rm foc}\gtrsim 1$, a significant gravitational-focusing effect leads to exponential accumulation of mass from the galactic DM halo into the gravitational atom. For instance, a dark matter axion with mass of the order of $10^{-14}$ eV and decay constant between $10^{7}$ and $10^8$ GeV would form a dense halo around the Sun on a timescale comparable to the lifetime of the Solar System, leading to a local DM density at the position of the Earth $\mathcal{O}(10^4)$ times larger than that expected in the standard halo model. For attractive self-interactions, after its formation, the gravitational atom is destabilized at a large density, which leads to its collapse; this is likely to be accompanied by emission of relativistic bosons (a `Bosenova')., Comment: 39 pages + appendices, 21 figures. For convenience we summarize the basic mechanism and results in Section 2

Observational evidence suggests the existence of dark matter (DM), which comprises approximately $84.4\%$ of matter in the universe. Recent advances in tabletop quantum sensor technology have enabled searches for nongravitational interactions of DM. Our experiment named ChangE utilizes Coupled Hot Atom eNsembles to search for liGht dark mattEr and new physics. We identify a strongly-coupled hybrid spin-resonance (HSR) regime that enhances the bandwidth of $^{21}$Ne nuclear spin by three orders of magnitude while maintaining high sensitivity. In combination with a self-compensating mode (SC) for low frequencies, we present a comprehensive broadband search for axion-like dark matter with Compton frequencies in the range of $[0.01, 1000]$ Hz. We set new constraints on the DM interactions with neutrons and protons, accounting for the stochastic effect. For the axion-neutron coupling, our results reach a low value of $|g_{ann}|\le 3\times 10^{-10}$ in the frequency range $[0.02 , 4]$ Hz surpassing astrophysical limits and provide the strongest laboratory constraints in the $[10, 100]$ Hz range. For the axion-proton coupling, we offer the best terrestrial constraints for the frequency below 100 Hz., Comment: 14 pages, 5 figures

Stimulated Raman Adiabatic Passage (STIRAP) is a widely used method for adiabatic population transfer in a multilevel system. In this work, we study STIRAP under novel conditions and focus on the fractional, F-STIRAP, which is known to create a superposition state with the maximum coherence. In both configurations, STIRAP and F-STIRAP, we implement pulse chirping aiming at a higher contrast, a broader range of parameters for adiabaticity, and enhanced spectral selectivity. Such goals target improvement of quantum imaging, sensing and metrology, and broaden the range of applications of quantum control techniques and protocols. In conventional STIRAP and F-STIRAP, two-photon resonance is required conceptually to satisfy the adiabaticity condition for dynamics within the dark state. Here, we account for a non-zero two-photon detuning and present control schemes to achieve the adiabatic conditions in STIRAP and F-STIRAP through a skillful compensation of the two-photon detuning by pulse chirping. We show that the chirped configuration - C-STIRAP - permits adiabatic passage to a predetermined state among two nearly degenerate final states, when conventional STIRAP fails to resolve them. We demonstrate such a selectivity within a broad range of parameters of the two-photon detuning and the chirp rate. In the C-F-STIRAP, chirping of the pump and the Stokes pulses with different time delays permits a complete compensation of the two-photon detuning and results in a selective maximum coherence of the initial and the target state with higher spectral resolution than in the conventional F-STIRAP.

Molecules containing short-lived, radioactive nuclei are uniquely positioned to enable a wide range of scientific discoveries in the areas of fundamental symmetries, astrophysics, nuclear structure, and chemistry. Recent advances in the ability to create, cool, and control complex molecules down to the quantum level, along with recent and upcoming advances in radioactive species production at several facilities around the world, create a compelling opportunity to coordinate and combine these efforts to bring precision measurement and control to molecules containing extreme nuclei. In this manuscript, we review the scientific case for studying radioactive molecules, discuss recent atomic, molecular, nuclear, astrophysical, and chemical advances which provide the foundation for their study, describe the facilities where these species are and will be produced, and provide an outlook for the future of this nascent field.

We propose a highly efficient and fast method of translational cooling for high-angular-momentum atoms. Optical pumping and stimulated transitions, combined with magnetic forces, can be used to compress phase-space density, and the efficiency of each compression step increases with the angular momentum. Entropy is removed by spontaneously emitted photons, and particle number is conserved. This method may be an attractive alternative to evaporative cooling of atoms and possibly molecules in order to produce quantum degenerate gases., Comment: 12 pages, 8 figures

We show that coupling of ultralight dark matter (UDM) to quarks and gluons would lead to an oscillation of the nuclear charge radius for both the quantum chromodynamics (QCD) axion and scalar dark matter. Consequently, the resulting oscillation of electronic energy levels could be resolved with optical atomic clocks, and their comparisons can be used to investigate UDM-nuclear couplings, which were previously only accessible with other platforms. We demonstrate this idea using the ${}^2S_{1/2} (F=0)\leftrightarrow {}^2F_{7/2} (F=3)$ electric octupole and ${}^2S_{1/2} (F=0)\leftrightarrow \,{}^2D_{3/2} (F=2)$ electric quadrupole transitions in ${}^{171}Yb^+$. Based on the derived sensitivity coefficients for these two transitions and a long-term comparison of their frequencies using a single trapped ${}^{171}Yb^+$ ion, we find bounds on the scalar UDM-nuclear couplings and the QCD axion decay constant. These results are at a similar level compared to the tightest spectroscopic limits, and future investigations, also with other optical clocks, promise significant improvements., Comment: 6+3 pages, 2 figures

We study cross-relaxation features near zero magnetic field with ensembles of nitrogen-vacancy (NV) centers in diamond and examine their properties in samples with a range (0.9 ppm - 16.0 ppm) of NV concentrations. The observed NV-NV cross-relaxation features between differently oriented NV centers in high (greater than 0.9 ppm)-NV-density samples hold promise for a variety of magnetometry applications where microwave fields (or any bias field) disturb the system under study. We theoretically determine the values of the bias magnetic fields corresponding to cross-relaxations between different axes and experimentally validate them. The behavior of zero-field cross-relaxation features as a function of temperature is also investigated., Comment: 8 pages, 7 figures, 1 table

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 read-out based measurements of for instance magnetic and electric fields, pressure, temperature and rotations.

Efficient initialization and manipulation of quantum states is important for numerous applications and it usually requires the ability to perform high fidelity and robust swapping of the populations of quantum states. Stimulated Raman adiabatic passage (STIRAP) has been known to perform efficient and robust inversion of the ground states populations of a three-level system. However, its performance is sensitive to the initial state of the system. In this contribution we demonstrate that a slight modification of STIRAP, where we introduce a non-zero single-photon detuning, allows for efficient and robust population swapping for any initial state. The results of our work could be useful for efficient and robust state preparation, dynamical decoupling and design of quantum gates in ground state qubits via two-photon interactions.

We measure electron and nuclear spin transition frequencies in the ground state of nitrogen-vacancy (NV) centers in diamond for two nitrogen isotopes ($^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$) over temperatures ranging from 77 K to 400 K. Measurements are performed using Ramsey interferometry and direct optical readout of the nuclear and electron spins. We extract coupling parameters $Q$ (for $^{14}\mathrm{NV}$), $D$, $A_{||}$, $A_{\perp}$, $\gamma_e/\gamma_n$, and their temperature dependences for both isotopes. The temperature dependences of the nuclear-spin transitions within the $m_s = 0$ spin manifold near room temperature are found to be +0.52(1) ppm/K for $^{14}\mathrm{NV}$ ($|m_I=-1> \leftrightarrow |m_I=+1>$) and -1.1(1) ppm/K for $^{15}\mathrm{NV}$ ($|m_I=-1/2> \leftrightarrow |m_I=+1/2>$). An isotopic shift in the zero-field splitting parameter $D$ between $^{14}\mathrm{NV}$ and $^{15}\mathrm{NV}$ is measured to be $\sim$ 120 kHz. Residual transverse magnetic fields are observed to shift the nuclear spin transition frequencies, especially for $^{15}\mathrm{NV}$. We have precisely determined the set of parameters relevant for the development of nuclear-spin-based diamond quantum sensors with greatly reduced sensitivity to environmental factors., Comment: 12 pages, 7 figures

A chirped-pulse quantum control scheme applicable to Coherent Anti-Stokes Raman Scattering spectroscopy, named as C-CARS, is presented aimed at maximizing the vibrational coherence in molecules. It implies chirping of three incoming pulses in the four-wave mixing process of CARS, the pump, the Stokes and the probe, to fulfil the conditions of adiabatic passage. The scheme is derived in the framework of rotating wave approximation and adiabatic elimination of excited state manifold simplifying the four-level model system into a ``super-effective'' two level system. The robustness, spectral selectivity and adiabatic nature of this method are helpful in improving the existing methods of CARS spectroscopy for sensing, imaging and detection. We also show that the selectivity of excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses.

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\times10^{-17}-8.3\times10^{-13} $ eV and quadratic interactions between a pseudoscalar UBDM field and SM fields in the range $5\times10^{-18}- 4.1\times10^{-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.

An experiment utilizing a TlF molecular beam is being developed by the CeNTREX collaboration to search for hadronic interactions that violate both time-reversal (T) and parity (P) invariance. Here we propose to use the same beam to look for a T-invariance conserving but P-nonconserving (PNC) effect induced by the anapole moment of the Tl nucleus, via a vector coupling of the two nuclear spins in TlF. To measure the nuclear anapole moment, the dc electric and magnetic fields in CeNTREX are replaced by rf fields resonant with a nuclear spin flip transition. We adapt the relativistic coupled cluster method in a combination with relativistic density functional theory for the calculation of the molecular PNC spin-spin vector coupling constant that links the experimental signal with the anapole moment. The value of the P-conserving spin-spin coupling constant calculated within the same approach is found to be in good agreement with available experimental data.

The field of magnetic resonance imaging with hyperpolarized contrast agents is rapidly expanding, and parahydrogen-induced polarization (PHIP) is emerging as an inexpensive and easy-to-implement method for generating the required hyperpolarized biomolecules. Hydrogenative PHIP delivers hyperpolarized proton spin order to a substrate via chemical addition of H2 in the spin-singlet state, but prior to imaging it is typically necessary to transfer the proton polarization to a heteronucleus (usually 13C) in the molecule. Adiabatic ultralow magnetic field manipulations can be used to induce the polarization transfer, but this is necessarily a slow process, which is undesirable since the spins continually relax back to thermal equilibrium. Here we demonstrate constant-adiabaticity field cycling and field sweeping for optimal polarization transfer on a model AA$'$X spin system, [1-13C]fumarate. We introduce a method for calculating constant-adiabaticity magnetic field ramps and demonstrate that they enable much faster spin-order conversion as compared to linear ramps used before. The present method can thus be utilized to manipulate nonthermal order in heteronuclear spin systems.

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 $3\times10^{-8}$\,rad/s/Hz$^{1/2}$ in the frequency range from 0.2 to 1.0 Hz, which is equivalent to the energy resolution of $3.1\times 10^{-23}$\,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 four orders of magnitude.

Self-compensated comagnetometers, employing overlapping samples of spin-polarized alkali and noble gases (for example K-$^3$He) are promising sensors for exotic beyond-the-standard-model fields and high-precision metrology such as rotation sensing. When the comagnetometer operates in the so-called self-compensated regime, the effective field, originating from contact interactions between the alkali valence electrons and the noble-gas nuclei, is compensated with an applied magnetic field. When the comagnetometer begins operation in a given magnetic field, spin-exchange optical pumping establishes equilibrium between the alkali electron-spin polarization and the nuclear-spin polarization. Subsequently, when the magnetic field is tuned to the compensation point, the spin polarization is brought out of the equilibrium conditions. This causes a practical issue for long measurement times. We report on a novel method for closed-loop control of the compensation field. This method allows optimization of the operating parameters, especially magnetic field gradients, in spite of the inherently slow (hours to days) dynamics of the system. With the optimization, higher stable nuclear polarization, longer relaxation times and stronger electron-nuclear coupling are achieved which is useful for nuclear-spin-based quantum memory, spin amplifiers and gyroscopes. The optimized sensor demonstrates a sensitivity comparable to the best previous comagnetometer but with four times lower noble gas density. This paves the way for applications in both fundamental and applied science.

$^{229}$Th with a low-lying nuclear isomeric state is an essential candidate for a nuclear clock as well as many other applications. Laser excitation of the isomeric state has been a long-standing goal. With relativistic $^{229}$Th ions in storage rings, high-power lasers with wavelengths in the visible range or longer can be used to achieve high excitation rates of $^{229}$Th isomers. This can be realized through direct resonant excitation, or excitation via an intermediate nuclear or electronic state, facilitated by the tunability of both the laser-beam and ion-bunch parameters. Unique opportunities are offered by highly charged $^{229}$Th ions due to the nuclear-state mixing. The significantly reduced isomeric-state lifetime corresponds to a much higher excitation rate for direct resonant excitation. Importantly, we propose electric dipole transitions changing both the electronic and nuclear states that are opened by the nuclear hyperfine mixing. We suggest using them for efficient isomer excitation in Li-like $^{229}$Th ions, via stimulated Raman adiabatic passage or single-laser excitation. We also propose schemes for probing the isomers, utilizing nuclear radiative decay or laser spectroscopy on electronic transitions, through which the isomeric-state energy can be determined with an orders-of-magnitude higher precision than the current value. The schemes proposed here for $^{229}$Th could also be adapted to low-energy nuclear states in other nuclei, such as $^{229}$Pa., Comment: 20+7 pages, 12 figures

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 ten orders of magnitude improvement than previous works.

State-of-the-art magnetic resonance imaging uses hyperpolarized molecules to track metabolism in vivo, but large superconducting magnets are required, and the strong magnetic fields largely preclude measurement in the presence of conductive materials and magnify problems of magnetic susceptibility inhomogeneity. Operating at zero and low field circumvents these limitations, but until now has not been possible due to limited sensitivity. We show that zero- and low-field nuclear magnetic resonance can be used for probing two important metabolic reactions: the conversion of hyperpolarized fumarate to malate and pyruvate to lactate. This work paves the way to a heretofore unexplored class of biomedical imaging applications., Comment: 10 pages, 7 figures

Quantum sensing provides sensitive tabletop tools to search for exotic spin-dependent interactions beyond the Standard Model, which has attracted great attention in theories and experiments. Here we develop a technique based on quantum Spin Amplifier for Particle PHysIcs REsearch (SAPPHIRE) to resonantly search for exotic interactions, specifically parity-odd spin-spin interactions. The present technique effectively amplifies the pseudomagnetic field generated by exotic interactions by a factor of about 200 while being insensitive to spurious external magnetic fields. Our studies, using such a quantum amplification technique, open the doors to exploring the parity-violation interactions mediated by Z' bosons in the challenging parameter space (force range between 3 mm and 0.1 km) and set the most stringent constraints on Z'-mediated electron-neutron couplings, significantly improving previous limits by up to five orders of magnitude. Moreover, our bounds on Z'-mediated couplings between nucleons reaches into a hitherto unexplored parameter space (force range below 1 m), complementing the existing astrophysical and laboratory studies., Comment: 8 pages, 5 figures

We describe a proposal to search for an intrinsic electric dipole moment (EDM) of the proton with a sensitivity of \targetsens, based on the vertical rotation of the polarization of a stored proton beam. The New Physics reach is of order $10^~3$TeV mass scale. Observation of the proton EDM provides the best probe of CP-violation in the Higgs sector, at a level of sensitivity that may be inaccessible to electron-EDM experiments. The improvement in the sensitivity to $\theta_{QCD}$, a parameter crucial in axion and axion dark matter physics, is about three orders of magnitude.

We present a concept for a high-precision optical atomic clock (OAC) operating on an Earth-orbiting space station. This pathfinder science mission will compare the space-based OAC with one or more ultra-stable terrestrial OACs to search for space-time-dependent signatures of dark scalar fields that manifest as anomalies in the relative frequencies of station-based and ground-based clocks. This opens the possibility of probing models of new physics that are inaccessible to purely ground-based OAC experiments where a dark scalar field may potentially be strongly screened near Earth's surface. This unique enhancement of sensitivity to potential dark matter candidates harnesses the potential of space-based OACs., Comment: Submitted to Quantum Sci. Technol. special issue: Cold atom in space

Motivated by the challenge of identifying intruder ions in a cold ion crystal, we investigate calorimetry from emitted fluorescence light. Under continuous Doppler cooling, the ion crystal reaches a temperature equilibrium with a fixed level of fluorescence intensity and any change in the motional energy of the crystal results in a modification of this intensity. We theoretically determine the fluorescence rate of an ion crystal as a function of the temperature, assuming that laser light is scattered along a two-level electronic transition, which couples to the crystal's vibrations via the mechanical effects of light. We analyze how the heat dissipated by collisions of an incoming intruder ion alters the scattering rate. We argue that an energy change by an incoming $^{229}$Th$^{10+}$ ion can be unambiguously detected within 100 $\mu$s via illuminating a fraction of a 10$^{3}$ ion crystal. This method enables applications including capture and spectroscopy of charged states of thorium isotopes and investigation of highly charged ions., Comment: 10 pages, 4 figures

Alkali-metal atomic magnetometry is widely used due to its high sensitivity and cryogen-free operation. However, when operating in geomagnetic field, it suffers from heading errors originating from nonlinear Zeeman (NLZ) splittings and magnetic resonance asymmetries, which lead to difficulties in mobile-platform measurements. We demonstrate an alignment based $^{87}$Rb magnetometer, which, with only a single magnetic resonance peak and well-separated hyperfine transition frequencies, is insensitive or even immune to NLZ-related heading errors. It is shown that the magnetometer can be implemented for practical measurements in the geomagnetic environments and the photon-shot-noise-limited sensitivity reaches $9\,{\rm{fT}}/\sqrt{\rm{Hz}}$ at room temperature., Comment: 8 pages, 5 figures

We consider possible extensions to quantum mechanics proposed by Steven Weinberg, and re-analyze his prediction of a new test based upon three atomic clocks in the same atom. We propose realistic experimental systems where this hypothesis can be tested. Two systems already set limits on deviations from quantum mechanics, while with another system, one would be able to search for new physics at the limit of sensitivity of the best atomic clocks., Comment: 4 pages, 3 figures

High-energy physics is primarily concerned with uncovering the laws and principles that govern nature at the fundamental level. Research in this field usually relies on probing the boundaries of established physics, an undertaking typically associated with extreme energy and distance scales. It is therefore unsurprising that particle physics has traditionally been dominated by large-scale experimental methods often involving high energies, such as colliders and storage rings, cosmological and astrophysical observations, large-volume detector systems, etc. However, high-sensitivity measurements in smaller experiments, often performed at lower energies, are presently experiencing a surge in importance for particle physics for at least two reasons. First, they exploit synergies to adjacent areas of physics with recent advances in experimental techniques and technology. Together with intensified phenomenological explorations, these advances have led to the realization that challenges associated with weak couplings or the expected suppression factors for new physics can be overcome with such methods while maintaining a large degree of experimental control. Second, many of these measurements broaden the range of particle-physics phenomena and observables relative to the above set of more conventional methodologies. Combining such measurements with the conventional efforts above therefore casts both a wider and tighter net for possible effects originating from physics beyond the Standard Model (BSM). This paper argues that this assessment points at a growing impact of such methods and measurements on high-energy physics, and therefore warrants direct support as particle-physics research. Leveraging the recent rapid progress and bright outlook associated with such studies for high-energy physics, could yield high returns, but requires substantial and sustained efforts by funding agencies., Comment: Contribution to Snowmass 2021, 55 pages, 5 figures

The applications of spin-based quantum sensors to measurements probing fundamental physics are surveyed. Experimental methods and technologies developed for quantum information science have rapidly advanced in recent years, and these tools enable increasingly precise control and measurement of spin dynamics. Theories of beyond-the-Standard-Model physics predict, for example, symmetry violating electromagnetic moments aligned with particle spins, exotic spin-dependent forces, coupling of spins to ultralight bosonic dark matter fields, and changes to the local environment that affect spins. Spin-based quantum sensors can be used to search for these myriad phenomena, and offer a methodology for tests of fundamental physics that is complementary to particle colliders and large scale particle detectors. Areas of technological development that can significantly enhance the sensitivity of spin-based quantum sensors to new physics are highlighted., Comment: contribution to Snowmass 2021, 23 pages, 4 figures; updated references and corrected typos

Static electric dipole moments of nondegenerate systems probe mass scales for physics beyond the Standard Model well beyond those reached directly at high energy colliders. Discrimination between different physics models, however, requires complementary searches in atomic-molecular-and-optical, nuclear and particle physics. In this report, we discuss the current status and prospects in the near future for a compelling suite of such experiments, along with developments needed in the encompassing theoretical framework., Comment: Contribution to Snowmass 2021; updated with community edits and endorsements

The expansion of our Universe is accelerating, due to dark energy. But the nature of dark energy has been a mystery since its discovery at the end of the past century. In Research Highlight https://doi.org/10.1002/ntls.20220003 , Justin Albert, Dmitry Budker and Hossein Sadeghpour provide an overview of how a laser photometric ratio star (a novel light source generated by laser excitation of the Earth's upper-atmospheric sodium layer, which will radiate equally brightly at wavelengths of 589 nm and 820 nm) can help us precisely calibrate telescopes in order to understand the nature of dark energy., Comment: Brief "Research Highlight" and cover article for Natural Sciences journal volume 2, issue 2 (Feb. 2022). 3 pages, 2 figures

Experimental searches for new, "fifth" forces are attracting a lot of attention because they allow to test theoretical extensions to the standard model. Here, we report a new experimental search for possible fifth forces, specifically spin-and-velocity dependent forces, by using a K-Rb-$^{21}$Ne co-magnetometer and a tungsten ring featuring a high nucleon density. Taking advantage of the high sensitivity of the co-magnetometer, the pseudomagnetic field from the fifth force is measured to be $<7$\,aT. This sets new limits on coupling constants for the neutron-nucleon and proton-nucleon interactions in the range of $\ge 0.1$ m. The coupling constant limits are established to be $|g_V^n|<6.6\times 10^{-11}$ and $|g_V^p|<3.0\times 10^{-10}$, which are more than one order of magnitude tighter than astronomical and cosmological limits on the coupling between the new gauge boson such as Z$'$ and standard model particles.

We present a comparative analysis of urban magnetic fields between two American cities: Berkeley (California) and Brooklyn Borough of New York City (New York). Our analysis uses data taken over a four-week period during which magnetic field data were continuously recorded using a fluxgate magnetometer of 70 pT/$\sqrt{\mathrm{Hz}}$ sensitivity. We identified significant differences in the magnetic signatures. In particular, we noticed that Berkeley reaches a near-zero magnetic field activity at night whereas magnetic activity in Brooklyn continues during nighttime. We also present auxiliary measurements acquired using magnetoresistive vector magnetometers (VMR), with sensitivity of 300 pT/$\sqrt{\mathrm{Hz}}$, and demonstrate how cross-correlation, and frequency-domain analysis, combined with data filtering can be used to extract urban magnetometry signals and study local anthropogenic activities. Finally, we discuss the potential of using magnetometer networks to characterize the global magnetic field of cities and give directions for future development., Comment: 8 pages, 7 figures