PHYSICAL REVIEW LETTERS 130, 201401 (2023)

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Search for Spin-Dependent Gravitational Interactions at Earth Range

S.-B. Zhang,1 Z.-L. Ba,1 D.-H. Ning,1 N.-F. Zhai,2 Z.-T. Lu ,1,3,* and D. Sheng 2,3,†
1
CAS Center for Excellence in Quantum Information and Quantum Physics, School of Physical Sciences,
University of Science and Technology of China, Hefei 230026, China
2
Department of Precision Machinery and Precision Instrumentation,
Key Laboratory of Precision Scientific Instrumentation of Anhui Higher Education Institutes,
University of Science and Technology of China, Hefei 230027, China
3
Hefei National Laboratory, University of Science and Technology of China, Hefei 230088, China
(Received 23 January 2023; revised 6 March 2023; accepted 15 March 2023; published 15 May 2023)

Among the four fundamental forces, only gravity does not couple to particle spins according to the
general theory of relativity. We test this principle by searching for an anomalous scalar coupling between
the neutron spin and the Earth’s gravity on the ground. We develop an atomic gas comagnetometer to
measure the ratio of nuclear spin-precession frequencies between 129Xe and 131Xe, and search for a change
of this ratio to the precision of 10−9 as the sensor is flipped in Earth’s gravitational field. The null results of
this search set an upper limit on the coupling energy between the neutron spin and the gravity on the ground
at 5.3 × 10−22 eV (95% confidence level), resulting in a 17-fold improvement over the previous limit. The
results can also be used to constrain several other anomalous interactions. In particular, the limit on the
coupling strength of axion-mediated monopole-dipole interactions at the range of Earth’s radius is
improved by a factor of 17.

DOI: 10.1103/PhysRevLett.130.201401

Among the four fundamental forces, the electromag- Coupling between the 1051 nucleons of Earth and spins in
netic, the strong, and the weak interactions are all depen- the laboratory is a form of monopole-dipole interaction at
dent on particle spins according to the standard model of Earth range [6]. Such an interaction can be mediated by
particle physics, only the gravitational interaction is spin ultralight, axionlike, scalar bosons, which are candidates
independent according to the general theory of relativity. for cold dark matter in the Universe [7]. For two particles a
This principle should be tested experimentally with ever (monopole coupling, mass) and b (dipole coupling, spin),
increasing precision [1]. At the same time, searches for spin- the monopole-dipole interaction can be written as [6,8,9]
gravity coupling also test the fundamental symmetries of the  
gravitational interaction, since such coupling would break ℏ gas gbp 1 1 −r=λ
V md ðrÞ ¼ σ · r̂ þ e ; ð2Þ
parity (P) and the time-reversal symmetry (T) [2,3]. These c 8πmb b rλ r2
symmetries are preserved in the electromagnetic and the
strong interactions, but are broken in the weak interaction. where gs and gp are the scalar and pseudoscalar coupling
Questions have been raised on the fundamental symmetry strength, respectively. mb is the particle mass with the
properties of the very weak gravitational interaction [2]. dipole coupling, r̂ is the unit vector connecting the two
The simplest form of spin-gravity coupling can be particles, and λ is the reduced Compton wavelength of the
express as [2,4] interaction propagator.
Searching for spin-gravity coupling has motivated a
V sg ðrÞ ¼ χσ · gðrÞ; ð1Þ
wealth of experimental efforts. Tests of the universal free
where χ is the coupling constant, ℏσ is the particle spin, and fall of atoms with different nuclear spins [10] or internal
gðrÞ is the gravitational acceleration at the location r. This states [11] were conducted with atom interferometers. Tests
P-odd and T-odd coupling introduces a gravitational dipole of local Lorentz invariance were performed using rotatable
moment to the particle, so that its center of mass and center of torsion balances and polarized massive objects [12,13].
gravity are separated accordingly [5]. Moreover, this cou- Searches for atomic energy shifts correlated with the
pling leads to a new force on the particle, Fa ¼ −∇V sg ðrÞ, flipping of the quantization axis relative to Earth’s gravity
which causes a spin-dependent local gravitational acceler- were also carried out, with 9Beþ ions stored in a Penning
ation. In this way, the spin-gravity coupling violates the trap [14], a 85Rb-87Rb comagnetometer [15,16], or a
199
equivalence principle. Hg-201Hg comagnetometer [17]. The most stringent
Spin-gravity coupling can also appear due to spin-mass upper limits on the spin-gravity coupling strength of the
coupling postulated in theories beyond the standard model. neutron have been set by Ref. [17].

0031-9007=23=130(20)=201401(6) 201401-1 © 2023 American Physical Society

 PHYSICAL REVIEW LETTERS 130, 201401 (2023)

Meanwhile, searching for monopole-dipole interactions A uniform bias field B0 (∼3.5 μT) is generated inside and
is dominated by the use of atomic magnetometers and points along the axis of the cylindrical shields. A circularly
comagnetometers [18,19]. The most stringent laboratory polarized “pump” laser beam is directed along B0 to
limits on jgNs gnp j=ℏc (N and n denote the nucleon and generate spin-polarized Rb atoms. A linearly polarized
neutron, respectively) over the range of λ > 1 m have been “probe” laser beam is used to measure the Rb polarization
provided by experiments using a 3He-K self-compensation component perpendicular to B0 . Here, the polarized Rb
comagnetometer [20] and a 199Hg-201Hg comagnetometer atoms are used both to hyperpolarize the Xe atoms and to
[17]. In addition, a model-dependent constraint has also sense the nuclear spin signals of Xe atoms as an in situ
been set by analyses of astronomical events [21], which magnetometer [22]. The two Xe isotopes are chosen for
surpasses the laboratory limit when λ < 2 × 104 m. their long nuclear spin coherence times, and for their nearly
In this Letter, we employ a ground-based 129Xe-131Xe-Rb equal collisional shifts in the Rb vapor [23]. To suppress the
atomic comagnetometer to search for the aforementioned effect due to the nuclear quadrupole moment of 131Xe, we
exotic spin-dependent interactions between the neutron amplify and resolve the quadrupole splittings by deliberately
spin and Earth. This comagnetometer configuration greatly employing elongated cell geometry [23]. The entire comag-
suppresses the influence due to drifts and fluctuations in the netometer system is mounted on a set of two rotation tables
bias field [19]. As a quantum compass, this comagnetom- (No. 1 and No. 2) and a tilt table [Fig. 1(a)].
eter is used to align the direction of the bias field along The comagnetometer operates in a similar way as in
Earth’s rotation axis with a precision of 0.58° (1σ), so that Ref. [24], and we extract the nuclear spin precession
the systematic effect in setting the bias field orientation frequency ω by fitting the comagnetometer signals [25].
is minimized. By measuring the ratio of nuclear spin- There are three sources that contribute to ω: first, the
precession frequencies between 129Xe and 131Xe as the bias Larmor precession, whose frequency ωL ¼ γB0 ; second,
field is flipped between being parallel and antiparallel to the Earth’s rotation [30] at angular velocity ΩE ; third, the
Earth rotation direction, we determine the Earth rotation rate anomalous spin-dependent couplings described in Eqs. (1)
with an accuracy of 2.6 nHz (1σ). After subtracting off and (2). It is customary to convert both Eqs. (1) and (2) into
Earth rotation effect, the remaining results lead to a limit the simpler expression of V ¼ ϵI · A, with ϵ as the fraction
improved by an order of magnitude on both the spin- of the particle spin projected onto the atomic spin vector I,
dependent gravitational interaction and the monopole- and A pointing along the direction of the local gravity. In
dipole coupling for the neutron spin at Earth range. this way, the new physics can be treated as a torque on Xe
The experiment is performed in Hefei, China, at the spins. The Larmor precession term is dominant so that ω
latitude of 31.82°. The comagnetometer cell has an inner can be approximately expressed as
dimension of 10 × 8 × 8 mm3 . It is filled with Rb atoms of
natural isotopic abundances, 4 Torr of 129Xe (nuclear spin ω ¼ jγB0 þ ΩE cos θ þ Aϵ cos ϕj; ð3Þ
I ¼ 1=2), 35 Torr of 131Xe (I ¼ 3=2), 5 Torr of H2 , and
160 Torr of N2 . The cell is placed at the center of a solenoid
system, and four layers of mu-metal shields [Fig. 1(a)]. where θ is the angle between ΩE and B0 , and ϕ is the angle
between A and B0 . The frequency ratio R of the two Xe
(a) (b) isotopes can be expressed as

ω129 1−ρ ϵ − ρϵ131

R¼ ≈ −ρ − ΩE cos θ − 129 A cos ϕ;
ω131 ωL;131 ωL;131
ð4Þ

where ωL;131 is the Larmor precession frequency of

131
Xe driven by its magnetic dipole moment. The ratio
of gyromagnetic ratios ρ ¼ γ 129 =γ 131 ¼ −3.373 37ð2Þ is
determined in this experiment, and the result is consistent
FIG. 1. (a) Illustration of the experimental setup. The comag- with that reported by Bulatowicz et al. [27]. The Earth
netometer is mounted on a system of a horizontally placed rotation frequency ΩE =2π ¼ 11 605.761 nHz has been
rotation table (No. 1), a tilt table, and a tilted rotation table
precisely determined with a sub-pHz error [31].
(No. 2). (b) Coordinate systems of the setup. The x-y-z system is
defined by the geographical orientations, and corresponds to table We aim to set the angle θ between the bias field (B0 ) and
No. 1; similarly, the x0 -y0 -z0 system corresponds to table No. 2. Earth’s rotation direction (ΩE ) to be close to zero, where
ΩE is contained in the y-z plane by definition, and tilted by θL ¼ cos θ is least sensitive to the angle-calibration uncertainty.
31.82° above the z axis. B0 forms a small angle β with the x0 -z0 Here we describe a compass procedure to determine the
plane, and its projection on x0 -z0 forms an angle α with z0 . Earth rotation direction using the comagnetometer.

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 PHYSICAL REVIEW LETTERS 130, 201401 (2023)
(a) (a)

(b)

(b)

FIG. 3. (a) All the data collected in the search for anomalous
couplings. Each data point represents an average result from 16
experiment cycles taken in over 60 min. The weighted average of
all data is Ωm =2π ¼ 11 605.2  2.5 (stat) nHz, with the reduced
χ 2 as 1.2. (b) Studies of systematic effects by varying the bias
FIG. 2. (a) Frequency-ratio amplitude Ramp as a function of φ. field, cell temperature, pump beam powers, etc. The weighted
For each data point, in order to determine the amplitude, R is average of all data is given in the window “All.” In both (a) and
measured at 13 positions of α, costing a measurement time of (b), the red lines mark the recommended value of Earth’s rotation
26 h. (b) Frequency ratio R as a function of α with φ ¼ 0 and frequency.
β þ ψ ¼ θL . R is shown as δRðαÞ ¼ RðαÞ − RðαÞ. Each data
point takes 2 h to collect. The red lines in both plots are fitting
results. φ0 and α0 are offset angles. The data in both plots are
taken with B0 ¼ 2.32 μT and T ¼ 110 °C. After φ is fixed at zero, R can be expressed as

ð1 − ρÞΩE
As shown in Eq. (5) of the Supplemental Material [25], θ R ¼ jρj − ðsin2 β þ cos2 β cos αÞ: ð6Þ
can be derived with the angles defined in Fig. 1(b). In order ωL;131
to determine β, we send a circularly polarized calibration
laser beam nearly parallel to B0 through the cell, and By fitting the experimental results in Fig. 2(b) using Eq. (6)
monitor its resonant absorption by Rb [25]. Modulated and repeating the experiment process three times, we
absorption spectroscopy is performed to align B0 with the determine the position of α ¼ 0° with an error of 0.28°
calibration laser beam. We then measure the angle between (1σ). Combining all of the measurement uncertainties, we
the laser beam and the x0 -z0 plane of table No. 2. In this way, align the bias field B0 to Earth’s rotation axis ΩE with the
β is calibrated to be −0.14°  0.30°. ψ is then set to result of θ ¼ 0°  0.58° (1σ).
31.96°  0.05° by adjusting the tilt table so that the central Once the alignment is complete, the search for new
values of ψ þ β are equal to the latitude angle θL . physics starts by comparing the frequency ratios between
The part of the measured frequency ratio R that is Rþ at θþ ¼ 0°  0.58° and R− at θ− ¼ 180° þ 2β, and
dependent on α is recording their difference ΔR ¼ R− − Rþ . We define the
resolved rotation rate Ωm of the comagnetometer as
ωL;131 ΔR=2ð1 − ρÞ to describe the search results as this
ð1 − ρÞΩE
Rα ¼ − fsin θL cos α sin ψ cos β þ cos θL quantity is independent of the magnitude of B0
ωL;131
× ½cos βðcos α cos φ cos ψ − sin α sin φÞg; ð5Þ ðcos θþ − cos θ− ÞΩE ðϵ129 − ρϵ131 ÞA cos ϕ
Ωm ¼ þ : ð7Þ
2 1−ρ
which can also be expressed as Rα ¼ Ramp ðφÞ sinðα − cÞ
for each chosen φ with c as a phase offset. Figure 2(a) For each data point of Ωm in Fig. 3(a), we spend four
shows the experimental results of Ramp at different rotation experimental cycles at θþ , followed by eight cycles at θ− ,
angles of table No. 1. By fitting the results using the then again with four cycles at θþ , for a total of 16 cycles
relation based on Eq. (5) and repeating the experiment over a total of 60 min including the time spent on the
process three times, we determine the position of φ ¼ 0° rotation of table No. 2. Our comagnetometer achieves a
with an uncertainty of 0.48° (1σ). typical rotation sensitivity of 1 × 10−7 Hz hr1=2 on Ωm =2π.

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TABLE I. Error budget of the spin-gravity coupling parameter improved over the previous best limit by a factor of 17
Asg =2π. [17,37]. This result also leads to an upper limit of 2.7 fm
(95% CL) on the separation (ℏjAsg j=2mg) between the
Correction Uncertainty center of mass and the center of gravity of the neutron.
(nHz) (nHz) The spin-gravity coupling also leads to a spin-dependent
Bias field alignment 17.3 13.3 term in the gravitational acceleration. For the two spin
Cell temperature correlation −3.8 5.1 states of the neutron, the difference in the acceleration on
Residual magnetic field −1.3 1.4 the ground is jδgs ðrE Þj ¼ 2ℏjAsg j=mn rE , with mn as the
Pump beam power correlation <0.1 <0.1 neutron mass and rE as the Earth radius. The Eötvös
Systematics total 12.2 14.3 parameter of the neutron is defined as
Statistical result 63.8
jδgs;n ðrE Þj 2ℏjAsg;n ðrE Þj
jηs;n j ¼ ¼ : ð8Þ
Total 12.2 65.4 gðrE Þ mn gðrE ÞrE
The results of this Letter provide an upper limit jηs;n j ≤
ΩE is precisely known, but the measured values of θ and 1.7 × 10−21 (95% CL). In comparison, free-fall experi-
β lead to a correction and error of −0.68  0.52 nHz on the ments with atom interferometers have placed limits of jηs j
ΩE term on the right-hand side of Eq. (7). While this is the only at the 10−7 level [10,11], although there the accel-
dominant systematic effect to determine the new physics, erations were measured more directly.
other sources of systematic uncertainties are also inves- For the monopole-dipole interaction in Eq. (2), the
tigated [25]. We deliberately vary experimental parameters, constraint set by this Letter on the coupling constants
including B0 , the oven temperature, the pump beam power, jgNs gnp j=ℏc surpasses the results extracted from the astro-
and the π=2 pulse amplitude, and find no effects on the
nomical events at λ > 1 × 103 m (propagator mass
measured Ωm values.
mp < 2.0 × 10−10 eV) (Fig. 4), and reaches 3.7 × 10−36
We plot all the data taken over a span of three months in
Fig. 3(a), and selectively plot several systematic studies in (95% CL) when λ > 1 × 108 m (mp < 2.0 × 10−15 eV),
Fig. 3(b). The weighted average of all the data is which is a 17-fold improvement over the previous best
Ωm =2π ¼ 11 605.0  2.5ðstatÞ þ 0.2ðsysÞ nHz, leading to limit [17].
an independent measurement of the Earth rotation rate The results of this experiment can also be used to study
ΩE;m =2π ¼ 11 605.7  2.5ðstatÞ þ 0.6ðsysÞ nHz. Though other related theoretical models of anomalous interactions
the precision of 3 × 10−4 achieved in this Letter is lower [18,40]. One class of these models treats Earth as a source
than that of the state-of- the-art very large ring laser of polarized electrons [41,42]. These electrons exist in iron-
gyroscope [32] and atomic interferometer [33], it is one containing minerals, and align along Earth’s magnetic field
order of magnitude better than the previous best results lines [41]. Therefore, the results of this Letter can be used to
using comagnetometers [17,34].
As in Ref. [17], we use the Schmidt model [35,36] for
nuclear spin analysis, and get ϵ129 ¼ þ1 and ϵ131 ¼ −0.2.
Combining these results and Eq. (7), we extract the spin-
gravity coupling parameter jAsg j=2π ¼ 3.1  65.4 nHz,
with the error budget of Asg listed in Table I. The energy
difference between a spin-up and a spin-down state of a
neutron on the ground, ℏjAsg j, is less than 5.3 × 10−22 eV
at the 95% confidence level (CL). As shown in Table II, this
limit on the spin-gravity coupling of the neutron is

TABLE II. Constraints (95% CL) on the energy difference ℏjAsg j

due to the spin-gravity coupling and the Eötvös parameter ηs.

System Spin ℏjAsg j (eV) jηs j Reference

FIG. 4. The upper limits (95% CL) on the monopole-dipole
AlNiCo-SmCo5 Electron 2.2 × 10−19 1.2 × 10−15 Ref. [13] coupling constants jgNs gnp j=ℏc. Line 1 is based on a 3He-129Xe
85
Rb-87Rb Proton 3.4 × 10−18 1.1 × 10−17 Ref. [15] comagnetometer [38]; line 2 uses a self-compensating 3He-K
9
Beþ Neutron 1.7 × 10−19 5.4 × 10−19 Ref. [14] comagnetometer [20]; line 3 is from the analysis of astronomical
199
Hg-201Hg Neutron 9.1 × 10−21 2.9 × 10−20 Ref. [17] observation [21,39]; line 4 is from the spectroscopy of trapped
129
Xe-131Xe Neutron 5.3 × 10−22 1.7 × 10−21 This Letter Beþ ions [14]; line 5 is from a 199Hg-201Hg comagnetometer [17];
and line 6 is from this Letter.

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 PHYSICAL REVIEW LETTERS 130, 201401 (2023)

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