
3
III. DATASETS
The adjustment of parameters, i.e., the fitting proce-
dure, presented in this work has been carried out using
two different datasets, CODATA18 and DATA22. The
CODATA18 dataset consists of data that was used in
the latest CODATA adjustment in Ref. [1], but restricted
only to the subset most relevant for constraining NP. This
subset contains observables related to the determination
of the Rydberg constant R∞, the proton and deuteron
radii, rpand rdrespectively, the fine-structure constant
α, and the relative atomic masses of the electron, pro-
ton, and deuteron: Ar(e), Ar(p) and Ar(d), respectively.
The inputs are listed in Tables S1,S3, and include theory
uncertainties in Table S2. The other observables and pa-
rameters included in the CODATA 2018 adjustment are
very weakly correlated with the selected data, and can
be neglected for our purpose.
The DATA22 dataset combines the updated CO-
DATA18 inputs with the additional data that improve
the overall sensitivity to NP (see Table S6 and S9). In
particular, we include the measurements of transition fre-
quencies in simple molecular or molecule-like systems,
the hydrogen deuteride molecular ion (HD+) [33–35], and
the antiprotonic helium atom (¯p3He and ¯p4He) [36,37].
These have an enhanced sensitivity to the NP models
with mediators that have large couplings to quarks (and
thus nuclei). The three benchmark models of this type
are the Higgs portal, hadrophilic and ULD scalars, cf.
Sec II.
The CODATA18 dataset is used as a reference point
to verify the implementation of the inputs and the ad-
justment procedure, while DATA22 is used to obtain our
nominal results. The full list of data in the two datasets,
as well as further discussion of the importance of includ-
ing certain observables when constraining NP, is given in
Supplemental Material, Sections. S2 and S3.
IV. LEAST-SQUARES ADJUSTMENT WITH
NEW PHYSICS
The experimental data are compared to the theoretical
predictions with NP following the linearized least-squares
procedure [38]. The theoretical prediction for an observ-
able Otakes the form,
O=OSM(gSM) + ONP(gSM, αφ, mφ) + δOth ,(3)
where OSM is the state of the art SM predic-
tion, and depends on the SM parameters gSM =
{R∞, rp, rd, α, Ar(e), Ar(p), Ar(d)}, while the NP contri-
bution ONP depends in addition on αφand mφ. The
theoretical uncertainties are included as in Ref. [1], by
adding a normally distributed variable δOth with zero
mean and standard deviation equal to the estimated un-
certainty of the theoretical expression. The δOth’s are
treated as yet another set of input data and varied in the
fit, along with gSM,αφ, and mφ, in order to minimize the
χ2function constructed from the input data and theory
predictions (see also Sec. S1).
The SM theoretical predictions for atomic transi-
tion frequencies, the electron anomalous magnetic mo-
ment, and bound-electron g-factors are from Ref. [1] (see
references therein). The predictions for the HD+and
¯pHe transition frequencies are from Ref. [39,40] and [41–
43], respectively, and are updated with the latest CO-
DATA recommended values, see Sec. S3 for details.
The NP contributions to atomic and molecular
ion transition frequencies are obtained using (time-
independent) first-order perturbation theory [44,45]. We
use exact nonrelativistic wavefunctions for hydrogen-like
atoms and very precise nonrelativistic numerical ones
from a variational method of Ref. [46] for HD+and ¯pHe.
Expectation values of the Yukawa potentials in Eq. (2)
are calculated for a grid of mφvalues, taking advantage
of the fact that their matrix elements in the chosen basis
can be obtained in an analytical form. The precision is
limited to O(α2) because of the neglected relativistic cor-
rections to the wavefunction. The NP contribution to the
free-electron (g−2)earises at one-loop [47,48], while for
bound electrons we include an additional tree-level con-
tribution from electron-nucleus interaction [49]. Finally,
we assume NP to have negligible effects in atom recoil
measurements as well as relative atomic mass measure-
ments from cyclotron frequency measurements in Pen-
ning traps.
We pay particular attention to the possible degeneracy
between the determination of SM and NP parameters. In
the mφ→0 limit, the dark photon is completely degener-
ate with the QED photon, since couplings of the two are
aligned, qi=Qi, and thus only the combination α+αφ
can be determined from data. This degeneracy should
be retained in the theoretical predictions (3), which in
principle requires calculating NP effects to the same very
high order as the SM. We propose an alternative pro-
cedure, which uses the state-of-the-art SM calculations
but requires NP contribution only at LO in αφ, and re-
produces the correct qi→Qi,mφa01 limit, where
a0≡α/(4πR∞)=(αme)−1is the Bohr radius.
For light vectors we rewrite the NP potential in Eq. (2)
as the sum of the Coulomb-like potential with QED cou-
pling Qiplus the remainder,
Vij
NP(r) = αφ
QiQj
r+e
Vij
NP(r),(4)
where e
Vij
NP(r)≡αφ(qiqje−mφr−QiQj)/r. The theory
predictions are evaluated at LO in e
VNP(r), while the NP
Coulomb term and the related relativistic corrections are
evaluated to the same order as the SM, which amounts
to replacing α→α+αφin the SM predictions. For any
observable Othe theoretical prediction is then
O=OSM (α+αφ)+ e
ONP (α+αφ, αφ, mφ),(5)
where OSM is the SM contribution now expressed as a
function of α+αφand e
ONP is the NP contribution from