Systematic Errors in the ACME Electron EDM Experiment

Daniel Ang
Harvard University
(Dated: March 9, 2017)
The search for the permanent electric dipole moment of the electron (eEDM) is a powerful probe
for high energy physics beyond the Standard Model. In the last few decades, atoms and now
molecules have provided the means to dramatically improve statistical sensitivity in measuring
de . However, increases in statistical sensitivity must be balanced with corresponding increases in
characterization and elimination of sources of systematic errors. In this paper, we focus on the
measurement methods and systematic errors present in the ACME EDM experiment [3], currently
the most sensitive experiment searching for the electron EDM. We discuss both heuristic models
and physical mechanisms which can result in systematic errors in measuring de , and methods taken
to reduce known systematic errors. We also discuss attempts to solve the several systematic-error-
related puzzles which still remain in the experiment.

I. INTRODUCTION AND THEORETICAL
MOTIVATIONS FOR ELECTRON EDMS
In physics, electric multipole moments arise when one
tries to study electric potentials by expressing them in
terms of the electric potentials of ideal basic combina-
tions of elementary charges, such as monopoles, dipoles,
quadrupoles, etc. This is called the multipole expansion.
The dipole term is the term proportional to 1/r2 , i.e. [5]
decades. Such an EDM would indicate the presence of a
T-violation (time-reversal violation) in nature. This can
be seen that if we perform the transformation t → −t to
a system where an electron EDM d~e is initially aligned
with the electron’s spin ~σ , then d~e → d~e but ~σ → −~σ .
Thus if |d~e | > 0, the system is T-odd. By the CPT the-
orem, where the product of CPT (charge, parity, and
time symmetry) must always be preserved, this implies
a CP-violation.

d~ · r̂
Vdip = , (1)
r2
where for a general charge distribution ρ(~r), the electric
dipole moment (EDM) d~ is defined to be
Z some CP-violation that results in a non-zero EDM for
d~ = ρ(~r)~rd3 r. (2)
Thus in this classical picture, an EDM can be roughly
understood as the degree to which an electric potential
resembles that of the charge configuration consisting of a
pair of positive and negative unit charges separated by a
distance s, where we take the limit s → 0. In order to fix
the value of d~ in Eq. 2 independent of coordinate system,
the origin is commonly taken to be at the center of mass.
Thus d ≡ |d~e | can be understood as the separation be-
tween the centers of charge and mass of the particle (or
system).
In atomic and particle physics, de is commonly given
the units e · cm. The (nonrelativistic limit) of the energy
contribution from a dipole moment when placed in an
~ is
electric field E
H = d~ · E.
~ (3)
In modern atomic, molecular, and optical physics, one
can talk about the EDMs of atoms and molecules sim-
ilar to EDMs in a classical system. It is common for
composite molecules to have a permanent EDM, such
as water. However, the search for a permanent non-
zero EDM in fundamental particles such as the neutron,
proton and electron have been ongoing for the last few
II. EDMS OF FUNDAMENTAL PARTICLES AS
A PROBE FOR NEW PHYSICS
The Standard Model of particle physics does allow for
fundamental particles. In the case of the electron EDM
(eEDM), this arises from coupling of the electron to vir-
tual quarks via the W boson [6]. However, the contri-
bution is only non-zero at the level of 4-loop Feynman
diagrams, which gives a very small SM prediction for d~e :
|d~e | ≤ 10−38 e · cm, (4)
much smaller than the sensitivity of the state-of-the-art
eEDM measurement, which is only at 10−28 e · cm.
However, many new models of physics beyond the
Standard Model (BSM) predict a much larger value for
d~e . These models contain more CP violation than the
SM, which is appealing because it can solve other major
problems in physics. One of the most notable puzzles is
that the CP-violation in the SM is too small to explain
electroweak baryogenesis in the early universe resulting
in the present asymmetry between baryonic matter and
antimatter. Some BSM models, such as the Minimal Su-
persymmetric Model (MSSM), predict |d~e | ∼ 10−29 e·cm
(with certain natural assumptions) [7]. Thus, AMO
eEDM experiments are a useful tool to test these the-
ories. Compared to efforts at large particle accelera-
tors, eEDM experiments are often several orders of mag-
nitude cheaper while probing comparable (TeV) energy
scales [4].

III. ELECTRON EDMS IN ATOMIC AND
MOLECULAR SYSTEMS
To make an experiment measuring an eEDM, one must
subject an electron to an electric field in order to create
a measurable energy shift as shown in Eq. 3. However,
it is difficult to perform experiments on free electrons. It
is much more advantageous to perform an experiment by
examining an unpaired valence electron in orbit around
the nucleus of an atom or molecule. When one takes into
account relativistic effects,1 we will have
d~A = αd~e , (5)
where d~A is the atomic/molecular EDM and α is a con-
stant that depends on the atom or molecule involved.
Generally, α ∝ Z 3 , where Z is the atomic number of the
atom [6].2 Hence the effective electric field “felt” by the
electron is amplified, amplifying the energy shift being
measured:
H 0 = d~e · E
~ eff , (6)
where E ~ eff = αE.
~ This allows one to apply electric fields
far beyond what is feasible in a laboratory. For example,
in the case of ThO, α ∼ 109 , so by applying a E ~ of tens
of kilovolts, one can get an effective electric field of tens
of gigavolts. Similarly large values of α also exist in the
case of YbF and Hf+ .
IV. SPIN PRECESSION MEASUREMENT FOR
ELECTRON EDMS
In state-of-the-art eEDM experiments such as the ThO
(Harvard-Yale) [4] and YbF (Imperial College) [8] exper-
iments, the measurement of the eEDM in a molecule is
performed via a spin precession measurement. In the rest
of this paper, we shall discuss the method of measuring
de and the systematic errors that can arise from it, us-
ing the case of the ACME EDM Generation I experiment
(henceforth referred to as “ACME I”) as the main case
study.3 This experiment published the best current limit
on de in 2014 [3].
In the ACME I experiment, spin precession is
performed using thorium monoxide molecules in the
|H 3 ∆1 , J = 1, M, Ωi metastable state. Ω is the quan-
tum number denoting the projection of total electronic
1 ~ B
In the non-relativistic limit, Schiff ’s theorem tells us that any
electron EDM will be canceled out by the other charges in the
atom or molecule. Sandars [1] was one of the first to realize that
the theorem is evaded in the relativistic limit.
2 Or the larger atom in a molecule.
3 The following explanation for the spin precession measure-
ment method is adapted from various published materials about
ACME I, especially [4], [6] and [9].
2
angular momentum onto the internuclear axis. The H-
manifold of ThO has Ω = 1 and contains a pair of so-
called Ω-doublet states. These states have opposite par-
ity, so when the molecule is subjected to an electric field
~ Stark shifts separate the energy levels by 2dH |E|
E, ~ (as-
suming M = ±1). We denote the two states by the
quantum number Ñ = n̂ · Ê = ΩM sign (Ê · ẑ) = ±1,
which also denotes whether the effective electric field is
aligned with the laboratory electric field (Fig. 1) [9].
A diagram of the whole experiment can be seen in
Fig. 2, although for the purposes of this paper we will fo-
cus only on aspects that are relevant to discussing the sys-
tematic errors arising in the experiment. The molecules
are first produced via laser ablation of a thorium tar-
get in a buffer gas-cooled cell. Initially, they are all
in the ground X state, with a mixture of different J
and M values. Optical pumping using a 943 nm laser
transfers molecules in the |X 1 Σ+0 , J = 1, M = ±1i state
to the short-lived |A3 Π0 , J = 0, M = 0i excited state,
which spontaneously decays to the metastable states
|H, J = 1, M = ±1, Ñ i and |H, J = 1, M = 0− i.
Next, optical pumping is performed with a 1090
nm laser between the states |H, J = 1, M = ±1, Ñ i
and |C 1 Π1 , J = 1, M = 0, P̃ = +1i. The 1090 nm laser
(which is called the prep laser ) is such that it can select
which Ñ state to pump out, but leaves the different M
states unresolved. Hence, it pumps out one of the two
possible superpositions of the two possible superpositions
of |M = ±1, Ñ i (called the bright state) out from the H-
manifold into the C-manifold, upon which they decay
into the ground state. The other superposition (the dark
state) remains and becomes the experimental state:
1
|ψ(τ ), Ñ i = √ (|M = +1, Ñ i − |M = −1, Ñ i). (7)
2
At this point, the molecules enter the “interaction re-
gion,” where the spin precession measurement begins.
Note that the forward (longitudinal) velocity of the
molecules is taken to be along the x̂ direction. Constant
~ = E ẑ) and magnetic (B ~ = B ẑ) fields are ap-
electric (E
plied uniformly in the ẑ direction, causing an energy shift
given by
~ − M µH |B|
∆H = − Ñ dH |E| ~ B̃
~ B|ηµ
− M Ñ B̃|E|| ~ ~ ~
B − M Ñ Ẽ(de · Eeff ), (8)
where µH is the magnetic moment of the H-state, and η
is a parameter characterizing the Ẽ-dependent magnetic
moment difference between different Ñ levels. We have
also used the notation B̃, Ẽ = ±1 to denote whether the
E, ~ are aligned or anti-aligned with the fixed laboratory
axis ẑ. The energy shift causes the initial state in Eq. 7
to acquire a phase
1 L
Z
dx
φ= (∆H(M = +1, Ñ ) − ∆H(M = −1, Ñ ) ,
2 0 v
(9)
 3

Figure 1. Structure of H-state of ThO, showing the various shifts dependent on Ñ and M . Figure adapted from [4].

Figure 2. Schematic of the whole ACME experiment, including the beam source, stem, and interaction region. Figure adapted
from [4].

where v is the forward velocity of the molecules. Compo-
nents with different M values acquire opposing phases,
resulting in the state
1 in the system that reduce the number of photons, such
|ψ(τ ), Ñ i = √ (eiφ |M = +1, Ñ i + e−iφ |M = −1, Ñ i).
2 etc. The relative polarization angles are chosen such that
(10)
We then project this spin-precessed state into a known
state by optical pumping on the H → C transition4 using
linearly polarized light (which we call the readout laser).
After some time the molecules will decay back to the
ground state X, resulting in fluorescence given by
 
1 + |C|
F (θ) = f N0 cos2 (φ − θ), (11)
2
where N0 is the number of molecules in the relevant Ñ
state, f is the fraction of detected fluorescence photons,
4 In ACME II, this is the H → I transition. Throughout this
paper we will mostly refer to the ACME I experiment.
θ ≡ θread − θprep is the relative polarization between the
preparation and readout lasers, and C is a unitless param-
eter between 0 and 1 characterizing other imperfections
as imperfect optical pumping, decay from C back to H,
|φ − θ| ≈ π/2.5
During the experiment, θread is rapidly switched at 200
kHz between alignment with the x̂ and ŷ lab axes, result-
ing in FX = F (0) and FY = F (π/2). We then compute
an asymmetry
FX − FY
A= = |C| cos (2(φ − θ)), (12)
FX + FY
from which we extract the phase φ. From Eq. 8, we can
5 We measure the contrast for a given Ñ , Ẽ, B̃ by dithering the
value of θ = θnr +θ̃∆θ, where θnr is the non-reversing component
of θ and θ̃ = ±1. The contrast is given by C = − 12 ∂A ∂θ
. It is
commonly measured to be ≈ 0.95.

see that by performing ion measurement multiple times6
and switching the relevant values of Ñ , Ẽ, B̃ = ±1, we
will obtain a parity sum of all the components of φ:
φ(Ñ , Ẽ, B̃) =Ñ φÑ + ẼφẼ + B̃φB̃
+Ñ ẼφÑ Ẽ + Ñ B̃φÑ B̃ + +Ẽ B̃φẼ B̃
+Ñ Ẽ B̃φÑ Ẽ B̃ (13)
from which we can extract whichever term we want by
adding multiple measurements of the appropriate com-
bination of parities. In practice, all 16 possible combi-
nations of the 4 binary switches Ñ , Ẽ, B̃, θ̃ are performed
(called a “block”)7 . Then the electron EDM de is ex-
tracted from the component of the phase φÑ Ẽ which does
not reverse under switching of Ñ Ẽ via the equation
φÑ Ẽ
ω Ñ Ẽ = , (14)
τ
where ω Ñ Ẽ is the precession frequency and τ the time
of precession. The spin precession time τ is determined
from the Zeeman precession phase: extracting φB̃ from
the equation φB̃ = µB gH |B|τ ~ , using known measured
values of µH and |B|.~
The fundamental statistical uncertainty on de comes
from the quantum shot noise, which can be expressed as
1 systematic error that shows up in the ACME experiment
δde = p , (15)
~
2|C|τ |Eeff | Ṅ T
where τ is the spin precession time, N is the number
of molecules, and T is the averaging time (commonly
taken to be about a week). For ACME I, this resulted in
δde ≈ 5 × 10−29 e · cm. This is an important number to
remember as we go through discussions about systematic
errors, as a systematic uncertainty smaller than statisti-
cal uncertainty means is effectively negligible.
V. PROCEDURE FOR SEARCHING FOR
SYSTEMATIC ERRORS
The ACME experiment’s method of extracting de al-
lows it to be resilient against potential sources of system-
atic errors which may enter the system in various parts
6 As the ThO beam source is produces molecules in batches (or
“shots”) which repeat at frep = 50 Hz (due to the method of
generating ThO via laser ablation), it is natural to denote spin
precession on one shot of molecules as one “measurement.” The
measurement would be repeated 25 times and then averaged,
creating one “trace,” before switching to a different combination
of binary switches.
7 A block actually consists of 25 × 4 × 16 = 1600 shots, as each
switch combination (giving a trace) is performed 4 times and
averaged.
4
Figure 3. Data acquisition structure of the ACME experiment
at the block and superblock level. Figure adapted from [4].
of the experiment. As long as the contribution from the
error source reverses under Ñ Ẽ, it will be “washed out”
as more data are averaged, remaining only as “harmless”
statistical noise. As the measurements are performed at a
repetition rate frep (where commonly, frep = 50 Hz), only
noise occurring at extremely close to nfrep (where n ∈ N)
will take impractically long to average out.8 Thus, any
must be those that correlate with Ñ Ẽ.9
An additional safeguard against systematic errors in
ACME is the presence of other binary switches in ad-
dition to the 4 main block switches. For example, in
Generation I there were 4 “superblock” switches, such as
L̃, which swapped the physical leads on the power supply
to the field plates generating the electric field,10 and P̃,
which switched frequency the readout laser beam to al-
ternate between the two Ω-doublet states in the C-state.
Fig. 3 shows a glimpse of the data acquisition structure at
the block and superblock level. For each possible value of
the superblock switches (24 = 16 possible states), all the
8
Even noise at exactly nfrep Hz is in principle still not a source
of systematic error, as long as it is not non-reversing under Ñ Ẽ.
That being said, it is still undesirable for the system to have
statistical noise coming from any source which causes a statistical
error larger than that which arises naturally from the quantum
shot noise, so much effort is still devoted to eliminating sources
of noise when one can.
9 Much of the discussion on systematic errors in this and following
sections was adapted from the thorough exposition in [10]. It
is also worthwhile to note that at the time of writing, ACME
II is already underway, introducing various improvements that
will result in its own possible plethora of systematic issues. This
reference also discusses these potential Generation II issues in
greater detail.
10 The Ẽ switched is performed by switching the set voltage on the
power supply.
 5

possible values of the block switches also had to be per- where α∆,i , α∆2 ,i , βdΩr ,i are constants of appropriate di-
formed. There were also even higher-level “uberblock” mension. To isolate the component that mimics an EDM
switches, such as changing the magnitude of E ~ and B~ and and thus a systematic error, we need to take ∆i ≡ ∆Ñ Ẽ
i
reversing the propagation direction of the readout laser. and Ωr,i ≡ ΩÑ Ẽ
r,i in the equation above, looking for only
With the exception of the last one (which we shall cover
the contributions to the phase that correlate with Ñ Ẽ.
in a later section), none of the superblock or uberblock
From this empirical model, we now proceed to the actual
switches caused any change in the measured de , so all the
physical mechanisms that can cause these terms to arise.
block data was simply averaged over.
In addition to the safeguards that are a part of the
fundamental data acquisition structure, over 40 other
A. Non-Reversing Electric Fields Resulting in
parameters were intentionally varied in search for possi- Changes to ∆i
ble systematic correlations with the φÑ Ẽ EDM channel.
These were divided (in Ref. [4] and [10]) into parame-
First, we shall focus on the ∆i factor in the first term
ters with an “ideal” value and those without. The latter
of Eq. 16. It turns out that this factor can arise from im-
category includes parameters used in the data analysis
perfections in the electric fields applied to the molecule,
routine and others which are outside of the scope of this
namely non-reversing fields or E nr .11 This could be the
paper. (In addition, none of the parameter variations
result of an electronic offset in the power supply to the
found a statistically significant systematic error.) We
field plates, for example. Such an imperfect E could be
shall instead focus on several entries in the former cat-
parameterized as
egory, especially those which relate more closely to the
atomic and molecular physics of the experiment. Exam- Eztot = Ez Ẽ + Eznr + ... (17)
ples of this category are non-reversing electric and mag-
netic fields, transverse magnetic fields (Bx,y ), prepara- where E is the intended applied field. We have also taken
tion/readout laser detunings from the ideal frequency, only the z-component of E (which is the intended direc-
etc. tion), assuming that the other components are zero or
For each of these parameters the deviation from the cancel out throughout the interaction region. The pres-
ideal was amplified up to 10 times and the resulting φÑ Ẽ ence of Eznr causes a Stark shift in the experimental H-
noted. These were called Intentional Parameter Varia- state that is odd under Ñ Ẽ, as can be seen in Fig. 4.
tions (IPV). It was assumed that the relation between The Stark shift changes the frequency for the H → C
φÑ Ẽ and each parameter could be well-characterized lin-
early, preventing the necessity of taking a full, two-week
dataset on each possible IPV. Higher-order polynomial
fits were also tried when applicable, but no significant
increase in systematic uncertainty was observed. It is of
course always possible that nonlinearity is present in be-
tween the data points that we took in the IPV, but this
possibility was lessened by taking data over as wide of
range of parameters as possible.

VI. SYSTEMATIC ERRORS CAUSED BY AC

STARK SHIFTS

We now proceed to discuss the systematic errors found

in ACME I, starting with the two major ones. One
of the main mechanisms by which additional terms can
contribute to φ and potentially result in a systematic-
inducing φÑ Ẽ is through AC Stark shifts coming from the
Figure 4. Structure of Stark shifts in the H-state as a result
prep and readout lasers. These shifts were first detected of Eznr . Notice that the sign of the shift changes depending
in ACME I as it was observed that the measured phase on the Ñ -state. Figure adapted from [4].
φ had a dependence on the laser detuning frequencies ∆i
and Rabi frequencies Ωi , where i ∈ {X, Y, prep}. This
dependence can be expressed as the general equation
X dΩr,i
δφ(∆, Ωr ) = [α∆,i ∆i + α∆2 ,i ∆2i + βdΩr ,i + ...], 11 For the rest of this paper, “nr” stands for “non-reversing” - i.e.,
Ωr,i
i X nr indicates the component of X which does not reverse under
(16) any binary switch in the experiment.
 6

transition, which we can parameterize as where dH is the transition dipole moment between H →
C and I is the laser intensity. Thus it seems that any
1 ΩÑ Ẽ Ñ Ẽ
r,i must be the result of some W (where W is the
nr
ωHC,i = ωHC − P̃i ∆C,J=1 + Ñ dH Eztot , (18)
2
laser power) or dÑ Ẽ
H . However, W
Ñ Ẽ
was measured using
where the P̃i term exists because we switch the parity photodiodes and found to be too small to explain ΩÑ Ẽ
r,i .
of the C-state addressed by the readout lasers (which is It was then thought that the effect could be explained
either X or Y ; see Section V). Assuming that the laser by dÑ Ẽ
H , arising from Stark interference between E1 and
frequency is ωL,i such that ∆i = ωHC,i − ωL,i , inserting M1 dipole transition amplitudes, the fuller derivations
the result of Eq. 17 into Eq. 18, we immediately see that which are present in [10] and [11]. However, despite the
an Ñ Ẽ-dependent term arises in ∆i : lengthy calculation in [10], it is conceded that the Stark
interference effect vanishes for interference of multiple
nr
∆i = ωHC + Ñ dH |Ez Ẽ + Eznr | + ... plane waves. Thus, while in the end ΩÑ Ẽ
r,i was thoroughly
= ∆nr Ñ Ẽ
i + Ñ Ẽ∆i + ... (19) measured and constrained to be at the 10−31 e · cm level,
its origin as well as its puzzling dependence on (k̂ · ẑ)
where ∆Ñ Ẽ
= dH Eznr (other terms, including those de- remains an open puzzle to be solved in future generations
i
pendent on Ẽ, Ñ , or P̃ have been subsumed into the of the ACME experiment.
“...”). Inserting this back into Eq. 16, this result in a Altogether, the resulting systematic error arising from
term that masquerades as the EDM in φ. the laser detuning and Rabi frequency is then given by
X
φÑ Ẽ
Eznr = α∆,i dH Eznr , (24)
i
B. The case of Ωr,i X
φÑ
ΩÑ
Ẽ
Ẽ = βdΩr,i (ΩÑ Ẽ nr
r,i /Ωr,i ). (25)
r
i
Analogously, one can derive a similar result for the
dependence of the H → C transition Rabi frequency,
assuming the existence of some mechanism to cause a C. Physical Mechanism for α∆,i , α∆2 ,i , and βdΩr ,i
Ñ Ẽ
non-reversing Ωr,i :
Now we shall proceed to explaining a model for how the
Ñ Ẽ
Ωr,i = Ωnr
r,i + Ñ ẼΩr,i + ... (20) AC Stark shifts are caused - in other words, how the con-
stant factors α∆,i , α∆2 ,i , βdΩr ,i arise in Eq. 16. According
Unlike the case of ∆Ñ Ẽ
arising from Eznr which we have to this model, when pumping on the H → C transition
i
(either with the prep or readout lasers) some mixing be-
just discussed, in ACME I a statistically significant ΩÑ
r,i
Ẽ
tween dark and bright states occurs due to imperfections
was detected, but the physical mechanism is still not fully
in the laser polarizations. This causes a precession phase
understood. This effect was first detected in the form of
shift.12
an Ñ Ẽ-dependent fluorescence signal that reversed with
We first start with the three states involved in the opti-
the laser propagation direction k̂ · ẑ,
cal pumping between H → C, as described in Section IV:
the dark and bright states of H and the excited C-state:
F Ñ Ẽ
≈ −(2.4 × 10−3 )(k̂ · ẑ) (21) |B(ˆ
), Ñ , P̃i , |D(ˆ
), Ñ , P̃i , |C, P̃i , (26)
F nr
where we have included the fact that the bright and dark
as well as a non-zero φÑ Ẽ B̃ which was similarly dependent
states depend on the polarization ˆ of the laser. The
on Bz and k̂ · ẑ. From this it is believed that the φÑ Ẽ B̃ above basis is valid valid for both the prep and read-
arises from the relation out stages of the experiment. We transform this into a
new 3-state basis in which it is easier to understand the
ΩÑ Ẽ
φÑ Ẽ B̃ = βdΩ
B̃
Bz r
nr
, (22) phenomenon [10]:
r
Ωr
|B± i ≡ ±κ± |C, P̃i + κ∓ |B(ˆ
), Ñ , P̃i ,
which is a B̃-odd AC Stark shift. Eq. 22 was empirically |Di = |D(ˆ
), Ñ , P̃i (27)
verified by inserting an artificial ΩÑ Ẽ into the experiment
and observing that φÑ Ẽ B̃ changed accordingly. for some coefficients κ± , which can be easily found, along
When looking for possible physical mechanisms that with the eigenvalues of the new basis vectors. We as-
sume that some physical mechanism causes the laser po-
could give rise to ΩÑ Ẽ , one can first observe that the
larization to be imperfect, possibly changing its ellipticity
Rabi frequency Ωr,i is determined by [11]

dH p
Ωr,i = Ii 0 c, (23) 12 Full details of the following calculations can be found in Ref. [10].
~
 7

and/or linear polarization angle. Allowing the new ba-
sis state vectors of Eq. 27 to vary in time, this means
that the laser polarization imperfection is also evolving
in time. One can thus define a complex polarization ro-
tation rate which takes into account both types of polar-
ization imperfection:
χ̇ = ξ˙ − i(θ̇ + δ),
where ξ ≡ − 21 S3 /I (S3 /I being the laser ellipticity Stokes
parameter) and δ is a detuning that accounts for the
Zeeman shift due to the presence of the magnetic field B
in the experiment. From here, the Hamiltonian can be
expressed in the new basis, as well as the time-evolving
state of the molecule during the spin precession:
|ψ(t)i = cD (t) |Di + cB+ |B+ i + cB− |B− i .
which imprinted some ellipticity on the light, given by the
expression [4]
S3 /I = Γ(x) sin (2(θ − φΓ )), (35)
where S3 /I is the ellipticity Stokes parameter, Γ(x) is the
material-dependent retardance on incident laser light on
(28) the field plates, θ is the linear polarization angle of the
laser and φΓ the angle of the fast axis of the birefringent
field plates. The form of Eq. 35 indicates that it is pos-
sible to minimize the imparted ellipticity by adjusting θ.
~ Indeed, various values of θ were tried and the resulting
dependence of φ on ∆ measured (see Fig. 5). The θ which
gave the flattest slope (in the case of the figure, θ = 0◦ )
was picked as the experimental configuration, minimizing
the effect of Eznr . In addition, Eznr was further reduced
(29)

Applying time-dependent perturbation theory, for the

case of the prep laser, one finally obtains a state that
consists of a mix of dark and bright components:

0prep , Ñ , P̃i = |D(ˆ

|D(ˆ prep , Ñ , P̃i (30)
+ dχΠ(χ, t) |B(ˆ
), Ñ , P̃i , (31)

where 0prep = prep + dχΠ(χ, t)iẑ × ˆ∗prep and Π(χ, t)

is a parameter that characterizes the dynamics of the
evolving laser polarization during the spin precession. In
the end, one will obtain

∂Im(Π)
α∆,prep ≈ − dξprep , (32) Figure 5. Dependence of measured phase φ on prep laser
∂∆prep
2 detuning ∆ for different values of θ. Figure adapted from [4].
∂ Im(Π)
α∆2 ,prep ≈ − (dθprep − tδ), (33)
∂∆prep
∂ Re(Π) by using a chopper wheel rotating at frep to reduce the
βdΩr ,prep ≈ (dθprep − tδ), (34) time-averaged laser power incident on the field plates by
∂Ωr
a factor of 2. All of these methods succeeded to reduce
explaining the origin of the constants in Eq. 16 for the Eznr systematic was to the ∼ 5 × 10−30 e · cm level.
case of the prep beam. A similar derivation can be per- The second possible source for polarization imperfec-
formed for the readout lasers as well. Thus we see how tions is the Gouy phase shift, which arises from the
z
the combination of an Enr and some residual bright state fact that Gaussian laser beams must result in polariza-
admixture in the experimental state can cause a shift in tion gradients at some level, which is a consequence of
the measured phase. Maxwell’s equations. Such an effect would be dependent
on the beam size. Assuming a laser beam propagating
in the z-direction, the resulting gradient would be in the
D. Sources of Polarization Imperfections xy-plane [10]:

The arguments of this section has so far shown that ∂θ λ2 y

≈ , (36)
any deviation in the polarizations of the lasers can poten- ∂x 2π wx wy
tially cause a phase shift due to its coupling to the Ñ Ẽ-
correlated Eznr . Thus, it is always preferable to minimize where λ is the laser wavelength and wx , wy are the dimen-
any sources of laser polarization gradients. In ACME I, sions of the beam. For ACME I, this effect turned out to
a particularly interesting mechanism was thermal stress- be too small to contribute significantly to the systematic
induced birefrigence of the electric field plates. This oc- error budget.13
curred as a result of the prep and probe lasers being shone
through the ITO-coated field plates responsible for pro-
ducing the electric field. The field plates absorbed the
13 However, in ACME II, instead of optical pumping, STIRAP is
laser light, causing it to heat up and inducing birefrigence

VII. Ẽ-CORRELATED SYSTEMATIC ERRORS
Due to the existence of the pair of opposite parity Ñ -
states and our ability to switch between them, the ACME
experiment is resilient against systematic effects resulting
in a contribution to φẼ , such as leakage currents, geomet-
ric phases and motional magnetic fields. These effects are
mostly washed away when we reverse Ñ . In addition, a
great advantage of ThO is that it is fully polarized by
only applying an electric field of ∼ 10 V/cm. Thus the
experiment is always operating in the regime where the
M -states are fully mixed, such that the contribution of
de to the Hamiltonian is always maximized.
However, there is still a small contribution to φÑ Ẽ in
the presence of φẼ because the two Ñ states have slightly
different magnetic moments, parameterized by η, as was
mentioned briefly when discussing Eq. 8. The contribu-
tion is given by [4]
η|Ez |µB Ẽ
φÑ
φẼ
Ẽ
= φ ,
gH
which was empirically verified by applying BzẼ = 1.4mG,
i.e., a magnetic field that reversed direction with Ẽ. The
resulting effect on φÑ Ẽ was found to be three orders of
magnitude smaller than the effect on φẼ . Thus this effect
did not contribute significantly to the systematic error
budget.
VIII. OTHER POSSIBLE SOURCES OF
SYSTEMATIC ERRORS
We have now finished discussing most of the theoreti-
cal explanations for the major systematic effects detected
in the ACME experiment for its 1st generation result [3].
As outlined in Section V, it is worthwhile to note that
besides these, almost all possible knobs on the experi-
ment were varied and amplified to see if any effect on
φÑ Ẽ would result. Examples include:
• Arbitrary large magnetic gradients (including in
the x, y directions). Such gradients were respon-
sible for the ultimate systematic limitations on the
earlier electron EDM experiment using PbO [13].
However, this effect was anticipated to be small for
ACME as the H-state has a very small value of gH .
• Laser detunings other than those correlated with
Eznr which we have already discussed previously
(i.e., ∆Ñ P̃
i , ∆i , etc.) were exaggerated.
used for state preparation, which involves highly focused laser
beams which would have resulted in a large Gouy polarization
gradient if not for the presence of a refinement beam which “re-
8
• The alignment between the readout laser beam and
the laboratory electric field was varied.
• The magnitude of Ez was varied. In each case,
the molecule was fully polarized, so no significant
change was expected.
• We did not include in our discussion several other
theoretical models of systematic errors which were
considered but estimated to come in at a negligi-
ble level, for example interference from levels other
than the three-level system we discussed in Sec-
tion VI C. The most complete exposition of all of
these models can be found in [10].
In all of the above cases (as well as others we did not have
space to include), there was no significant effect on φÑ Ẽ .
Still, in the final systematic error budget published in
[3], some uncertainties from the above effects were added
anyway as a precaution, based on experience of other
experiments (notably PbO [13] and YbF [8]). Even this
(37) extremely conservative total systematic uncertainty was
still below the statistical uncertainty: the final measured
value on |de | published in [3] was
de = (−2.1 ± 3.7stat ± 2.5syst ) × 10−29 e · cm, (38)
a 12-fold improvement over the previous result of [2].
IX. SUMMARY AND DISCUSSION
From our discussion of systematic effects, we see that
while there are several traits of ThO which make it possi-
ble for ACME to reach extraordinary statistical precision
(most notably its large internal electric field and high
electric polarizability), the true power of the ThO ex-
periment lies in the magic of the H-state, peculiarly the
Ω-doublet structure. As we have seen, and the method
of extracting de by measuring an asymmetry and then
switching Ñ , Ẽ, B̃, θ̃ states makes it incredibly resilient
against most systematic effects. Still, there remain two
major contributors to systematic error: Eznr , which is rel-
atively well-understood and the mysterious ΩÑ Ẽ
r . How-
ever, the fact that statistical improvements to ACME II
have been accomplished smoothly gives us good reason
to hope that in the next generation of the ACME exper-
iment more thorough investigations on these systemat-
ics and any new ones can be performed rapidly.14 One
can appreciate that the ACME experiment has resulted
in great gains in understanding systematics arising from
EDM searches which can potentially be of great benefit to
concurrent and future electron permanent EDM searches
[8][14].
prepares” the initial state at the start of the precession measure-

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