PHYSICAL REVIEW LETTERS 121, 103601 (2018)

Observation of Three-Body Correlations for Photons Coupled to a Rydberg Superatom

Nina Stiesdal,1 Jan Kumlin,2 Kevin Kleinbeck,2 Philipp Lunt,1 Christoph Braun,1 Asaf Paris-Mandoki,1,3
Christoph Tresp,1 Hans Peter Büchler,2 and Sebastian Hofferberth1
1
Department of Physics, Chemistry and Pharmacy, Physics@SDU, University of Southern Denmark, 5320 Odense, Denmark
2
Institute for Theoretical Physics III and Center for Integrated Quantum Science and Technology,
University of Stuttgart, 70550 Stuttgart, Germany
3
Instituto de Física, Universidad Nacional Autónoma de México, Mexico City, Mexico
(Received 31 May 2018; published 4 September 2018)

We report on the experimental observation of nontrivial three-photon correlations imprinted onto

initially uncorrelated photons through an interaction with a single Rydberg superatom. Exploiting the
Rydberg blockade mechanism, we turn a cold atomic cloud into a single effective emitter with collectively
enhanced coupling to a focused photonic mode which gives rise to clear signatures in the connected part
of the three-body correlation function of the outgoing photons. We show that our results are in good
agreement with a quantitative model for a single, strongly coupled Rydberg superatom. Furthermore, we
present an idealized but exactly solvable model of a single two-level system coupled to a photonic mode,
which allows for an interpretation of our experimental observations in terms of bound states and scattering
states.

DOI: 10.1103/PhysRevLett.121.103601

Engineering effective interactions between individual
optical photons is essential for applications in classical
and quantum computation, communication, and metrology
[1–3]. The most established approach to achieve two-
photon interaction is strong coupling of light to individual
quantum emitters, either in resonators [4–7] and wave-
guides [8–13] or through tight focusing in free space
[14–16]. A complementary approach combines electro-
magnetically induced transparency and strong interaction
between atoms in Rydberg states to convert photons into
interacting Rydberg polaritons in an extended medium
[17–19]. Here we exploit a combination of the two concepts
by using the Rydberg blockade mechanism [20] to convert
an atomic ensemble containing N individual atoms into a
single effective two-level quantum system, a Rydberg
superatom, with strongly enhanced coupling to a single
photonic mode [21,22].
A central concept for quantifying the influence of an
effective photon-photon interaction in any of these systems
is to study the intensity correlations imprinted by the
interaction onto initially uncorrelated photons by the
determination of n-body correlation functions:
hE† ðs1 Þ…E† ðsn ÞEðsn Þ…Eðs1 Þi
gðnÞ ðs1 ; …; sn Þ ¼ Qn †
: ð1Þ
i¼1 hE ðsi ÞEðsi Þi
Here, the operators E† ðsÞ and EðsÞ describe the creation
and annihilation, respectively, of photons at time s. The
outgoing photon rate is related to these operators via
IðsÞ ¼ hE† ðsÞEðsÞi. Two-photon correlations gð2Þ have
been extensively studied for a variety of systems [23],
and the observation of antibunching is accepted as a
characteristic fingerprint of a single-photon source [24],
while bound states of two photons have been observed as
strong bunching feature in Rydberg polariton systems [25].
To study the interaction between three photons, it is natural to
turn to third-order correlations gð3Þ [26–28]. While any two-
body correlation will also induce a signal in the three-body
correlation function, a natural approach is to subtract these
trivial contributions via the cumulant expansion to identify
the pure three-body correlations. This approach leads to the
connected part of the three-body correlation function:
X
ð3Þ
gc ðs1 ; s2 ; s3 Þ ¼ 2 þ gð3Þ ðs1 ; s2 ; s3 Þ − gð2Þ ðsi ; sj Þ: ð2Þ
i<j
ð3Þ
Note that gc vanishes if one photon is separated from the
other two. Furthermore, for any classical Gaussian state of
photons, the connected part of the three-body correlation
function is zero.
Here, we report the first experimental observation of
three-photon correlations by clear signatures in the con-
nected part of the three-body correlation function of
initially uncorrelated photons interacting with a single
Rydberg superatom. Our setup is based on a cold atomic
cloud interacting with a focused photonic mode coupling
to a highly excited Rydberg state via a far detuned
intermediate state. The transversal size of the photonic
mode as well as the longitudinal extent of the atomic cloud
is smaller than the Rydberg blockade volume, resulting in a
single effective emitter with collectively enhanced coupling

0031-9007=18=121(10)=103601(6) 103601-1 © 2018 American Physical Society

 PHYSICAL REVIEW LETTERS 121, 103601 (2018)
(a) (d)
(b) (c)
FIG. 1. (a) Sketch of the experimental setup to couple a single
Rydberg superatom to a few-photon light field. (b) Single-atom
level scheme. A weak probe and a strong control field couple the
ground state jgi via the intermediate state jei to the Rydberg state
jri. (c) Because of the Rydberg blockade, the atomic ensemble
behaves as a single two-level system with ground state jGi and
collective excited state jWi. In addition to decay, the excited state
can dephase into the dark state manifold fjDi igN−1
i¼1 . (d) Time traces
of the outgoing probe photon pulses (blue points) for incoming
pulses (broken lines) with three different peak photon rates
Rin ¼ 3.4 μs−1 , Rin ¼ 6.7 μs−1 , and Rin ¼ 15.2 μs−1 . Solid
orange lines show fits of our single-emitter model to the data.
to the probe light [22]. We demonstrate that such a
superatom gives rise to nontrivial three-body correlations,
in good agreement with a quantitative model for our
system. Finally, we present an idealized but exactly
solvable model of a single two-level system coupled to a
photonic mode, which allows for an interpretation of our
experimental observations in terms of a three-body bound
state coherently superimposed with two-body bound states
and scattering states. We note that recent experiments with
Rydberg polaritons have also found signatures consistent
with a three-body bound state of photons [28].
The experiment starts with trapping an ensemble of
24 × 103 laser-cooled Rb87 atoms at a temperature of
5.9 μK in an optical dipole trap positioned in the focus
(w0 ¼ 6.5 μm) of a weak probe beam at a wavelength of
780 nm [Fig. 1(a)]. The extensions of the atomic medium
(given by 1=e of the Gaussian density distribution) are σ z ¼
6.5 μm along the probe beam and σ x;y ¼ 10; 21 μm in the
transverse directions. We couple atoms from their ground
state jgi ¼ j5S1=2 ; F ¼ 2; mF ¼ 2i to the Rydberg state
jri ¼ j111S1=2 ; J ¼ 1=2; mJ ¼ 1=2i by overlapping the
probe beam with a strong counterpropagating control beam
λc ¼ 479 nm [Fig. 1(b)]. With a single-photon detuning
Δ ¼ 2π × 100 MHz and the two-photon detuning δ on
Raman resonance, the intermediate state jei ¼ j5P3=2 ;
F ¼ 3; mF ¼ 3i can be adiabatically eliminated, reducing
the dynamics of each atom to those of a resonantly driven
two-level system, with the upper-state decay rate being
103601-2
dominated by spontaneous Raman decay via jei with a rate
of Γ ¼ Ω2 =ð2ΔÞ2 Γe .
With a van der Waals coefficient of C6 ¼ 1.88 ×
105 GHz μm6 [29] and a control field Rabi frequency
Ω ¼ 2π × 12 MHz, the radius of the Rydberg blockade
volume is sufficiently large to blockade the whole inter-
section of the probe beam and sample, so that only a single
Rydberg excitation is allowed at any time. We verify this
through the sub-Poissonian counting statistics of field-
ionized Rydberg atoms detected on a microchannel plate.
Under these circumstances, N ≈ 5 × 103 atoms within the
overlap volume with the probe beam couple collectively to
the propagating light mode. Specifically, the N-body
ground state jGi ¼ jg1 ; …; i couples to the many-body
pffiffiffiffigNP
excited state jWi ¼ ð1= N Þ Nj¼1 eik·xj jji, where jji ¼
jg1 ; …; rj ; …; gN i is the state with the jth atom in jri and all
others in jgi, k is the sum of the wave vectors of the probe
and control fields, and xj denotes the position of the jth
atom. These two states form a single two-level superatom,
which couples topthe ffiffiffiffi probe light with collective coupling
constant gcol ¼ N g0 Ω=ð2ΔÞ [Fig. 1(c)]. The complete
basis of collective states also contains N − 1 dark states
fjDi igN−1
i¼1 formed by linear combinations of fjjigj¼1 .
N
Since all these states are orthogonal to jWi, they do not
couple to the probe light, but they still contain one Rydberg
excitation blocking the medium. The thermal motion of the
individual atoms constitutes the main dephasing from the
strongly coupled state jWi into the collective dark states in
our system. Additionally, the exchange of virtual photons
between atoms provides a coupling between the jWi state
and the manifold of dark states fjDi igN−1 i¼1 [30–33], which
can provide a fundamental limit on the minimal dephasing
rate [34].
We probe the superatom with Tukey-shaped probe pulses
with a peak photon rate Rin and collect the transmitted
probe photons with a set of four single-photon counters
[Fig. 1(a)]. After each probe pulse, a field-ionization pulse
removes the possibly remaining excitation in the medium,
resetting the superatom to state jGi. Figure 1(d) shows time
traces of the outgoing probe pulses for three different
photon rates Rin ¼ 3.4 μs−1 , Rin ¼ 6.7 μs−1 , and Rin ¼
15.2 μs−1 . Because of the low total photon number in the
probe pulses, the Rabi oscillation of the Rydberg popula-
tion [35–37] is visible in the transmitted photon stream as a
periodic modulation, which results from the absorption and
subsequent stimulated emission of single photons by the
coherently driven two-level atom.
On the theoretical side, the quantitative description of
the experimental setup is described in detail in Ref. [22].
The basic idea is to treat the superatom as a single two-level
system coupled to a quantized light field:
Z
dk pffiffiffi
H¼ ℏcka†k ak þ ℏ κ ½E† ð0Þσ GW þ Eð0Þσ †GW ; ð3Þ
2π
 PHYSICAL REVIEW LETTERS 121, 103601 (2018)
where ak and a†k are photon annihilation andR creation
pffiffiffi
operators, respectively, while EðxÞ ¼ ½ c=ð2πÞ dkeikx ak
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
is the electric field operator measured in photons=time,
pffiffiffi
and σ αβ ¼ jαihβj. Here, κ ≡ gcol =2 describes the collec-
tive coupling between the superatom and the light field and
accounts for the collectively enhanced spontaneous decay
rate κ. Eliminating the photonic modes for a coherent input
pulse leads to a master equation for the reduced density
matrix ρðtÞ of the atom alone:
i
∂ t ρðtÞ ¼ − ½H0 ðtÞ; ρðtÞ þ ðκ þ ΓÞD½σ GW ρðtÞ
ℏ
þ γ d D½σ DW ρðtÞ þ ΓD½σ GD ρðtÞ ð4Þ
with the Lindblad dissipator D½σ¼σρσ †p−ðσ † †
ffiffiffi  σρþρσ σÞ=2
and the driving Hamiltonian H0 ðtÞ ¼ ℏ κα ðtÞσ GW þH:c:
Here, the coherent field amplitude αðtÞ is related to the
time-dependent mean photon rate by jαðtÞj2 ¼ Rin ðtÞ. In
addition to the intrinsic collectively enhanced decay κ into
the photonic mode, we include phenomenologically the
spontaneous decay of the Rydberg level with rate Γ as well
as the dephasing of the superatom state jWi into the
manifold of dark states with rate γ d . The outgoing pffiffiffi electric
field operator is determined by EðtÞ ¼ αðtÞ − i κσ GW ðtÞ.
Fitting these parameters by comparing the theoretical
predictions with the experimental outgoing photon time
traces [orange lines in Fig. 1(d)] yields a single set of
parameters: κ ¼0.55μs−1 , Γ¼0.14μs−1 , and γ d ¼1.49 μs−1 .
Next, we calculate the third-order correlations
gð3Þ ðs1 ; s2 ; s3 Þ [Eq. (1)] from the outgoing photon traces.
A natural choice for the visualization of these correlations pffiffiffi
is to transform to Jacobi coordinates
pffiffiffiffiffiffiffiffi R ¼ ðs 1 þs 2 þs 3 Þ= 3,
pffiffiffi
η ¼ ðs1 − s2 Þ= 2, and ζ ¼ 2=3½ðs1 þ s2 Þ=2 − s3 . Since
we are investigating the response of the superatom to a
pulsed probe, the correlation function is not stationary and
thus depends on the center-of-mass value R as well as on
the relative coordinates η and ζ. Nevertheless, this choice of
coordinates lets us average the gð3Þ function over a limited
range of R, corresponding to times ðs1 ; s2 ; s3 Þ within the
flattop part of the Tukey pulse. In Fig. 2(a), we show the
third-order correlation function gð3Þ ðη; ζÞ for the input
−1
photon rate pffiffiffi Rin ¼ 6.7 μs averaged over the time range
Rrange ¼ 3 × ð2.5…3.5Þ μs [with respect to the time axis
shown in Fig. 1(d)]. While the averaging over R certainly
reduces the visibility of the three-body correlations, it is
essential to extract a significant signal from the few-photon
data for a realistic number of repetitions of the experiment.
Within the theoretical model described above any multi-
time correlation functions for a coherent input pulse are
conveniently calculated using the quantum regression
theorem; alternative approaches using Keldysh formalisms
have also been developed [39]. Note that, for a single
superatom, the quantum regression theorem is exact, as the
103601-3
(a) (b)
FIG. 2. (a) Cut through the experimental third-order correlation
gð3Þ ðs1 ; s2 ; s3 Þ for input photon rate Rin ¼ 6.7 μs−1 along the
η,ffiffiffiζ averaged over the center-of-mass
relative Jacobi coordinates p
coordinate range Rrange ¼ 3 × ð2.5…3.5Þ μs. (b) Correspond-
ing theoretical calculation based on the single-emitter model
using the parameters extracted from the fitted curves in Fig. 1(d).
Note the different scales on the colorbars, the contrast of the
experimentally observed correlations is reduced due to finite
photon detection efficiency (see Supplementary Material [38]).
emitted photons never interact with the system again [40].
For other input photon states, a more sophisticated quantum
field formalism can be employed. The theoretical third-
order correlations based on the parameters extracted from
the time trace fits and averaged over the time range Rrange
are shown in Fig. 2(b), reproducing to very good agreement
the bunching and antibunching features observed in the
experimental data.
To quantify pure three-body correlations in the outgoing
photon stream, we now extract the connected third-order
ð3Þ
correlation function gc by subtracting the two-body
correlations for all pairwise combinations of time coor-
dinates s1 , s2 , and s3 from gð3Þ , as defined in Eq. (2).
ð3Þ
Figures 3(a)–3(c) show cuts gc ðη; ζÞ through the measured
connected three-body correlation function for all three
investigated photon input rates Rin ¼ 3.4 μs−1 , Rin ¼
6.7 μs−1 , and Rin ¼ 15.2 μs−1 averaged over Rrange, deter-
mined from the measured second- and third-order corre-
lation functions. Even for low photon numbers, we find a
clear signal of three-photon correlations in the connected
part of gð3Þ with a three-photon bunching at short distances,
accompanied by an antibunching at intermediate separa-
tions, followed by another ring of bunching. This sequence
of bunching and antibunching features increases with
increasing photon numbers. Note that gð3Þ for a transla-
tionally invariant system exhibits a sixfold symmetry in
Jacobi coordinates. The reduction to a threefold symmetry,
visible in particular in Fig. 3(c), is a consequence of the
finite length of our probe pulse. In Figs. 3(d) and 3(e), we
show the corresponding theoretical predictions from our
quantitative model, which well reproduce the observed
structure in the experimental data.
 PHYSICAL REVIEW LETTERS 121, 103601 (2018)
(a) (d)
(b) (e)
(c) (f)
FIG. 3. Connected part of the three-photon correlation function
ð3Þ
gc in the Jacobi coordinates η, ζ. (a)–(c) show experimental results
for Rin ¼ 3.4 μs−1, Rin ¼ 6.7 μs−1 , and Rin ¼ 15.2μs−1 , respec-
tively. (d)–(f) show the corresponding theoretical predictions.
While this agreement between the theory and experiment
suggests that our simple single-emitter model captures the
physics of the superatom-light interaction and the effective
photon-photon interaction mediated through the superatom
very well, it is not straightforward to understand the
microscopic origin for the appearance of three-photon
correlations from this model. In order to provide a micro-
scopic and qualitative understanding of these correlations,
we turn to the theoretical study of an idealized setup, which
allows for a fully analytical solution. For this purpose, we
point out that the Hamiltonian Eq. (3) is exactly solvable
via the Bethe ansatz [41]. While such an approach ignores
the additional dephasing and spontaneous emission of the
excited state, it allows us to gain a microscopic under-
standing of the possible correlations induced by a single
superatom. A first important aspect is that the exact
eigenstates for three photons can be characterized as a
three-photon bound state, a combination of a two-body
bound state with an additional scattering photon, and
finally pure scattering states [41]. Especially, the three-
photon bound state naturally provides a nontrivial contri-
bution to the connected part of the correlation function. A
second important aspect is the relation between the out-
going wave function and the incoming photon wave
function, which for the considered problem can be derived
in a closed form [42]. For the present setup, we are
103601-4
(a) (b)
FIG. 4. Three-photon correlation functions derived from the
ð3Þ
wave function ψ out of the exactly solvable idealized model in
the Jacobi coordinates η, ζ. (a) The correlation function gð3Þ
exhibits strong three-photon bunching at η ¼ ζ ¼ 0, with a
subsequent antibunching and finally saturation at gð2Þ if one
photon is separated from the other two. (b) The connected part
ð3Þ
of the correlation function gc still shows a strong nontrivial
contribution.
Q
interested in an incoming state ψ in ¼ i ψðsi Þ for n
photons in the single photon mode ψ with width τ.
Then, the outgoing n-photon wave function after interact-
ing with a single superatom at times s1 ≥    ≥ sn reduces
to (see Supplemental Material [38])
P
ðnÞ
ψ out ðs1 ;…;sn Þ ¼ ∂ α1 …∂ αn eðκ=2Þ i ðsi −2αi Þ ϕðs1 − α1 Þ

Y n 
× ½ϕðsi −αi Þ −ϕðsi−1 þαi−1 Þ ð5Þ
i¼2 αi ¼0
R
with ϕðsÞ ¼ s∞ dtψðtÞe−κt=2 ; the wave function for all
values of fsi g is obtained by requiring the bosonic
symmetry of the wave function. For three photons in a
wide incoming mode τκ ≫ 1, the wave function in the
center of the pulse reduces to (s1 ≥ s2 ≥ s3 )
ð3Þ
ψ out ¼ 1 þ 12e−κ½ðs1 −s3 Þ=2 − 4ðe−κ½ðs1 −s2 Þ=2 þ e−κ½ðs2 −s3 Þ=2 Þ;
ð6Þ
from which we can analytically derive the three-body
correlation functions shown in Fig. 4. We find a very
strong three-photon bunching around η ¼ ζ ¼ 0. The
contribution of the three-body bound state to this signal
can be observed by the decomposition of the wave function
ð3Þ
ψ out ¼ 4e−κðs1 −s3 Þ þ ψ sc . The first term describes the three-
body bound state, while ψ sc accounts for the remaining
contributions of scattering states and two-photon bound
states with ψ sc ¼ 1 at s1 ¼ s2 ¼ s3 . Therefore, the three-
body bound state provides the dominant contribution to
the three-photon bunching signal, but contributions of
the remaining states are still significant. Especially, the
 PHYSICAL REVIEW LETTERS 121, 103601 (2018)
exponential decrease of the bunching signal at s2 ¼ s3
exhibits a decay κ instead of the faster decay 2κ expected
from the three-body bound state wave function.
Comparing this result with the experimentally observed
correlation functions, we find that the idealized setup exhibits
the characteristic features of three-photon bunching at
short distances and antibunching at intermediate distances
observed in the experiment for low photon numbers. We
expect, therefore, that the microscopic origin of the three-
body correlations in the experiment are well captured by an
understanding of the idealized model as the combination of
a three-photon bound state, scattering states, and two-photon
bound states. Note that the width of these signals is increased
due to the reduced losses in the idealized setup. Furthermore,
the appearance of oscillations for higher number of photons
can be understood as the single emitter undergoing Rabi
oscillations, which gives rise to a characteristic beating for
an increasing photon number.
In conclusion, the experimental observation of three-
photon correlations imprinted by a single Rydberg
superatom on an initially uncorrelated photonic state is
well accounted for by a single-emitter model, where the
dephasing of the collectively excited state as well as the
spontaneous decay are included. On a microscopic level,
the appearance of the three-photon correlations is well
understood in an idealized setup, which suggests that the
observed three-photon bunching signal here cannot be
purely attributed to a three-photon bound state in contrast
to recent observations on Rydberg polaritons [28].
Observing such three-photon correlations imprinted by
a single two-level systems sheds light on the fundamental
processes of absorption and emission at the quantum level
and highlights the potential for experimentally realizing
photonic strongly correlated many-body systems in quan-
tum nonlinear optical systems. Besides further improving
the emitter-light coupling and investigating intrinsic
superatom dephasing mechanisms, we envision the scal-
ing of our system to more complex arrangements of
multiple superatoms for implementing quantum optical
networks [1,3].
We thank Florian Christaller and Simon W. Ball for
contributing to the construction of the experimental setup.
This work is supported by the European Union under
the ERC consolidator grants SIRPOL (Grant No. 681208)
and RYD-QNLO (Grant No. 771417) and the Deutsche
Forschungsgemeinschaft (DFG) under SPP 1929 GiRyd
Project No. HO 4787/3-1. A. P-M. acknowledges support
from UNAM-PAPIIT IA101718 RA101718.
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