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Photon-Phonon Atomic Coherence Interaction of Nonlinear Signals in

Various Phase Transitions Eu 3+ : BiPO4

Article in Nanomaterials · December 2022

DOI: 10.3390/nano12234304

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Article

Photon–Phonon Atomic Coherence Interaction of Nonlinear

Signals in Various Phase Transitions Eu3+: BiPO4
Huanrong Fan 1,†, Faizan Raza 2,†, Irfan Ahmed 3,4, Muhammad Imran 1, Faisal Nadeem 1, Changbiao Li 1,*,
Peng Li 1,* and Yanpeng Zhang 1,*

1 Key Laboratory for Physical Electronics and Devices of the Ministry of Education & Shaanxi Key Lab of
Information Photonic Technique, Xi’an Jiaotong University, Xi’an 710049, China
2 State Key Lab of Modern Optical Instrumentation, Centre for Optical and Electromagnetic Research,

College of Optical Science and Engineering, International Research Center for Advanced Photonics,
Zhejiang University, Hangzhou 310027, China
3 Department of Electrical Engineering, Sukkur IBA University, Sukkur 65200, Pakistan

4 Department of Physics, City University of Hong Kong, Hong Kong SAR 99907, China

* Correspondence: cbli@[Link] (C.L.); ponylee@[Link] (P.L.);

ypzhang@[Link] (Y.Z.)
† These authors contributed equally to this work.

Abstract: We report photon–phonon atomic coherence (cascade- and nested-dressing) interaction

from the various phase transitions of Eu3+: BiPO4 crystal. Such atomic coherence spectral interaction
evolves from out-of-phase fluorescence to in-phase spontaneous four-wave mixing (SFWM) by
changing the time gate. The dressing dip switch and three dressing dips of SFWM result from the
strong photon–phonon destructive cross- and self-interaction for the hexagonal phase, respectively.
Citation: Fan, H.; Raza, F.; More phonon dressing results in the destructive interaction, while less phonon dressing results in
Ahmed, I.; Imran, M.; Nadeem, F.; the constructive interaction of the atomic coherences. The experimental measurements of the pho-
Li, C.; Li, P.; Zhang, Y. ton–phonon interaction agree with the theoretical simulations. Based on our results, we proposed a
Photon–Phonon Atomic Coherence model for an optical transistor (as an amplifier and switch).
Interaction of Nonlinear Signals in
Various Phase Transitions Eu3+: Keywords: atomic coherence; spectral interaction; phonon/photon dressing; spontaneous
BiPO4. Nanomaterials 2022, 12, 4304. four-wave mixing
[Link]
nano12234304

Academic Editor(s): Carlos Baleizão,

Ermelinda M.S. Maçôas and Onofrio 1. Introduction
M. Marago
In the past years, it was desirable to couple a single atomic-like spin to a supercon-
Received: 16 October 2022 ducting qubit, where a nanomechanical resonator is coupled to a two-level system to in-
Accepted: 2 December 2022 duce strong phonon–phonon interactions [1,2]. However, the entanglement generated is
Published: 4 December 2022 affected by different systems in a traditional method that often needs a strong spin–pho-
Publisher’s Note: MDPI stays neu-
non interaction to exceed the decay of the phonons [3,4]. Phonon dispersion relation and
tral with regard to jurisdictional
lattice-spin coupling of Eu3+ have been reported [5,6]. A thermal phonon at elevated tem-
claims in published maps and institu- peratures, lattice vibration structural transition, and thermal expansion behavior in
tional affiliations. LaPO4: Eu have also been studied [7].
Recently, the photon–phonon dressing coupling in Eu3+ ions doped BiPO4 has been
studied [8,9], as Eu3+/Pr3+ ions are very sensitive to the site symmetry and its surrounding
crystal field of the host material compared to other crystal ions [10–12]. Therefore, it can
Copyright: © 2022 by the authors. Li- be achievable to obtain such a potential application in BiPO4 crystal. The crystal structure
censee MDPI, Basel, Switzerland. of BiPO4 has two polymorphic forms, monoclinic (M) and hexagonal (H) phases. The dif-
This article is an open access article ference in the symmetry of the lattice structure results in different interactions [13,14]. The
distributed under the terms and con- H phase of crystal is more structurally asymmetric than the M phase in Eu3+ because of a
ditions of the Creative Commons At- more atomic-like system. Bismuth phosphate (BiPO4) has drawn significant attention as a
tribution (CC BY) license ([Link] host medium for doping lanthanide ions due to its comparable ionic radius of Bi3+(1.11 Å)
[Link]/licenses/by/4.0/).
with that of lanthanide ions [15–17].

Nanomaterials 2022, 12, 4304. [Link] [Link]/journal/nanomaterials

Nanomaterials 2022, 12, 4304 2 of 16

The Eu3+: BiPO4 is one of the most promising atomic-like mediums known for its long
coherence time (ms) [8] due to photon–phonon coupling in doubly dressed states with
potential applications in quantum memory [18–20].
Interactions of doubly dressed states and the corresponding properties of atomic sys-
tems have attracted considerable attention in recent decades. In this regard, two kinds of
doubly dressed processes (in cascade- and nested-parallel schemes) were reported in an
open five-level atomic system [21,22]. Nie et al. theoretically investigated the similarities
and differences between different kinds of single dressing schemes for six-wave mixing
to examine the interaction between multi-wave mixing in a five-level atomic system [23].
Next, we will consider such multi-nonlinear signals’ interaction with the coupling of
a lattice vibration phonon and photon dressing.
In this paper, we investigated two multi-dressing cross-interactions obtained from
the various phase transitions of Eu3+: BiPO4 crystal by changing the time gates. The spec-
tral cross-interaction evolves from out-of-phase FL, to hybrid (FL+SFWM), and to in-phase
SFWM (anti-Stokes signal). Moreover, we demonstrate that the FL and SFWM destructive
interaction results from more phonon dressing, and such dressing is achieved with a mul-
tiparameter temperature (300 K), H phase, and broadband excitation.

2. Experimental Scheme
The ion PO43−: [Bi3++Eu3+] has five molar ratios (7:1, 20:1, 6:1, 1:1, 0.5:1) for the Eu3+:
BiPO4 sample with different lattice vibration structures. In our experiment (Figure 1a), we
used five BiPO4 samples with different combinations and concentrations of a pure H phase
and low-temperature monoclinic phase (LTMP), where the H phase refers to C2, and
LTMP refers to the C1 site symmetry, respectively. The sample (7:1) corresponds to the
pure M phase, (20:1) corresponds to the mixed [more M (75%) + less H (25%)] phase, (6:1)
corresponds to the mixed [half H (50%) + half M (50%)] phase, (1:1) corresponds to the
mixed [less H (25%) + more M (75%)] phase, and (0.5:1) corresponds to the pure H phase.
The concentration of the Eu3+ ions is 5% consistent across all five samples with different
phase transitions. Figure 1c shows the fine structure energy levels of the Eu3+: BiPO4 crys-
tals. The Eu3+: BiPO4 has the ground state 7F1 and excited state 5D0 (mj = 0). The ground
state 7F1 can split into mj = −1 (587.3 nm), mj = 0 (592.3 nm), and mj = +1 (597.3 nm) under
the crystal field effect of the BiPO4 crystal and dressing effect.
To implement the experiment, Eu3+: BiPO4 samples were held in a cryostat (CFM-
102). The temperature was controlled through liquid nitrogen from 300 K (large phonon
Rabi frequency G Tpi with more thermal phonons) to 77 K, where G Tpi = − μ kl E pi /  is the
Rabi frequency of the phonon field (I = 1, 2; T= (T1, T2) = (300 K, 77 K)). The μ kl is the
dipole moment between |k〉and |l〉 of the crystal field splitting in the 7F1 state (Figure 1b),
E pi is the phonon field, where such phonon builds atomic coherence for the crystal field
splitting in 7F1.
In the experiment, the G Tpi and phase transition detuning j
Δ pi are controlled by the
temperature and different samples, respectively. The frequency detuning of the phonon
field is Δ pij = Ω kl − ω pij (j = a (7:1), b (20:1), c (6:1), d (1:1), and e (0.5:1) sample), as shown in
Figure 1b, where Ωkl is the frequency between |k〉 and |l〉. The ω pij is the phonon fre-
quency of the phonon field, which is determined by the vibration frequency of the crystal
lattice state mode. The different frequencies of the phase transitions ( ω api < ω epi , Δ api > Δ epi )
can couple to the different lattice vibrations for Eu3+: BiPO4, resulting in different phonon
dressing ( | G Tp i | 2 / i Δ ap i < | G Tp i |2 / i Δ ep i ).
Nanomaterials 2022, 12, 4304 3 of 16

Figure 1. (a) Experimental setup, (b) Shows photon and phonon four-dressing energy level. (c)
Shows energy levels of Eu3+: BiPO4 for transition 7F1→5D0. (d) The schematic diagram of proposed
optical transistor as an amplifier and switch.

Figure 1a shows the schematic diagram of the experimental setup. Here, we used two
tunable dye lasers (narrow scan with a 0.04 cm−1 linewidth) pumped by an injection-
locked single-mode Nd3+: YAG laser (Continuum Powerlite DLS 9010, 10 Hz repetition
rate, 5 ns pulse width) to generate the pumping fields, broadband E1 (ω1, Δ1) and
narrowband E2 (ω2, Δ2). The broadband excitation E1 couples to more crystal field splitting
levels 5D0 and 7F1 (Figure 1b), resulting in more lattice vibration (phonon dressing).
However, the narrowband excitation E2 couples to fewer splitting levels, resulting in less
lattice vibration. The frequency detuning here is Δi = Ωmn − ωi , where Ω mn is the
frequency between the crystal field splitting levels 5D0 and 7F1, and ω i is the optical
frequency. The Rabi frequency of the optical field is defined as Gi = − μ mn Ei /  , where μmn
is the dipole moment of the crystal field splitting with the different states 5D0 and 7F1
excited by the Ei between the levels |m〉and |n〉, as shown in Figure 1b. Such a photon
builds the atomic coherence of the crystal field splitting with the different states (5D0 and
7F1). The pulse generated from the Nd3+: YAG laser is used to simultaneously trigger a

boxcar-gated integrator and oscilloscope. The input laser beams are along the [010] axis
of the BiPO4 crystal, which is perpendicular to the optical axis. The spectral optical outputs
are obtained by scanning the laser frequency. The grating motor of the two dye lasers is
scanned by a computer to form the x-axis, and the intensity of the excitation spectrum is
the average of ten shots from the gated integrator (Figure 1a) appearing on the y-axis.
The optical signal generated from the Eu3+: BiPO4 crystal is detected via confocal
lenses and photomultiplier tubes (PMTs). In our experimental setup, PMT1 is precisely
placed to detect the narrowband FL and spontaneous four-wave mixing (SFWM) signal,
whereas PMT2 is placed to detect the broadband FL and SFWM signal. Such a detector
placement is based on the different distances from the detector to the sample (Figure 1a).
Hence, the PMT affects the ratio of out-of-phase FL and in-phase SFWM. The out-of-phase
FL1 signal and FL2 signals are generated through the excitation of the E 1 and E 2
lasers, respectively. The in-phase E s1 signal is generated by a combination of the E 1
Nanomaterials 2022, 12, 4304 4 of 16

and reflection E 1′ under the phase-matched condition ( k 1 + k 1′ = k S + k AS ). At the same

time, the spectral signals from the different energy levels with different lifetimes can be
obtained through boxcar-gated integrators which can be controlled from the time gate.
The time gate can control the ratio of out-of-phase FL and ES/AS.
Therefore, the photon–phonon atomic coherence interaction can be controlled by
changing the time gate, broadband/narrowband excitation, and thermal/phase transition
phonon.

2.1. Theoretical Model

2.1.1. Photon–Photon Atomic Coherence Cross-Interaction
The single laser or two lasers excitation shows photon dressing. Different lattice
vibrations produced different frequency phonons. Such different frequency phonons can
match to different crystal field splitting levels 5D1−7F1, 5D0−7F1, and 5D0−7F3 in the ion Eu3+,
so more phonon results in effective dressing. The three sharp dips are hard to be explained
only by photon field dressing. Therefore, the phonon can be used to explain the three
sharp dips. The cross-interactions, which evolve from FL to hybrid (coexistence of second
order FL and SFWM), to SFWM are below
| ρ F( 2)1 + ρ F( 22) | 2 = | ρ F( 21) |
2
+ | ρ F( 22) 2
| +2 | ρ F( 21) || ρ F( 22) | cos(θ F ) (1)

(3) (3) (3) 2 (3) (3) (3)

| ρ AS 1 + ρ AS 2
2
| =| ρ AS 1 | + | ρ AS 2 |
2
+2 | ρ AS 1 || ρ AS 2 | cos(θ AS ) (2)

| ρ HX 2
| =| ρ F( 21) + ρ F( 2)2 + ρ S(3)1 + ρ S(3)2 |
2
(3)
When the laser fields E1 and E2 are applied, the density matrix elements of out-of-
phase FL for the [H+M]-phase Eu3+: BiPO4 via perturbation chain ρ11(0) ⎯E→ (E )
1 ρ (1) ⎯⎯
12 → ρ 22 (2) and 1
*

(0) E2
*
(1) ( E ) (2) 2 2
ρ00 ⎯→ ρ 20 ⎯⎯→ ρ 22 (2)
2 can be written as ρ F 1 = − | G1 | /(( Γ 12 + i Δ 1 + | G 2 | /( Γ 02 + i ( Δ 1 -Δ 2 ))) Γ 22 ) ,
ρ F 2 = − | G 2 | /(( Γ 20 + i Δ 2 + | G1 |2 /( Γ 21 − i ( Δ 1 -Δ 2 ))) Γ 22 ) , where ρ F( 21) = | ρ F( 21) | e iθ1 , ρ F( 22) = | ρ F( 2)2 | e iθ 2 ,
(2) 2

θ F = θ1 − θ 2 . In the Λ-type three-level system, the third-order density matrix elements

ρ A( 3S) via (0) E1
ρ11 (1) E
⎯→ ρ 21 ⎯→ ρ 22 (2) E1′
⎯→ ρ 20((3) S
AS )
can be written as
(3) (3)
(3)
ρ AS 2
= − iG S G1G1′ / (( Γ 21 + i Δ1 )( Γ 22 + i Δ1 + | G2 | /( Γ 20 + i Δ1 -i Δ 2 ))( Γ 20 + i Δ1 + i Δ1′ )) , where ρ AS 1 =| ρ AS 1 |e
iθ AS 1
,
(3)
ρ AS 2 =|
(3)
ρ AS 2 |e
iθ AS 2
, θ AS = θ AS1 − θ AS 2 . The Γ ij = (Γ i + Γ j ) / 2 is the transverse decay rate, where
Γ i / j = Γ pop + Γ ion − spin + Γ ion − ion + Γ phonon + Γ dres sin g . Γ phonon is more related to the broadband
excitation.
In physics, the ρ F( 21) generated from the field E1 contains external field dressing
(2)
| G2 |2 , and ρ F 2 from the field E2 contains external field dressing | G1 |2 , as shown in
Figure 2. Therefore, the | ρ F( 21) + ρ F( 22) | 2 shows the photon2 and photon1 dressing cross-
interaction of the FL signal [16] at the profile E1/E2 resonance, as shown in Figure 3. In
Equations (2) and (3), the | ρ A(3)S 1 + ρ A(3)S 2 | 2 and ρ F( 2)1 + ρ F( 2)2 + ρ AS
(3) (3) 2
1 + ρ AS 2 | are similar to the
(2) (2) (3) (3)
| ρF1 + ρF 2 | with two single external dressings. Therefore, the | ρ
AS1 + ρ AS 2 | (Figures 4–7)
2 2

and | ρH | (Figure 7) show the cross-interaction of the SFWM and hybrid signals,
X 2

respectively.

2.1.2. Photon–Phonon Atomic Coherence Self-Interaction

The self-term | ρ F( 22) | 2 (or | ρ F( 21) | 2 ) is taken from in Equation (1) with the external
dressing. The phonon1 dressing | G Tp 1 | and internal dressing | G2 |2 (or | G1 |2 ) are 2

included in the self-term | ρ ′′ | =| − | G 2 |2 /(( Γ 20 + i Δ 2 + d1 ) Γ 00 |2 with the broadband E1

(2)
F2
2

dressing (or | ρ F′′(12) |2 =| − | G1 |2 /(( Γ12 + i Δ 1 + d 2 ) Γ 22 |2 with the broadband E1 generation),

where d1 =|G Tp1 |2 /( Γ 10 + i Δ 2 -i Δ pj 1 )+ | G1 |2 /( Γ 21 + i Δ 2 -i Δ 1 ) (or
Nanomaterials 2022, 12, 4304 5 of 16

d 2 =|G Tp1 |2 /( Γ 10 + i Δ 1 + i Δ pj 1 )+ | G 2 |2 /( Γ 02 + i Δ 1 -i Δ 2 ) ). For example, the | ρ F′′(2)

2 |
2
with two cascade
dressings is expanded as follows
| ρ F′′(2) 2 (2)
′(4)
2 | =| ρ F 2 + ρ F ′′(4)
2 +ρ F 2 |
2
(4)

The | ρ F′′ (22 ) |

2
and contain | ρ F′′(2)
| ρ F′′ (12 ) 2
|
2
′′(2) ′′(2) ′′ ) in Equation (4) and
2 | +2 | ρ F 1 || ρ F 2 | cos(ϕ F
(2) 2 (2) (2)
′′ ) , which show the out-of-phase FL2 and FL1 self-interaction of
| ρ F′′ 1 | + 2 | ρ F′′ 1 || ρ F′′ 2 | cos(ϕ F

the two lasers, respectively. However, when the external field dressing is neglected at off-
resonance, the Equation (4) becomes one laser self-interaction of FL.
The photon1 excites atomic coherence ( Γ12 and ρ12 ) between |1〉 and |2〉 couples to
the phonon1 atomic coherence by a common level |1〉 (Figure 1b) in | ρ F′′(2) 2
2 | . The photon2

excites atomic coherence ( Γ20 and ρ20 ) between |0〉 and |2〉. By using Taylor expansion
for cascade dressing, the dressing (atomic coherence) coupling effect is transferred into
the nonlinear generating process in Equation (4). Thus, we obtain the generating
Hamiltonian H = i κ F α 1†α 2†α †p 1 + H .c . for sixth-order nonlinearity, where
κ F = − iϖ F χ ( 6 ) E F E 1 E 2 E p 1 / 2 . The ϖ F is the central frequency of FL.
Next, the difference from the self-term | ρ AS
(3)
2 |
2
(or | ρAS(3)1 |2 ) in Equation (2), the internal
2 2
dressing | G2 | (or | G1 | ) and two phonon dressings ( | G Tp 1 | 2 and | G Tp 2 |2 ) are included in
(3) (3) (3) (3)
ρ′′′′
AS 2 (or ρ′′′′
AS1 ). Where ρ ′′′′
AS 2 = − iG S 2 G 2 G 2 / d 0 (or ρ ′′′′
AS 1 = − iG S 1G1G1′ / (( Γ 21 + i Δ 1 ) d 2 d 3 ) ),

d 0 = ( Γ 20 + i Δ 2 + d1 + |G1 |2 / ( Γ 21 + i Δ 2 − i Δ 1 ))( Γ 22 + i Δ 2 )( Γ 20 + 2 i Δ 2 )
,
d2 = Γ20 +iΔ1′ +iΔ1
2
d 1 = | G 2 | / ( Γ 20 + i Δ 1 + | G Tp 1 |2 / ( Γ 01 + i Δ 1 - i Δ j T 2
p 1 + |G p 2 | / ( Γ 31 + i Δ 1 - i Δ j j
p 1 + Δ p 2 ))
, ,
d3 =Γ22 + iΔ1 + d4 + d6 2
d 4 = |G 2 | / ( Γ 20 + i Δ 1 + i Δ 2 + d 5 )
, ,
d 6 = |G1 |2 / ( Γ 20 + 2 i Δ 1 )
d 5 = | G Tp 1 |2 / ( Γ 01 + i Δ 1 + i Δ 2 - i Δ j T 2
p 1 + |G p 2 | / ( Γ 31 + i Δ 1 + i Δ 2 - i Δ j j
p1 + Δ p 2 )
, . The
(3) 2
| ρ ′′′′
AS 1 | with the four cascade-nested dressing is expanded as follows
(3) 2 (3) (5) (5) (7) (9 ) 2
| ρ ′′′′
AS 1 | = | ρ AS 1 + ρ AS 1 + ρ ′AS 1 + ρ AS 1 + ρ AS 1 | (5)
The in-phaseanti-Stokes | ρ ′′′′
AS 2 |
2
and | ρ ′′′′
AS 1 |
2
contain
(3) 2 (3) (3) (3) 2 (3) (3)
′′′′
| ρ AS 2 | + 2 | ρ AS 1 || ρ AS 2 | cos(θ AS )
′′′′ ′′′′ ′′′′ in Equation (5) and ′′′′
| ρ AS 1 | + 2 | ρ AS 1 || ρ AS 2 | cos(θ AS
′′′′ ′′′′ ′′′′ ) ,

which show anti-Stokes2 and anti-Stokes1 self-interaction of the two lasers, respectively.
When the external dressing is neglected at off-resonance, Equation (5) becomes one laser
self-interaction of anti-Stokes.
The phonon1 excites atomic coherence ( Γ10 and ρ10 ) between |0〉 and |1〉. The
phonon2 excites atomic coherence ( Γ31 and ρ31 ) between |1〉 and |3〉 (Figure 1b). In the
(3)
four nested-cascade dressing of ρ′′′′ AS 2 , the atomic coherence from the nested coupling

among the photon1, phonon1, and phonon2, couples with the atomic coherence of the
photon2 (Figure 1b) in a cascaded manner. Similar to Equation (4), the dressing coupling
effect is transferred into the nonlinear generating process in Equation (5). Thus, we also
obtain the generating Hamiltonian which can be written as H 2 = i κ A S α 1†α 2†α †p 1α †p 2 + H .c . for
ninth-order nonlinearity, where κ S = − iϖ AS χ ′( 9 ) E A S E S E1 E 2 E p1 E p 2 / 2 . The ϖ AS is the
central frequency of anti-Stokes.

2.1.3. Simulation of Nonlinear Signals Dressing Interaction

Figure 2a shows the FL1 and FL2 self-terms | ρ F( 21) | 2 + | ρ F( 22) |2 , the cross-term
2 | ρ F 1 || ρ F 2 | cos(θ F ) in the cross-interaction of the two lasers | ρ sum |
(2) (2) (2) 2
at Δ1 = Δ 2 / 2 versus the
detuning difference Δ = Δ1 − Δ2 from Equation (1), respectively. | ρ F( 21) | 2 and | ρ F( 22) | 2 have
the maximal values at Δ = ±4.1 THz and Δ = ±3.6 THz, respectively. Hence, there exist
two peaks at around Δ = ±10 THz in the hot curve that represents the cross-interaction
| ρ sum | . The purple curve shows the cross-term 2 | ρ F 1 || ρ F 2 | cos(θ F ) . Here, the value below
(2) 2 (2) (2)
Nanomaterials 2022, 12, 4304 6 of 16

or above zero suggests destructive or constructive interference, respectively. In fact, the

variations of the phase difference between the second-order FL1 and FL2 change the
constructive interaction into destructive interaction, and vice versa. Furthermore, by
ρ F( 2)1 =| ρ F( 2)1 | e iθ1 and ρ F(2)2 =| ρ F(2)2 | e iθ2 , we obtain | ρ F( 21) + ρ F( 21) | 2 − | ρ F( 21) | 2 − | ρ F( 22) | 2 = 2 | ρ F( 21) | ρ F( 21) | cos(θ F )
from Equation (1). Figure 2b shows the phases θ 1 , θ2 , and the phase difference θ F
versus Δ as given in Table 1. As the θ1 and θ2 are changed, the θ F alternates between
−0.7π and 0.7 π . The interaction switches from constructive ( [−0.7π ,0.5π ) ), destructive (
[0.5π ,0.7π ) ), constructive ( [−0.5π ,0.5π ) ), and destructive ( [−0.7π, −0.5π) ) and constructive (
[−0.5π ,0.7π ) ) as given in Table 2. Our simulation (Figure 2) is obtained by scanning
Δ =Δ 2 − Δ1 [23], and our experimental result (Figures 3–7) is gained by scanning the
dressing field Δ 2 .For simplicity, we only considered the external dressing in simulation
Equation (1). Furthermore, Equations (1)–(3) reveal the cross-interaction of the two lasers.
If the internal dressing and phonon dressing are considered, the cross-interaction becomes
complicated.

Figure 2. (a1) The total signal intensity of | ρ F( 21 ) |

2
+ | ρ F( 22) |
2
(hot curve), (a2) the interaction item
2 | ρ F( 21 ) || ρ F( 22) | c o s (θ ) versus Δ (purple curve), (a3) | ρ (2) 2
sum | (green curve), (a4) | ρ F( 21 ) |
2

(blue curve), (a5) | ρ F( 22) |

2
(black curve). Figure 2b: The parameters are G1 = 2.3 THz, G2 = 6.1 THz.
(b1) θ F (hot curve), (b2) θ1 (black curve), (b3) θ 2 (blue curve) versus Δ . Evolution of θ F , the
constructive and the destructive interaction versus Δ . Figure 2b: The destructive or constructive
interaction is studied in this system [23].

Table 1. Experimental parameters, Variables in the equations and Corresponding definition.

Experimental Parameters Variables Corresponding Definition

Time gate ρ F( 2 ) /ρ AS
(3)
FL/SFWM density matrix
Temperature Gi / G Tpi Photon Rabi frequency /phonon Rabi frequency
Sample
Band excitation j Photon frequency detuning/phonon frequency
Δ i / Δ pi
detuning
PMT
θ Fi FL phase

Table 2. Evolution of θ F , the constructive and the destructive interference versus Δ .

Δ = Δ1 − Δ 2 [ −10, −1.1) [−1.1, −0.2) [ −0.2, 0.2) [0.2, 1.1) [1.1, 10]
θ F = θ1 − θ2 [ −0.7π , 0.5π ) [0.5π , 0.7π ) [ −0.5π , 0.5π ) [ −0.7π , −0.5π ) [ −0.5π , 0.7π ]
interaction constructive destructive constructive destructive constructive
Nanomaterials 2022, 12, 4304 7 of 16

2.2. Experiments
The photon excitation atomic coherence between the different states (5D0 and 7F1) can
be coupled to the phonon excitation atomic coherence in the same state (7F1). Unlike the
photon atomic coherence of the crystal field splitting with the different states, the phonon
atomic coherence of the crystal field splitting in the same state is difficult to optically
excite.
Moreover, the phonon dressing can control the destructive and constructive
interaction. The constructive interaction results from less phonon dressing (77 K, M phase,
narrowband E2), whereas the destructive interaction is caused by more phonon dressing
(300 K, H phase, broadband E1).

2.2.1. FL Dressing Cross- and Self-Interaction

Figures 3–7 show the connected spectrum of the dressing cross-interaction of the two
lasers with a different bandwidth. The spectrum profile of such interactions can be
achieved by connecting several spectra together by scanning Δ 2 / Δ1 at a different
detuning ( Δ1 / Δ 2 ) and can be written as | ρ F /AS 1 + ρ F / AS 2 |2 =R1 (θ F / AS ) + N1 (θ F / AS )=R2 (θ F / AS ) + N 2 (θ F / AS ) .
When the Δ i (i = 1, 2) is scanned, the Ri and N i show a resonance and non-resonance
profile term, respectively. The broad peak ( N i (θ F / AS = 0) profile) and broad dip ( N i (θ F / AS = π )
profile) in Figures 3–7 show the constructive and destructive interaction, respectively.
Figure 3a,b,e,f show the constructive cross-interaction of FL (sharp peak Ri (θ F = 0) ,
broad peak Ni (θ F = 0) (profile)) at the E1/E2 resonance. When the time gate is fixed at 1
μs, the FL emission turns out to be dominant. The increasing sharp peaks at the E1
N2 (θF = 0) , as shown in Figure 3(a3,e3), and E2 N1 (θ F = 0) , as shown in Figure 3(b3,f3), in
off-resonance come from a constructive cross-interaction due to | ρ F(2)1 + ρ F(2)2 |2 from
Equation (1). Such an increasing sharp peak comes from the (6:1) sample and is recorded
at a far detector position. Moreover, the broad peaks Ni (θ F = 0) , as shown in Figure
3a,e,b,f, come from a single dressing constructive cross-interaction N1 (θ F = 0) and
N2 (θF = 0) , respectively, which agrees with the two single external dressing simulations
illustrated in Figure 2(a3). The sharp peaks at E1, as shown in Figure 3a,e and at E2, as
shown in Figure 3b,f in off-resonance result from the self-interaction with the internal
dressings | G2 |2 and | G1 |2 , respectively.

(6:1) phase-Eu3+:BiPO4 (1:1) phase-Eu3+:BiPO4

(a1) (a2) (a3) (a4) (a5) (b3)
(b1) (b2) (b4) (b5) (e1) (e2) (e3) (e4) (e5) (f1) (f2) (f3) (f4) (f5)
Intensity

Intensity

565 590 615 Wavelength(nm) 565 590 615 Wavelength(nm)

(c4) (c5)
(c1) (c2) (c3)
Intensity
Intensity

(d5) (h5)
(d4) (h1)
(h4)
(d1) (d2)
(g1) (g5)
(d3) (g2) (h2) (h3)
(g3) (g4)
A
565 590 615 Wavelength(nm) 565 590 615 Wavelength(nm)

Figure 3. (a,c) show self- and cross- interaction of FL observed from Eu3+ doped BiPO4 [molar ratio
(6:1)] at different E1 wavelengths (567.4 nm, 584.4 nm, 587.4 nm, 589.4 nm, 612.4 nm) and E2 scanned
from 567.4 nm to 607.4 nm at PMT1 (far detector position) and PMT2 (near detector position),
respectively. (b,d) show self- and cross- interaction of FL at different E2 wavelengths (567.4 nm, 587.4
nm, 588 nm, 588.4 nm, 602.4 nm) and E1 scanned from 567.4 nm to 612.4 nm. (e–h) show spectral
signal intensity for (1:1) sample, which is same condition as (a–d). The time gate = 1 μs.
Nanomaterials 2022, 12, 4304 8 of 16

Figure 3c shows the cross-interaction of FL (sharp dip R2 (θF′′ = π ) ) and broad peak
N2 (θF′′ = 0) ) at the E1 resonance. Compared with the sharp peak (Figure 3c) at the E1 off-
resonance, the dressing small dip R2 (θF′′ = π ) at the E1 resonance, Figure 3(c3), results from
the switch of the two cascade dressings (external photon | G1 |2 and phonon1
| G Tp 11 | 2 /( Γ 10 + i Δ cp 1 ) + | G 1 | 2 / ( Γ 20 + i Δ 1 ) in Equation (4). Moreover, the sharp peak R2 (θ F = 0) at
the E1 resonance, Figure 3(a3), is transferred into a small dip R2 (θF′ = π ) , as shown in
Figure 3(c3), due to phonon1 dressing | G Tp 11 |2 /( Γ 10 + i Δ cp 1 ) at the near detector position
(broadband FL). Similar to Figure 3a,b,e,f, the broad peak, as shown in Figure 3c, results
from the constructive cross-interaction N2 (θF′ = 0) with less phonon dressing.
Figure 3d,g,h show the destructive cross-interaction of FL (sharp dressing dip
Ri (θ F′′ = π ) ), broad dip Ni (θF′′ = π ) (profile)) at the E1 resonance. Compared with the sharp
dip at the E2 off-resonance from the destructive self-interaction (Figure 3d), the sharp dip
at the E2 resonance, as shown in Figure 3(d3), increases due to the destructive cross-
interaction R1 (θ F′′ = π ) with the external dressing | G2 |2 of ρ F′′(12 ) in | ρ F′′(12 ) + ρ F( 22) |2 at the
broadband excitation E1 and 300 K. This is because the more crystal field splitting levels
7F1 (Figure 1b) and lattice vibrations are coupled by broadband excitation E1. Moreover,

the 300 K results in more thermal phonons with large GTp11 . The broad dip (Figure 3d)
comes from a stronger destructive cross-interaction N1(θF′′ = π ) with more phonon
dressing. The sharp dressing dips at the E2 off-resonance (Figure 3d) come from the self-
interaction from Equation (4).
The sharp dips at the E1 off-resonance come from the phonon1 dressing
| G Tp 11 |2 /( Γ 10 + i Δ cp 1 ) of ρ F′′ 1 , as shown in Figure 3d. The sharp dip R1 (θ F′′ = π ) at the E1
(2)

resonance results from the cascade dressing | G 2 | 2 + | G p 1 | 2 /( Γ 10 + i Δ 2 + i Δ dp 1 ) of ρ F′′(12 ) , as

shown in Figure 3(d3). Such a cascade dressing coupling results in photon1–phonon2–
phonon1 ( α 1† , α 2† , α p1
† in χ ( 6 ) ) atomic coherence coupling.
Figure 3g corresponds to the simulation (Figure 5g) modelled through Equation (4).
Compared with the sharp dip at the E1 off-resonance, Figure 3g, the sharp dip at the E1
resonance, Figure 3(g3), decreases due to the cross-interaction R2 (θF′′ = π ) with the
phonon1 dressing | G Tp11 |2 /( Γ 10 + i Δ dp1 ) + | G1 |2 from Equation (4) at the narrowband
excitation. The broad dip, as shown in Figure 3g, comes from the strong destructive cross-
interaction N2 (θF′′ = π ) with more phonon dressing. Similar to Figure 3d, the broad dip
(Figure 3h) can be explained by a stronger destructive cross-interaction N1(θF′′ = π ) with the
phonon1 dressing | G Tp11 |2 /( Γ 10 + i Δ dp1 ) + | G 2 |2 of ρ F′′(12 ) . Compared with the small dip at the E1
resonance, Figure 3(c3), the large dip is, as shown in Figure 3(g3), due to the phase
transition phonon dressing | G Tp11 |2 /( i Δ cp1 + i Δ 1 ) < | G Tp11 |2 /( i Δ dp1 + i Δ 1 ) . Such a phonon dressing
dip results from the resonance detuning Δ dp1 ( Δ dp1 < Δ cp1 ), which is due to the high phonon
frequencies ω dp1 ( ω dp1 > ω cp1 ) for the H-phase samples (6:1, 1:1), as shown in Figure 3d,h.
The experimental setup presented in Figure 1a is used to realize the optical transistor
as an amplifier and switch (Figure 1d) where the Eu3+ : BiPO4 crystal behaves as a transistor
with the E1 beam as its input (ain); the E2 is a control signal, aout is the output of the
transistor detected at PMT. The transistor gain (g) depends upon the external dressing
effect which can be controlled through the detuning of the E2 beam [24,25]. In Figure 1d,
the transistor as a peak amplifier1 and dip amplifier2 are realized from the spectral
intensity results presented in Figure 3b,d, respectively. The signal amplification (peak or
dip) results from photon dressing and varies with experimental parameters such as the
position of the PMT, laser detuning (bandwidth) and Eu3+ :BiPO4 sample. At a far PMT
(Figure 3b), only a peak amplication (amplifier1) is observed as FL is weak (no dressing)
whereas strong FL (strong dressing) at a near PMT shows a dip amplication (amplifier2),
as shown in Figure 3d. By exploring the relationship between the transistor amplifier and
Nanomaterials 2022, 12, 4304 9 of 16

laser bandwidth, we observed that the narrowband laser E2 (Figure 3a) has a higher
transistor gain than the broadband laser E1 (Figure 3b). Furthermore, our results show that
(6:1) the Eu3+ :BiPO4 sample has a higher amplication factor than (1:1) Eu3+ :BiPO4.
In contrast to the amplifer, the transistor switch results from the photon–phonon
atomic coherence interaction strongly depend upon several exprimental parameters such
as the sample temperature, laser detuning (bandwidth, power), and molar ratio of the Eu3+
:BiPO4 sample. For example, the (0.5:1) BiPO4 sample has more phonons due to strong
lattice vibrations compared to the (0.5:1) BiPO4 sample. In addition, a higher temperature
will result in more phonons, resulting in prominent spectral switching. To understand the
workings of a transistor as an amplifier, we set the E2 at off-resonance ( Δ 2 ≠ 0 ), then the
amplitude of both the sharp peak in Figure 3(b1), and sharp dip in Figure 3(d1), are very
low. When the detuning of the E2 approaches resonance ( Δ 2 = 0 ), the sharp peak in Figure
3(b3), and dip in Figure 3(d3), amplifies by a factor. The amplification of the spectral
signals can be explained by the high gain (g = 3.6) caused by the strong external dressing
| G2 |2 at the resonance wavelength.
Next, we extend our research and study the cross-interaction of SFWM in the
following Section 2.2.2.

2.2.2. SFWM Dressing Cross- and Self-Interaction

The out-of-phase FL (time gate = 1 μs) interaction is transferred to the in-phase SFWM
interaction (time gate = 500 μs). When the time gate is increased to 5 μs, the SFWM signal
(sharp R i ) is dominant.
Figure 4a shows the constructive cross-interaction of SFWM (two sharp peaks
R1(θ AS = 0) , broad peak N1(θAS = 0) (profile)) at the E1 resonance. Compared with the two
sharp peaks at the E2 off-resonance (Figure 4a), the two sharp peaks, Figure 4(a3), at the E2
resonance also increase due to the constructive interaction R1(θ AS = 0) with | ρ AS
(3) (3) 2
1 + ρ AS 2 |

in Equation (2). Such two sharp peaks can be explained by the crystal field splitting levels
(|1〉,|0〉) due to the high resolution of in-phase SFWM. The broad peak comes from the
cross-interaction N1(θAS = 0) , as shown in Figure 4a.

(a3) (b3)
(7:1) phase- Eu3+:BiPO4

(a1) (a2) (a4) (a5)

(b1) (b2) (b4) (b5)

Intensity

565 590 615 Wavelength(nm)

(20:1) phase- Eu3+:BiPO4

(c1) (c2) (c3) (c4) (c5) (d1) (d2) (d3) (d4) (d5)
Intensity

565 590 615 Wavelength(nm)

Figure 4. (a1–a5,b1–b5) show SFWM cross-interaction observed from Eu3+ doped BiPO4 [molar ratio
(7:1)] at different narrowband laser E2 (567.4 nm, 587.4 nm, 588 nm, 588.4 nm, 602.4 nm) while
broadband laser E1 is scanned from 572.4 nm to 612.4 nm at different broadband laser E1
wavelengths (567.4 nm, 584.4 nm, 587.4 nm, 596.4 nm, 612.4 nm) and narrowband laser E2 is scanned
Nanomaterials 2022, 12, 4304 10 of 16

from 567.4 nm to 607.4 nm at 300 K, respectively, at PMT1. The time gates are 5 μs and 20 μs,
respectively, gate width = 400 ns. (c,d) show SFWM cross-interaction for the (20:1) sample at the
time gate = 10 μs and 20 μs, respectively. The other experimental condition is the same as (a,b),
respectively, at PMT1.

Figure 4b,d show the constructive cross-interaction of SFWM (single sharpest peak
′ = 0) , broad peak N 2 (θ AS
R2 (θ AS ′ = 0) ) at the E1 resonance. Compared with the sharpest peak
′ = 0) at the E1
at the E1 off-resonance (Figure 4b), the amplitude of the sharpest peak R2 (θ AS
resonance, Figure 4(b3), decreases due to the constructive cross-interaction with the
phonon1-assisted G 2 dressing ( G Tp 12 and G 2 share the common atomic coherence)
(| G 1 | 2 + | G Tp 1 |) 2 / ( Γ 10 + i Δ 1 + i Δ ap 1 ) of ρ ′AS(3)2 . Compared with the sharp peak, Figure 4(a3), the
linewidth of such a sharp peak decreases due to less thermal phonons (77 K) with a small
′ = 0) , as shown in
G Tp 12 . The broad peak comes from the constructive interaction N 2 (θ AS
Figure 4(b), with less phonon dressing. However, the sharpest peak, Figure 4b, at the E1
off-resonance is due to the self-interaction.
Figure 4c shows the constructive cross-interaction of SFWM (two sharp peaks
′′ = 0) , broad peak N1(θAS
R1(θ AS ′′ = 0) ) at the E2 resonance. The proportion of the two sharp
peaks accounts for roughly 80% and the proportion of the single sharp dips only accounts
for roughly 20%, as shown in Figure 4c. Compared with the two sharp peaks (the left peak
from splitting energy level mj = − 1 ; the right peak from splitting energy level mj = 0 ) at
the E2 off-resonance, as shown in Figure 4c, two such sharp peaks, Figure 4(c3), at the E2
resonance decrease due to the constructive cross-interaction R1(θ AS ′′ = 0) . The broad peak
(Figure 4c) comes from the constructive interaction N1(θAS ′′ = 0) . The small sharp dip,
Figure 4(c3), at the E2 resonance is obtained from the destructive cross-interaction due to
the phonon1 dressing | G Tp1 |2 /( Γ 10 + i Δ 2 + i Δ bp1 ) + | G 2 |2 in Equation (5).
Compared with the two sharp peaks at the E2 resonance for the (7:1) sample, Figure
4(a3), the small sharp dip at the E2 resonance, as shown in Figure 4(c3), results from the
more phonon dressing ( Δ ap1 > Δ bp1 , | G Tp12 |2 / i Δ ap1 < | G Tp12 |2 / i Δ bp1 ) for H-sample (20:1). Such a small
sharp dip results from the switch of the two cascade dressings (external photon | G2 |2 and
phonon1 | G Tp 11 |2 /( Γ 10 + i Δ bp 1 ) + |G 2 |2 of ρ ′A(3)
S 1 ), because the phonon dressing is easily
distinguished by in-phase SFWM.
Similar to Figure 4(b3), the sharpest peak at the E1 resonance also decreases due to
the constructive cross-interaction R2 (θ AS ′ = 0) with the phonon1-assisted dressing, as
shown in Figure 4(d3).
Figure 5a shows the constructive cross-interaction of SFWM (sharp peak R2 (θ AS = 0) ),
and the broad peak N 2 (θ AS = 0) ) at the E1 resonance. Similar to Figure 4b,d, the sharp
peak, Figure 5(a3), at the E1 resonance decreases compared to the sharp peaks at the E1
off-resonance, Figure 5a, due to the cross-interaction R2 (θ AS = 0) with the phonon1-assisted
dressing (| G1 |2 + | G Tp 11 |) 2 / ( Γ 10 + i Δ 1 + i Δ cp 1 ) of ρ ′AS(3)2 . The broad peak at the E1 off-resonance
comes from the constructive interaction R2 (θ AS = 0) due to less phonon dressing.
Nanomaterials 2022, 12, 4304 11 of 16

(a1) (a2) (a3) (a4) (a5) (b1) (b2) (b3) (b4) (b5) (e1) (e2) (e3) (e4) (e5)
(g1) (g5)

Intensity
(g2) (g4)

(g3)
565 590 615 Wavelength(nm)
(c5) (d2) (d3) (d4) (f3)
(h1)
Intensity

(f1) (f2) (h5)

(f4)
(c3) (h2)
(d1) (f5) (h4)
(c1)
(h2)

(c2) (c4) (d5) (h3)

565 590 615 Wavelength(nm)

Figure 5. (a,c) show SFWM cross- interaction observed from Eu3+ doped in molar ratio (6:1) BiPO4 at
different E1 wavelengths (567.4 nm, 584.4 nm, 588.4 nm, 596.4 nm, 612.4 nm) and E2 scanned from
567.4 nm to 607.4 nm at PMT1 and PMT2 at 300 K, respectively. (b,d) show SFWM cross- interaction
at different E2 wavelengths (567.4 nm, 587.4 nm, 588 nm, 588.4 nm, 602.4 nm) and E1 scanned from
567.4 nm to 612.4 nm at PMT1 and PMT2 in 300 K, respectively. (e,f) show SFWM cross-interaction
at 77 K. The other experimental conditions are the same as (a,c), respectively. Time gate = 500 μs.
(g1–g5) show the simulation result corresponding to (b1–b5). (h1–h5) show the simulation result
corresponding to Figures 3(g1–g5) and 7(e1–e5).

Figure 5b shows the constructive cross-interaction of SFWM (two sharp peaks

′′ = 0) , broad peak N1(θAS
R1(θ AS ′′ = 0) ) at the E2 resonance. Compared with the small dip at the
E2 resonance, Figure 4(c3), the small dip at the E2 resonance, Figure 5(b3), increases due to
′′ = 0) with the phonon1 dressing | G Tp 11 |2 /( Γ 10 + i Δ 2 + i Δ cp 1 ) in
the cross-interaction R1(θ AS
Equation (5). Such a small sharp dip results from the switch of the two cascade dressings
(3)
| G Tp 11 |2 /( Γ 10 + i Δ cp 1 ) + | G 2 |2 of ρ ′′AS 1 . The broad peak, as shown in Figure 5b, comes from the
constructive cross-interaction N1(θAS ′ = 0) due to less phonon dressing.
Figure 5c shows the cross-interaction of SFWM (sharp peak R 2 (θ A′′′S = 0 ) , broad dip
N 2 (θ A′′′S = 0 ) (profile)) at the E1 resonance. The sharp dip at the E1 off-resonance (Figure
5c) is transferred into the sharp peak at the E1 resonance, Figure 5(c3), due to the
constructive cross-interaction R 2 (θ A′′′S = 0 ) with the phonon1 dressing | G Tp 11 | 2 + | G 1 | 2
of ρ A′′ (S31) at the narrowband excitation. Such a transition (sharp dip R 2 (θ A′′′S = π ) to a
sharp peak R 2 (θ A′′′S = 0 ) ) results from the switch of the three cascade dressings (internal
photon G 2 , external photon G1 and phonon1 G p 1 of | G Tp 11 |2 /( Γ 1 0 + i Δ cp 1 ) + | G1 |2 + | G 2 |2 in
| ρ A( 3S) 1 + ρ A′′′S( 32) | 2 ). The broad dip comes from the strong constructive interaction
N 1 (θ A′′′S = π ) , as shown in Figure 5c, with more phonon dressing. More interestingly, the
sharp dips at the E1 off-resonance (Figure 5c) result from the self-interaction in Equation
(5). Such sharp dips are obtained from 300 K due to more thermal phonon dressing (large
G Tp 11 ). Compared with the sharpest peak at the E1 off-resonance for the (7:1) and (20:1)

samples (Figure 4c,d), the sharp dip at the E1 off-resonance (Figure 5c) decreases due to
the phase transition phonon dressing ( | G Tp 11 | 2 / i Δ cp 1 > | G Tp 12 | 2 / i Δ ap ,1b ) for (6:1) more H-
phase sample.
Figure 5d shows the destructive cross-interaction of SFWM (three sharp dips
R 1 (θ A′′′′ ′′′′
S = π ) , broad dip N 1 (θ A S = π ) ) at the E2 resonance. The differences with the three

sharp dips at the E2 off-resonance from the destructive self-interaction in Equation (5), as
shown in Figure 5d, and the three sharp dips at the E2 resonance, as shown in Figure 5(d3),
′′′′ = π ) with the phonon1 and phonon2
result from the destructive cross-interaction R1 (θ AS
dressing. The broad dip, as shown in Figure 5d, is obtained from the stronger destructive
Nanomaterials 2022, 12, 4304 12 of 16

′′′′ = π ) with more phonon dressing at 300K and the broadband

cross-interaction N1 (ϕ AS
excitation. Figure 5d corresponds to the simulation result (Figure 5h) from Equation (5).
The three sharp dips at the E2 off-resonance (Figure 5d) result from the three nested
dressings (internal photon G1 , two phonons). However, the decreasing three sharp dips
R 1 (θ A′′′′
S = π ) at the E2 resonance, Figure 5(d3), come from the external dressing | G2 |2 of
the four nested-cascade dressings (internal photon G1 , external photon G 2 and two
(3)
phonons) | G1 |2 / ( Γ 20 + |G Tp 11 |2 / ( Γ 10 -i Δ cp 1 + |G Tp12 |2 / ( Γ 13 -i Δ cp 1 - i Δ cp 2 )))+ |G 2 |2 of ρ′′′′
AS1 Equation (5) in
| ρ A( 3)S 2 + ρ ′′′′ (3) 2
. Such four dressing coupling results from the photon1–phonon2–
AS1 |

phonon1–phonon2 ( α 1† , α 2† , α †p1 , α †p 2 in χ ( 9 ) ) atomic coherence coupling.

More phonon dressing results from more lattice vibrations at 300K for Eu3+: BiPO4
than the other samples (Eu3+/Pr3+: YPO4 [24] and Pr3+: Y2SO5 [26]). The model for the
phonon-controlled transistor switch is presented, as shown in Figure 1d, where ‘enhancement
peak’ and ‘suppression dip’ correspond to ‘ON-state’ and ‘OFF-state’, respectively. When
the input signal (Figure 5b) is at a single ON-State (higher than baseline), then the
corresponding output signal (Figure 5d) is at a single OFF-State (lower than baseline). Such
a spectral switch can be controlled by single phonon dressing ( | G p 1 | 2 ). Our experimental
results defined the switching contrast as C= |Ioff –Ion|/ (Ioff +Ion), where Ioff is the intensity at
the OFF-state and Ion is the intensity at the ON-state. The maximum switching contrast C
for a single state switch is about 82%, as shown in Figure 3(b3,d3). Furthermore, when the
ON-state of the input signal is observed with two sharp peaks, Figure 5(b3), the
corresponding output signal has the OFF-state with three sharp dips, as observed in Figure
5(d3). Such a multi-states switch can be controlled by two phonon dressings ( | G p 1 | 2 ,
| G p 2 |2 ). The switching contrast C is about 93.6% for the multi-states switch measure for
Figure 5(b3) and Figure 5(d3).
Figure 5e,f show the constructive cross-interaction of SFWM (single sharpest peak
′ = 0) , broad peak N 2 (θ AS
R2 (θ AS ′ = 0) ) at the E1 resonance. Compared with the sharpest
peaks at the E1 off-resonance, as shown in Figure 5e, the sharpest peak R2 (θ AS ′ = 0) at the E1
resonance, as shown in Figure 5(e3), increases due to the constructive cross-interaction
with the phonon1-assisted dressing (| G1 |2 + | G Tp 12 |) 2 / ( Γ 10 + i Δ 1 + i Δ cp 1 ) of ρ ′AS(3)2 at 77 K. Figure
5g shows the simulation results corresponding to the experimental results (Figure 5b). The
′ = π ) (Figure 5c) to broad peak N 2 (θ AS
transition from the broad dip N 2 (θ AS ′ = 0) (Figure
5f) is due to the reduction of phonon dressing. Therefore, thermal phonon dressing plays
a key role in the cross-interaction.
In order to explore further, we further compare the FL and SFWM interaction in
Section 2.2.3.

2.2.3. Comparison of FL and SFWM Interaction

The cross-interaction, as shown in Figures 6 and 7, evolves from out-of-phase FL to
hybrid (coexistence of second order FL and SFWM), to in-phase SFWM by changing the
time gate (1 μs to 500 μs) obtained from the (0.5:1) sample.
Figure 6a,b show the constructive cross-interaction of FL (sharp peak R1 (θ F = 0) ,
broad peak N1 (θ F = 0) ) at the E2 resonance. Similar to Figure 3(a3,b3,e3,f3), the increasing
sharp peaks, Figure 6(a3), at the E2 resonance are due to the constructive cross-interaction
R1 (θ F = 0) in Equation (1). Compared with the sharp peak at the E2 off-resonance (Figure
6b), the sharp peak R1 (θ F = 0) at the E2 resonance, Figure 6(b3), decreases due to the
phonon1-assisted dressing (| G 2 |2 + | G Tp11 |) 2 / ( Γ 10 + i Δ 2 + i Δ ep1 ) of ρ F′ (3)
1 (similar to Figure 5a).
Figure 6c,d show the constructive cross-interaction of SFWM (two sharpest peaks
′ = 0) , broad peak N1(θAS
R1(θ AS ′ = 0) ) at the E2 resonance. When the time gate increases to 500
μs, compared with the two sharpest peaks at the E2 off-resonance, as shown in Figure 6c,d,
Nanomaterials 2022, 12, 4304 13 of 16

′ = 0) at the E2 resonance, as shown in Figure 6(c3,d3),

the two sharpest peaks R1(θ AS
decrease due to the phonon1-assisted dressing (| G 2 |2 + | G Tp12 |) 2 / ( Γ 10 + i Δ 2 + i Δ ep1 ) in ρ ′A(3)
S1

(similar to Figures 4(c3) and 5(a3)). The spectral linewidth of the sharp peak, as shown in
Figure 6(a1), at 300K is nine times larger than the linewidth at 77 K, as shown in Figure
6(c1), due to more thermal phonon dressing ( | G Tp11 |2 / i Δ ep1 > | G Tp12 |2 / i Δ ep1 ).
Similar to the sharp peak with the (6:1) sample at 300 K (large GTp11 ), as shown in
Figure 5(a,b), the two sharpest peaks with the (0.5:1) sample are also shown at 77 K (small
G Tp 12 ), as shown in Figure 6(c,d) due to the phase phonon dressing | G Tp 12 | 2 /( i Δ ep 1 + i Δ 1 )
from the resonance detuning ( Δ ep1 ≈ 0 ). Therefore, compared with out-of-phase FL (Figure
6a,b), in-phase SFWM is more sensitive to phonon dressing (Figure 6c,d).

(a3) (c5)
(a2)
Intensity

(a4)

Intensity
(a1) (a5)
(c1) (c3) (c4)

SFWM Signal
FL Signal

(c2)
565 590 615 Wavelength(nm)
(d3) (d4) (d5)
(b5)
(d1)
Intensity

Intensity
(b1) (b3)
(b4)
(b2)
(d2)
565 590 615 Wavelength(nm)

Figure 6. (a,b) show FL cross-interaction observed from the output signals of Eu3+ doped in molar
ratio (0.5:1) BiPO4 at different E2 wavelengths (567.4 nm, 587.4 nm, 588 nm, 588.4 nm, 602.4 nm) and
E1 scanned from 572.4 nm to 612.4 nm at 300 K, at PMT1 and PMT2, respectively. The time gate is
10 μs. (c,d) show SFWM cross-interaction at 77 K at the time gate = 800 μs, respectively. The other
experimental condition is the same as (a,b).

Figure 7a,b show the constructive cross-interaction of FL (sharp peak R2 (θ F = 0) ,

broad peak N2 (θF = 0) ) at the E1 resonance. When the time gate is fixed at 1 μs, compared
with the sharp peak at the E1 off-resonance, as shown in Figure 7a, the sharp peak
R2 (θ F = 0) at the E1 resonance, as shown in Figure 7(a3), increases (similar to Figure 6a).
The sharp peak R2 (θ F = 0) at the E1 resonance, as shown in Figure 7(b3), decreases
compared to the sharp peaks at the E1 off-resonance, as shown in Figure 7b, due to the
phonon1-assisted dressing (| G1 | + | G Tp 11 |) 2 / ( Γ 21 + i Δ 1 + i Δ ep 1 ) of ρ F′ ( 22 ) .
Figure 7c,d show the constructive cross-interaction of the hybrid (single sharpest
peak R2 , broad peak N 2 ) at the E1 resonance. When the time gate increases to 100 μs,
compared to the sharpest peak at the E1 off-resonance, as shown in Figure 7c,d, the
sharpest peaks R2 at the E1 resonance, as shown in Figure 7(c3, d3), decrease due to the
constructive cross-interaction with the phonon1-assisted dressing of R2 in Equation (3).
The broad peaks N 2 , as shown in Figure 7c,d, can be explained by the constructive cross-
interaction with less phonon dressing.
Figure 7e shows the destructive cross-interaction of SFWM (single sharpest dips
′′ = π ) , broad dip N 2 (θ AS
R2 (θ AS ′′ = π ) ) at the E1 resonance. When the time gate increases to
500 μs, compared to the difference with the sharpest dip at the E1 off-resonance, the
sharpest dip R2 (θ AS ′′ = π ) at the E1 resonance, as shown in Figure 7(e3), decreases due to
the stronger destructive cross-interaction with the phonon1 dressing. Such a decrease in
the sharpest dip R2 (θ AS ′′ = π ) results from the external dressing | G 1 | 2 of the two cascade
Nanomaterials 2022, 12, 4304 14 of 16

dressings | G Tp 11 |2 /( Γ 1 0 + i Δ dp 1 ) + | G 1 | 2 in ρ ′′AS(3)2 . Moreover, the broad dip ′′ = π )

N 2 (θ AS is
obtained from 300 K and the (0.5:1) sample with more phonon dressing.
Similar to Figure 5c, Figure 7f shows the cross-interaction of SFWM (single sharpest
peak R2 (θ AS ′′ = 0) , broad dip N 2 (θ AS ′′ = π ) at the E1 resonance. Compared to the sharp dip
at the E1 off-resonance, as shown in Figure 7f, the sharpest peak at the E1 resonance, as
shown in Figure 7(f3), comes from the constructive cross-interaction R2 (θ AS ′′ = 0) with less
phonon dressing. Such a transition (sharpest dip R2 (θ AS ′′ = π ) to the sharpest peak
R2 (θ AS ′′ = 0) ) results from the switch of the three cascade dressings
(3)
| G Tp 11 |2 /( Γ 10 + i Δ ep 1 ) + | G1 | 2 + | G 2 |2 of ρ ′′′
AS 2 . Similar to Figure 5c, the broad dip in Figure 7f, comes

′′ = π ) with more phonon dressing.

from the strong destructive cross-interaction N 2 (θ AS

(a3) (a4) (e5)

(a2) (c3) (c4)

SFWM Signal
(c2) (e2)

Intensity
Intensity

Intensity
(a1) (a5) (e4)
(c1)
(c5) (e1)
(e3)
Hybrid Signal
FL Signal

565 590 615 Wavelength(nm)

(b5) (d3)
(b1) (d4)

SFWM Signal
(f2)
(f5)
Intensity

Intensity

Intensity
(d5)
(b3)
(d2) (f1)
(b2) (f4)
(b4) (d1) (f3)
565 590 615 Wavelength(nm)

Figure 7. (a,b) show FL cross-interaction observed from Eu3+ doped in molar ratio (0.5:1) BiPO4 at
different E1 wavelengths (577.4 nm, 584.4 nm, 587.7 nm, 592.4 nm, 612.4 nm) and E2 scanned from
567.4 nm to 607.4 nm at PMT1 and PMT2, respectively, at the near time gate (1 μs). (c,d) show hybrid
cross-interaction at the middle time gates (100 μs). (e,f) show SFWM cross-interaction at the far time
gate (500 μs). The other experimental condition is the same as (a,b), respectively.

Therefore, the out-of-phase FL constructive interaction (Figure 7a,b) can be evolved

to the in-phase SFWM destructive interaction (Figure 7e,f). The H-phase result (Figures 5
and 6) comes from sensitive phonon dressing and easy distinction for in-phase SFWM.
Moreover, the linewidth of the peak increases from 0.4 ± 0.1nm , as shown in Figure
7c, to 4.7 ± 0.1nm , as shown in Figure 7a, due to the Γ phonon of the generating process. The
width of the dressing dip increases from 0.6 ± 0.1nm , as shown in Figure 5d, to
5.9 ± 0.2nm , as shown in Figure 3d, due to the Γ phonon of the dressing process. The
destructive cross-interaction R1 , as shown in Figures 3d and 5d, results from more phonon
dressing with the same area. However, such more phonon dressing shows different
phenomena for the single sharp FL dip, as shown in Figure 3d, and the three sharpest
SFWM dips, as shown in Figure 5d.

3. Discussion
From our results, we conclude that, unlike cross-interaction N i [non-resonance],
the internal and external dressing atomic coherence coupling results in switching between
constructive to destructive for Ri (Figures 3c, 4b, 5b,c, and 7f). The resonant cross-
interaction Ri is distinguished from the non-resonant cross-interaction N i without
internal dressing.
Furthermore, the destructive interactions result from cascade dressing (Figures 3d–f,
4c, 5b,c and 7e) and four nested-cascade dressing (Figure 5d), respectively. The cascade
dressing and nested dressing suggest strong and stronger photon–phonon atomic
Nanomaterials 2022, 12, 4304 15 of 16

coherence coupling (leading to the three dressing dips, as shown in Figure 5d),
respectively.

4. Conclusions
In summary, we theoretically and experimentally studied the constructive and
destructive photon–phonon atomic coherence interaction. The destructive spectral
interactions result from cascade dressing and four nested-cascade dressing, respectively.
Here, we controlled the spectral interactions through the temperature, laser
detuning/bandwidth, and molar ratio of the Eu3+ :BiPO4 crystal. Due to more phonon
dressing caused by high lattice vibrations, H-phase BiPO4 shows strong photon–phonon
atomic coherence interaction. The cascade dressing with strong photon–phonon atomic
coherence coupling led to the single sharp dip. Moreover, the four nested-cascade
dressing with stronger photon–phonon atomic coherence coupling led to three sharp dips.
Furthermore, the spectral evolution of the spectral cross-interaction from out-of-phase FL,
to hybrid, and to in-phase SFWM is controlled by the time gates. The experimental results
were verified through theoretical simulations. From our experimental results, the optical
transistor (amplifier and switch) was also realized from the photon–phonon atomic
coherence interaction where the signal amplification (peak or dip) is controlled by photon
dressing and the switch results by the photon–phonon interaction. By controlling the
phase transition, laser detuning, and temperature, a high amplifier gain of about 3.6 and
switching contrast (93.6%) is achieved from our proposed technique.

Author Contributions: Conceptualization, Y.Z.; methodology, H.F., P.L. and Y.Z.; software, H.F.;
validation, H.F., F.R. and Y.Z.; formal analysis, H.F., I.A. and Y.Z.; investigation, M.I. and F.N.;
experiment, H.F., M.I. and F.N.; resources, Y.Z.; data curation, H.F.; writing—original draft
preparation, H.F.; writing—review and editing, H.F. and F.R.; visualization, C.L.; supervision, C.L.
and P.L.; project administration, Y.Z.; funding acquisition, Y.Z. All authors have read and agreed to
the published version of the manuscript.
Funding: This work was supported by the National Key Research and Development Program of
China (2017YFA0303700, 2018YFA0307500), Key Scientific and Technological Innovation Team of
Shaanxi Province (2021TD-56), National Natural Science Foundation of China (61975159, 11904279,
12174302, 62022066, 12074306, 12074303).
Data Availability Statement: Data underlying the results presented in this paper are not publicly
available at this time but may be obtained from the authors upon reasonable request.
Conflicts of Interest: The authors declare no conflict of interest.

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