4440 Vol. 45, No.
16 / 15 August 2020 / Optics Letters
Gas identification in high-Q microbubble
resonators
Zhong-Di Peng,1,4 Chang-Qiu Yu,2 Hong-Liang Ren,3 Chang-Ling Zou,1,4
Guang-Can Guo,1,4 AND Chun-Hua Dong1,4, *
1
CAS Key Laboratory of Quantum Information, University of Science and Technology of China, Hefei 230026, China
2
School of Electronics and Information, Hangzhou Dianzi University, Hangzhou 310018, China
3
College of Information Engineering, Zhejiang University of Technology, Hangzhou Zhejiang 310023, China
4
CAS Center For Excellence in Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026,
China
*Corresponding author: chunhua@ustc.edu.cn
Received 15 June 2020; revised 9 July 2020; accepted 9 July 2020; posted 10 July 2020 (Doc. ID 400381); published 6 August 2020
A new, to the best of our knowledge, experimental mecha-
nism is reported to realize the identification of gas by a
microcavity sensor. Instead of measuring the change in
the environment refractive index or absorption, the gas is
detected indirectly and indentified by using the thermo-
optics effect of a high-quality-factor microbubble resonator.
When passing gas through the microbubble, the pressure
induces a geometric deformation and thus an observable
frequency shift, and the thermal bistability response varies
due to the higher heat dissipation by gas molecules. With the
two output parameters, we can unambiguously distinguish
gas with different molecular weights, e.g., He, N2 , and CO2 .
Our demonstration opens a new avenue of microcavity sens-
ing by using indirect interaction between light and matter,
realizing a multiple-parameter sensing approach for gas or
solvent identification. © 2020 Optical Society of America
https://doi.org/10.1364/OL.400381
The whispering-gallery-mode (WGM) microcavity currently
attracts much interest, such as microbubbles, microspheres,
microrings, and microtoroids [1–4]. These microresonators
have been investigated widely for a variety of applications such
as optical sensing [2,5–9], nonlinearity optics [10–13], ultra-
low-threshold lasing [14,15], cavity optomechanics [16,17],
and cavity quantum electrodynamics (QED) [18–20]. Among
these applications, WGM microcavity-based sensors hold great
potential in high-precision sensing benefiting from their high
quality factor (Q) and small mode volume [1,6]. Research fields
in WGM sensors have seen enormous growth over the years,
and WGM microcavity-based sensors have also been employed
for temperature sensing [5,21,22], pressure sensing [23], force
sensing [24], and gas sensing [25,26]. Among different kinds
of microresonstor sensors, the microbubble resonator with a
thin shell has become distinguished because the empty channel
inside is a promising candidate for optofluidic sensing [27–30].
The microcavity sensing application relies mainly on the
direct interaction between the optical fields in the microcavity
and the parameter to be detected. For example, a force will
0146-9592/20/164440-04 Journal © 2020 Optical Society of America
Letter
change the geometry of a microcavity and thus shift the fre-
quency, and a nanoparticle adhering to the microcavity will
induce scattering losses and broaden the cavity linewidth.
Therefore, the sensing mechanisms [7] can be summarized
as reactive interactions, including resonant mode shift [31],
mode splitting [32], and dissipative interactions, including
resonant mode broadening [33,34] and dissipative sensing
[35]. However, the performance of a direct interaction sensing
mechanism in gas sensing is limited because the optical proper-
ties of a microcavity are hardly changed by the dilute gas in the
evanescent field of optical modes, and different gases have very
similar optical properties at the wavebands we are interested in,
so we cannot identify different gases with different densities.
In this work, we demonstrate a gas identification sensor
through indirect light–matter interaction, i.e., the mechanical
and thermal responses in high-Q microbubble resonators. As
we know, the resonance frequency will be red shifted when
increasing the flow rate because of the higher pressure in the
microbubble, while the thermal effect induced by the higher
input power [5,22,36,37] is decreased due to the thermal dis-
sipation by the passing gas. The different gas component has
different thermal conductivity [26]. Thus, the thermal response
can be compressed by the gas velocity and help to distinguish
different gases, i.e., He, N2 , and CO2 , in our experiment. Gas
qualitative identification and detection are applied widely in
environmental monitoring, medical auxiliary diagnosis, indus-
trial production, and public safety [38–41]. In addition, this
gas identification sensor can be independently distinguished
with the shifted frequency, which is avoided to monitor the gas
velocity. Our approach may potentially help future applications
of gas identification and quantitative detection, and provide a
way to reduce the thermal effect in a high-Q microcavity.
The thin-wall (down-scaled) microbubble resonator was
fabricated by locally heating an internally pressurized glass capil-
lary. First we tapered the capillary with an initial inner diameter
of 100 µm and initial outer diameter of 170 µm to a uniform
waist with an outer diameter of 47 µm [15]. Heated by two
cross-propagating CO2 laser beams, the tapered capillary’s wall
then became soft and expanded to form a bubble shape [29,42].
 Letter
Fig. 1. (a) Schematic of the experimental setup. FPC, EDFA, FRM,
and PD are fiber polarization controller, erbium-doped fiber amplifier,
flow rate meter, and photon detector, respectively. (b) Microbubble
cavity used in the experiment with diameter of 118 µm and wall
thickness of 3.9 µm. (c) Typical calculated distribution of the optical
modes at the cross section of the microbubble. (d) Typical transmission
in the microbubble with lower input power of 42 µw. The red line is
Lorenz fitting with linewidth of 25 MHz, corresponding to the loaded
Q factor of 7.7 × 106 and resonance wavelength of 1554.38 nm.
Finally, we obtained a microbubble resonator with a diameter of
118 µm and wall thickness of about 3.9 µm, which allows gas to
flow through two openings, as shown in Fig. 1(b).
The capillary was glued on a stage and controlled by a three-
dimensional micromanipulation to approach a tapered optical
fiber, which is launched a tunable continue-wave (CW) laser
around 1550 nm to excite the optical modes in the microres-
onator, as indicated in Fig. 1(a). The tapered fiber was touching
the microbubble resonator, in order to keep the coupling sys-
tem stable with a high flow gas rate. A function generator was
sent to the laser with a scanning range up to 16.4 GHz. The
polarization of the input light was controlled by a fiber polari-
zation controller (FPC). The output light was monitored with
a 150 MHz photon detector (PD), which was connected to a
digital oscilloscope. The whole system was placed in a clean
chamber to reduce contamination and perturbation from out-
side. Under low input light power, the loaded Q was measured
to be 7.7 × 106 , as shown in Fig. 1(d). This resonance mode
was also used in the following measurement. Calculated by the
dynamic evolution equation, the intrinsic Q (Q 0 ) was estimated
to be 1.96 × 107 . Figure 1(c) shows the radial and polar mode
profiles of the fundamental mode in the microbubble resonator,
which has evanescent fields inside and outside the shell.
When the laser was scanning through the cavity mode with
high power, the transmission was significantly different, as
shown in Fig. 2(a). This effect is called the thermal effect in
the microresonator, which is induced by the strong pump
laser heating the microcavity and shifting the cavity resonance
Vol. 45, No. 16 / 15 August 2020 / Optics Letters 4441
Fig. 2. (a) Typical transmission of optical mode with thermal effect,
when N2 passes through the microcapillary at different flow rates. The
input power is 2.7 mW with scanning speeds of 0.33 MHz/µs. The
solid lines show the experimental results, and the blue dotted lines
show simulation results with different K /C p . (b) Frequency shift
versus gas flow rate induced by three different kinds of gas. (c) Thermal
broadening versus flow gas velocity passing through the microbubble.
[5,22,36,37]. Then, the N2 gas flows through the microbubble,
and a different thermal response can be observed with a different
gas flow rate. Here, we connected one end of the microcapillary
to a source of pressurized gas via a pressure reducing vavle, which
can control the gas flow rate. The thermal response became
weak as the gas flowed through the microcapillary, while the gas
removed the heating from the microcavity. Consequently, as
the rate of gas flowing through the microcapillary increased, a
reduction in the linewidth of the mode with the thermal effect
was recorded. However, the damping of the intrinsic Q factor
can be ignored during the experiment, corresponding to the
stable dip in the transimisson. This is also demonstrated by
monitoring the transimission with low input power.
The dynamical thermal behavior and subsequently the con-
nection between this thermal response and gas flow rate are
discussed in this section. With sufficient power coupled to the
microcavity, the dynamic thermal behavior can be observed
with a broadening thermal linewidth [36,37] and hysteretic
optical resonance response. Considering the cavity medium
with a thermal expansion coefficient of ε and a thermal-optic
 4442 Vol. 45, No. 16 / 15 August 2020 / Optics Letters Letter

dn
coefficient of dT
, the cavity resonance frequency can be written shift makes it hard for us to distinguish these gases. However,
as [37] the relevant frequency broadening is shown in Fig. 2(c), which
    represents the extent of thermal response change with the flow
1 dn rate of various gases. The gases can be easily distinguished in our
ω0 (t) = ω0 1− ε+ 1T , (1)
n0 d T experiment from three kinds of gas through the dramatic change
in thermal broadening.
where ω0 is the cold cavity resonance frequency, and 1T is the With increasing the flow rate of gases, the linewidth of the
power-induced temperature change within the mode volume. mode decreases with different variation trends when passing
Here, the thermal-dynamic equation of intracavity tempera- CO2 , N2 , and He through the microcapillary while the reso-
ture change and field can be expressed as [15,36,37] nance frequency is red shifted. Figure 3(a) shows the thermal
d 1T broadening versus frequency shift by three different kinds of gas.
Cp = −K 1T(t) + αabs |E c (t)|2 , (2) In other word, this shifted frequency can be recorded during the
dt
experiment instead of the gas flow rate. It is very useful in prac-
s tical application. The decreasing trend of the thermal response
d E c (t) 2ke of different gases is in accordance with their increasing trend
= −[k0 + ke + i1ω(t)]E c (t) + i E in (t), (3)
dt τc of parameter K /C p. Figure 3(b) shows the fitted thermal con-
ductivity divided by thermal capacity (K /C p ) varing the flow
where C p and K are the heat capacity and thermal conduc- rate. It is easy to note that these results are inversely proportional
tivity between the cavity mode volumn and surroundings, to the thermal broadening. And from the theory of optical hot
respectively. αabs is the absorption coefficient of the intracavity wire anemometry, the heat dissipation, Hloss = (A + Bvl )δT
power for the increased temperature. E c (t) is the intracavity [45,46], is related to the gas flow rate of v, which is proportional
field amplitude of the pump power. The first term on the right to the shifted frequency δω. A and B are empirical constants,
side of Eq. (2) expresses the heat dissipation process, while the l is a fitting exponent (usually 0.5 for a simple hot wire), and
second term depicts the intracavity power absorption process. δT is the difference between cavity temperature at some flow
k0 = ω0 /2Q 0 and ke = ω0 /2Q e are the decrement of internal rate and the environmental temperature. We simply regard the
losses and the decrement of the coupler device, with Q 0 and parameter A + Bvl ∝ A 0 + B 0 |δω|l as a variable representing
Q e being the intrinsic and external Qs, respectively. τc is the thermal conductivity K to simulate the corresponding dynamic
cavity round-trip time. 1ω(t) is the detuning between the exci- thermal behavior as K ∝ A 0 + B 0 |δω|l . The fitting results
tation scanning frequency and the cavity resonance frequency agree well with the experimental results, as shown in Fig. 3(b).
ω0 . With the input–output relation of the waveguide coupled We believe that the fluctuations in the experiment come from
resonator, the transient
√ transmitted field can be obtained as the fluctuations in gas flow, especially with a low rate. The
T = |E in (t) + i 2ke τc E c (t)|2 . comparison results of the variation trend through simulation
As shown by blue dotted lines in Fig. 2(a), the normalized are in high coincidence with the relative size of K constants of
light transmission is obtained by numerical simulation with these three gases [47]. Similarly, we can use different variation
different K . Comparing the fitting and experiment results in
Fig. 2(a), our theoretical model is consistent with experiment
results. We set ε + n10 ddTn = 6 × 10−6 (1/◦ C), and from the
fitting, we obtain αabs /C p = 9.75 × 1011 (◦ C/J), with other
parameters k0 /2π = 4.93 MHz, ke /2π = 7.96 MHz from the
measurements. However, the obtained parameters K /C p are
changed as the flow rate, as indicated in Fig. 2. It is clear that
K /C p increase with the increasing flow rate, which means the
flowing gas increases the thermal dissipation.
Figure 2(b) shows the frequency shift varying the flow rate
induced by different gas, i.e., He, N2 , and CO2 . The shifted
frequency comes from the pressure-induced refractive index
change of gas and material, and the geometry change of the
microbubble [43,44]. The refractive index of low density gas is
given as n = 1 + α P P [43], where P and α P are the pressure
and the measured coefficient depending on the temperature,
respectively. Considering the gas in the evanescent field of the
inner shell, the analysis shows that the influence of the pressure-
induced refractive index on the optical mode shift is tens of
MHz/SCCM (SCCM, standard cubic centimeters per minute)
scale only. It is one order of magnitude lower than the influence
of the geometric effect, which is consistent with the results
in Ref. [44]. In addition, for these three gases, the α P has one Fig. 3. (a) Thermal broadening versus frequency shift of three
order of magnitude difference. In our results, there is no huge different kinds of gas. (b) Fitted thermal conductivity (K /C p ) versus
difference for the frequency shift, which also implies that the frequency shift. The dotted lines show the corresponding simulation
influence of the geometric effect on the optical mode shift is results, with (A 0 , B 0 ) of (216.9, 1343.3), (1254.8, 480), and (1215.9,
dominant. In other words, the slight difference in frequency 355.9) for He, N2 , and CO2 , respectively.
 Letter
trends between the linewidth of the mode with the thermal
effect and flow rate of gas to distinguish other kinds of gases. In
addition, we noticed that there is a crossing point for the curves
He and N2 in Fig. 3, which indicates that the relation between
the thermal shift and pressure by the flowing gas is not simply
proportional to the molecule weight. Although the mechanism
of the different responses distinguishable worth further studies,
the identification approach could be extended to other gas
molecules.
In conclusion, we have demonstrated gas identification by
an optical microcavity. The gas identification is a challenge for
conventional reactive or dissipative sensing mechanisms; thus,
we proposed a new approach based on the indirect mechanical
and thermal responses of the optical modes to the gas flow in a
microbubble. Also, multiple parameters can be extracted from
the two reponses, and thus the identification is allowed in a two-
dimensional parameter space. In our experiments, three kinds
of gases, i.e., He, N2 , and CO2 , can be distinguished through
observing the changing trend of linewidth of a mode due to
the thermo-optics effect. In this experiment, the measurement
of the gas flow rate is avoided, which is beneficial in practical
applications. When further extending the multiple parameter
sensing, for exmple, coating the inside of the microbubble res-
onator with a functionalized polymer [39], more gases would
be distinguished with this thermal response with different
flow rates, which is easily controlled in the microbubble tube
even without monitoring. Therefore, the indirect interaction
mechanism and multiple-parameter sensing has great potential
in future microcavity sensing applications, ranging from gas
recognition and gas-velocity sensing, to nanoparticle sizing.
Funding. National Key Research and Development (RD)
Program of China (2016YFA0301303); National Natural
Science Foundation of China (11722436, 11934012,
61741506, 61805061); Natural Science Foundation of
Zhejiang Province (LY20F050009); Open Fund of the State
Key Laboratory of Advanced Optical Communication Systems
and Networks, China (2020GZKF013); Anhui Initiative in
Quantum Information Technologies (AHY130200).
Acknowledgment. This work was partially carried out
at the USTC Center for Micro and Nanoscale Research and
Fabrication.
Disclosures. The authors declare no conflicts of interest.
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