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Meiji University

Title

Sonoluminescence and bubble dynamics in viscous

liquids

Author(s)

崔,博坤, 竹内,優太, 山田,恭旦

Citation

電機情報通信学会技術研究所報告, 112(186): 9-12

URL

http://hdl.handle.net/10291/20891

Rights

CopyrightⒸ電子情報通信学会2012 本技術研究報告に

掲載された論文の著作権は(社)電子情報通信学会に

帰属します。

Issue Date

2012-08

Text version

publisher

Type

Journal Article

DOI

(2)

一般社団法人 電子情報通信学会 THE INSTITUTE OF ELECTRONICS, I~'FORMATION AND COM!,几'NICA TI ON ENGINEERS 信学技報 IEICE Technical Report USZOlZ-35(2012-08)

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Pak-Kon Choi t • Yuuta Takeuchi • Takaaki Yamada

Department of Physics, Meiji University 1-1-1 Higashimita, Tama-ku, Kawasaki, 214-8571 Japan E-mail:

t

[email protected] Abstract Multibubble sonoluminescence pulses of Na and continuum emissions were measured from NaCl-ethylene glycol solution saturated with Xe at 28 kHz. The Na emission consisted of multiple-peak pulses and single pulses. The intrinsic pulse width estimated from single pulses was 0.37 ns, which differs from 10-165 ns obtained by previous work. High-speed shadowgraphs of bubble dynamics and high-speed movies (32,000 fps) of sonoluminescence were observed. The observations suggest that the multiple-peak pulse is due to the superposition of single peaks resulting from bubbles fragmented from a characteristic bubble which repeats the fragmentation and coalescence. Characteristic spatial distribution of sonoluminescence was observed in aqueous solution of glycerol using a horn-type transducer. The distribution of sonoluminescence exhibited a sphere and a wedge shape at low and high acoustic pressures, respectively. The results of acoustic emission were used to interpret the difference in bubble dynamics in water and viscous liquid. Keyword Sonoluminescence, Na emission, bubble dynamics, ethylene glycol, glycerol, viscous liquid 1.Introduction Intense ultrasound irradiated in liquid creates bubbles which grow up from gas nuclei dissolved in liquid. These acoustic bubbles expand and contract with synchronizing the cycle of acoustic pressure. Sonoluminescence [SL] is emitted at the timing of bubble collapse. Na atom emission can be observed from aqueous solutions of Na Cl [ 1], and the SL pulses measured are single-peak pulses. In NaCl ethylene-glycol solutions, on the other hand, the shape of Na emission pulses were multiple-peak as well as single-peak [2,3]. In this report, we point out that the multiple-peak pulses are associated with bubble dynamics peculiar to viscous liquids such as ethylene glycol [4]. We have also observed characteristic behavior of bubble dynamics using a horn-type transducer in aqueous solution of glycerol. Results of SL and acoustic emission spectra were presented.

2. Experiments

The sample cell used was a 300 mL cylindrical quartz flask with a valve. A bolt-clamped ceramic transducer with a resonance frequency of 28 kHz was bonded to the bottom of the flask. One molar NaCl solution in ethylene glycol was carefully degassed while stirring then saturated with Xe gas at a pressure of l atm. The applied acoustic power was determined by calorimetry to

be 5.6 W, corresponding to an acoustic pressure of 2.3 atm. The SL emission was optically filtered and detected using a cooled photomultiplier (Hamamatsu, H7422-01) with a rise time of 750 ps and a digital oscilloscope (Agilent, DS05052A) with a 500 MHz bandwidth and a sampling speed of 4 G/s. Single-shot waveforms of SL pulses were measured through self-triggering. Two optical filters were used: a band-pass filter transmitting light at a wavelength of 589 nm to detect Na emission, and a blue filter transmitting light at wavelengths in the range of 300-500 nm to detect continuum emission. An instrumental time-response curve was estimated using a femtosecond laser (Spectra Physics, Mai Tai). The time-response curve was well fitted by a Gaussian and the mean and standard deviation of the full width at half maximum (FWHM) were l.40 ns and 0.08 ns, respectively. The statistical analysis of each pulse-width measurement was carried out using a set of hundred items of data.

Shadowgraph movies of cavitating bubbles in the ethylene glycol solution were taken using a high-speed video camera (Shimadzu, HPV-2) with a maximum frame rate of 1,000,000 fps. We used a zoom lens with a maximum magnification factor of 15 and a working distance of 40 mm.

In another experiment we recorded SL movies of Na emission. Since the sensitivity of the high-speed camera was not sufficient for SL

(3)

movies, we incorporated an image intensifier unit (Hamamatsu, Cl 0880-03) having a microchannel plate and an image booster into the high-speed camera. This enabled us to obtain SL movies at a frame rate of as high as 32,000 fps.

3. Results and discussion 3.1 SL pulse widths of Na

Sonoluminescence from NaCl-ethylene glycol solution saturated with Xe was separated by two different filters, which yielded a Na-emission pulses and continuum-emission pulses. Figure I shows an oscilloscope tracing of Na emission, displayed over a time span of 500 ns, which reveals one multiple-peak pulse denoted as "M" and three single pulses denoted as "S". Five hundred Na emission pulses were acquired, 52% of which were multiple-peak pulses and the remainder were single pulses. 20

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100 200 Relative time (ns) Fig.I Sonoluminescence pulses from Na atoms observed in ethylene glycol solutions of NaCl. Arakeri and Giri [3] reported the pulse widths of Na emission in ethylene glycol solution at 32 kHz. They obtained only single pulses, the FWHM of which was 62 ns for Ar-saturated solution. When the average of the multiple-peak pulses observed in the present experiment was fitted with a Gaussian curve, the FWHM was in the range of 20-61 ns. These values appear to agree with the results of Arakeri and Giri; however, there is an essential difference between their results and the present results. The multiple-peak pulses suggest the superposition of single pulses with a small width. This discrepancy may be caused by the response time of the photomultiplier and oscilloscope The response time of the present system system.

was estimated to be 0.96 ns from measurements of a laser pulse with l 00 fs width, which is negligible compared with the instrumental width. The widths of pulses comprising the multiple-peak pulses were about 1.4 ns, and therefore these pulses may not have been resolved with the system used by Arakeri and Giri because of its slow response time. The time intervals between pulses in the multiple-peak pulse in Fig. l are about4 ns, which is much smaller than the intervals between single pulses, of l 00 ns or more. This suggests that the multiple-peak pulses are caused by the superposition of SL from different bubbles that have some correlation with each other, and also suggests that single pulses are generated from independent bubbles. Gaussian curves were well fitted to the single pulses observed, giving an FWHM of 1.4~ ns with a standard deviation of

O.O~ns for the Na emission. The estimated instrumental width was l.40ns. The intrinsic width with the standard error in the mean was then obtained to be 0.37土0.04nson the basis that the sum of the squares of the intrinsic width and instrumental width is equal to the square of the experimental width. Coonnssiidering that multiple-peak pulses were only obtained from Na emission in ethylene glycol solution but not in aqueous solution, we assume that the multiple-peak pulses are specific to viscous liquids such as ethylene glycol, the viscosity of which is twenty times greater than that of water. Movies sonoluminescence

We obtained shadowgraph movies of bubble dynamics in 1 M NaCl-ethylene glycol solution. The frame speed was 250,000 fps and nine frames can be captured in one cycle of bubble expansion and contraction. The salient feature of the bubble dynamics in the present solution is complex oscillation of a large bubble followed by the emission of tiny daughter bubbles. Four frames are extracted as shown in Figs. 2(a)-(d). A large bubble is formed after frequent coalescences of small bubbles and expands to a maximum diameter of about 160 μm, as indicated in Fig. 2(a). When this bubble contracts, the bubble exhibits nonspherical shape and fragments into three 3.2 of bubble shadowgraph and

or

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-more bubbles which are in contact with each other

as shown in Fig. 2(b). The fragmented bubbles

coalesce again in the expansion phase. The bright

point seen at the center of the expanded bubble is a

back light that passed through the bubble,

indicating that the expanded bubble is not a cluster

of small bubbles but single. We also obtained the

movie of large bubble which repeats fragmentation

into many bubbles and immediate coalescence.

Tiny bubbles seen in the region upper right of the

large bubble are emitted from the large bubble. Fig.2 Four frames in shadowgraph movies of bubble dynamics in1 M NaCl-ethylene glycol solution.A large bubble shows nonspherical oscillation and fragments into several small bubbles which coalesce in the expansion phase Then, we propose that the characteristic bubble in Fig.2 is responsible for the multiple-peak

SL pulse as shown in Fig. 1. The large bubble

splits into several daughter bubbles at collapse and

each daughter bubble produces Na emission. To

verify our proposition, SL images corresponding to

the bubble shadowgraph were observed.

Although the SL from the present solution is

intense, as can be easily seen in a dim room, it was

difficult to capture moving pictures with the

high-speed camera due to a lack of sensitivity. To

amplify the SL signals, we employed an image

intensifier unit incorporating a microchannel plate

and an amplifier in front of the high-speed camera.

Using this system we succeeded in capturing SL

movies at a speed of 32,000 fps, a value

comparable to the ultrasonic frequency of 28 kHz.

Fig.3 represents a frame of SL movie of Na

emission showing that luminous spot "A"

propagates in the direction denoted by the arrow.

Since an event of SL occurs once during the

ultrasonic period of 36 μs which is larger than an

exposure time of 31 μs, each luminous point in the

single frame corresponds to a flash of SL produced

by one bubble. Figure 3 shows that the spot A

seems to be a cluster of luminous points, indicating

the spot A being several emission sites.

The translation speed of large bubble such as

one shown in Fig. 2 was estimated from the frame

size and rate to be in the range 0.3 -1.0 m/s. The

speed of the spot A was estimated to be 0.6 m/s.

Both speeds are in good agreement. Thus, we may

confidently infer that the the spot A represents the

SL from the characteristic bubble shown in Fig. 2.

The spot A is probably the source of the multiple-peak pulse and independent luminous points are responsible for the single pulses in Fig. 1. Fig. 3 A frame of Na emission photographed at a speed of 32,000 fps. Each luminous point in a frame corresponds to a flash ofSL.

3..33 Sonoluminescence using a horn-type

transducer

Using a horn-type ultrasonic transducer with a

frequency of f0=24 kHz and a power of 400 W

(Hielsher, UP 400S), SL was observed from

aqueous solution of 69 % glycerol. Figure 4

shows the SL emitting blue-white continuum

spectrum in 69% glycerol (upper) and

argon-saturated water (lower). The left and

right-hand side pictures were obtained at ultrasonic

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Fig.4 Pictures of sonoluminescence around 24kHz -ultasonic horn tip at the powers of 16W (left) and 64 W (right) in aqueous solution of 69 % glycerol (upper) and argon-saturated water (lower). 0 0 0 2 4 6 v > S P ) a p n l ! l d E < -80

3f•/-4

f

Sfo/4

2f

Water

3

f

20 40 60 80 Frequency (kHz) 0 0 0 2 4 6 S 8 P ) a ' p n l !

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f•/2 Glycerol 69%

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which are equivalent to the power of 16 and 64 W,

respectively. At the amplitude of 20 % the SL

reveals~a round shape, whereas the SL reveals a

wedge shape at the amplitude of 40 %. The bubble

pictures shows a similar behavior as the SL. The

SL from water, on the other hand, showed only a

wedge shape at every amplitude.

High-speed shadowgraph at 32,000 fps of

cavitating bubbles was observed under the horn tip.

The observation result indicated that the number of

bubbles was small and bubbles showed spherical

oscillation in 69 % glycerol compared with that in

water. The bubble clusters were frequently seen

in water.

Acoustic emission was also measured with a

hydrophone (B & K, type8103). Figure 5 shows

measured spectra in water (upper) and 69 %

glycerol (lower) at the amplitude of 20 %. In

water several multiples of /0/2 and /0/4, besides

harmonics nfo and broadband noise were obtained.

In 69% glycerol multiples of /o/2, harmonics nf

and broadband noise were obtained. This suggests

complex bubble oscillations occur in water, which

accords with the high-speed observation.

In conclusion, bubble oscillation and dynamics

in viscous liquids are very different from those in

water. Further experimental and theoretical works

are expected to interpret the complex dynamics in

viscous liquids. References [I]P.-K. Choi, "Sonoluminescence of inorganic ions in aqueous solutions" in Theoretical and Experimental Sonochemistry Involving Inorganic Systems, eds. Pankaj and M. Ashokkumar (Springer, Dordrecht, 2010) pp.337-356. [2] A. Giri andV.H. Arakeri, "Measured pulse width of sonoluminescence flashes in the form of resonance radiation," Phys. Rev. E 58, R2713-R2716(1998) [3]V. H. Arakeri and A. Giri,''Optical pulse characteristics of sonoluminescence at low acoustic drive levels," Phys. Rev. E 63, 066303(200I). [4] P.-K. Choi, Y. Sawada, and Y. Takeuchi, "Multibubble sonoluminescence pulses from Na atoms in viscous liquid"J.Acoust. Soc. Am. 131 (5), EL 413-419,(2012). 0 20 40 60 80 100 Frequency (kHz) Fig. 5. Acoustic emission spectra observed in water (upper) and 69 % glycerol using a horn-type transducer at 24 kHz. -12

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