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SONOLUMINESCENCE in WATER MIXTURES and in LIQUID METALS a Thesis Submitted for the Degree of Doctor of Philosophy in the Univers

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SONOLUMINESCENCE in WATER MIXTURES and in LIQUID METALS a Thesis Submitted for the Degree of Doctor of Philosophy in the Univers SONOLUMINESCENCE IN WATER MIXTURES AND IN LIQUID METALS A Thesis submitted for the Degree of Doctor of Philosophy in the University of London by FREDERICK RONALD YOUNG, M.A. (CAMBRIDGE). ABSTRACT Sonoluminescence from viscous liquid-water mixtures has been measured using a magnetostrictive transducer with a titanium velocity transformer and a photomultiplier tube. The results suggest a correlation between sonoluminescence and viscosity. The same apparatus has been used to measure the sonoluminescence from water containing dissolved gases. An inverse relationship between the sonoluminescence and thermal conductivity of the gas supports the theory that the light is basically due to an adiabatic compression of the gas during the rapid collapse of the cavitation bubbles. Sonoluminescence from liquid metals has been measured using a lead zirconate titanate transducer with a glass velocity transformer and the same photomultiplier tube. Thermal diffusivity of the metal appears to have an inverse relationship with sonoluminescence again supporting the thermal origin of the light. 3 ACKNOWLEDGEMENTS The author wishes to thank Dr. R.W.B.Stephens for his constant guidance and encouragement, Mr. E.A.Neppiras for his advice, and his colleagues in the Acoustics Group for much help and many stimulating discussions. He wishes to thank Mr. T. Shand and Mr. E. Abbott of the workshop of the Physics Department for constructing the mechanical parts of the apparatus, Mr. O.R.Milibank for making the glassware, and Mr. F.Martin for guiding the author's attempts at making the simpler parts of the apparatus. He is grateful to Mr.P.Coppock, Mr. M.Wallace and Mr.M.O.Jackson for the photographic work, and Miss B. Lloyd-Jones and Mr.J.T.Graham for library assistance. He would like to express his appreciation to Mrs.J.D.Harris and Miss E.C.Pope for their patience and good humour in helping the author to produce this thesis. The author is deeply grateful to the Hertfordshire County Council for leave of absence and for financing the research, and to Dr.D.O.Bishop, Dr.J.F.Richardson, Dr.H.Tropper, Mr.GX.Warren and Mr.B.Wood of the Watford College of Technology for their help, advice and encouragement. Finally, he wishes to thank his wife for welcoming his intention to do this research and for constantly supporting him in the vicissitudes which have accompanied the production of this thesis. And the four winds, that had long blown as one, Shone in my ears the light of sound, Called in my eyes the sound of light. Dylan Thomas. 5 CONTENTS ABSTRACT 2 ACKNOWLEDGEMENTS 3 CONTENTS 5 SYMBOLS AND UNITS 7 CHAPTER 1 SURVEY OF SONOLUMINESCENCE 1.1. Definitions and Historical Review 10 1.2. Instrumentation for Observing Sonoluminescence 10 1.3. Model Bubble Experiment on Sonoluminescence 11 1.4. Luminescence from Hydrodynamic Cavitation 14 References in Chapter 1 17 CHAPTER 2 SONOLUMINESCENCE FROM VISCOUS LIQUID-WATER MIXTURES 2.1. Introduction 20 2.2. Design of Experimental Arrangement 20 2.3. Calibration Measurements 23 2.3.1. Acoustic Power Output 23 2.3.2. Sound Pressure Amplitude 26 2.3.3. Sensitivity of Photomultiplier Tube 29 2.4. Experiments 33 2.5. Results 33 References in Chapter 2 34- CHAPTER 3 SONOLUMINESCENCE FROM WATER CONTAINING DISSOLVED GASES 3.1. Introduction 37 3.2. Design of Experimental Arrangement 37 3.3. Calibration Measurements- 40 3.4.. Experiments 40 3.5. Results 43 References in Chapter 3 50 6 CILIITER 4. SONOLUMINESCENCE PROM LIQUID METALS 4.1. Introduction 51 4.2. Design of Experimental Arrangement 51 4.3. Calibration Measurements 61 4.3.1. Acoustic Power Output 61 4.3.2. Sound Pressure Amplitude 63 4.3.3. Sensitivity of Photomultiplier Tube 64 4.3.4. Thermocouple 64 4.4. Summary of Liquid Metal Experiments 64 4.5. Results 64. 4.5.1. Correlation of ¶ater and Mercury Experiments 64. 4.5.2. Mercury 65 4.5.3. Gallium 85 4.5.4. Indium 89 4.5.5. Tin 95 4..5.6. Bismuth 98 4.5.7. Collected Results 103 4.5.8. Bismuth in a Magnetic 'Field 103 4..6. Discussion of Results 105 4.6.1. Correlation of Sonoluminescence 105 with other Parameters 4.6.2. Cavitation Threshold Results 114 4.6.3. Mercury Results 114 References in Chapter 4 115 Suggestions for further work 116 Publications 117 7 SYMBOLS AND UNITS SI units are used, except where conventional units are much more familiar. Symbol Units Quantity (if used) Attenuation coefficient in Y=Yoe-" a nepers m 1 Density p kg m-3 Energy J Frequency f Hz Magnetic flux density wb m-2 Power W Radiation impedance Z kg s m-2 Resistivity Pi Om Sound displacement amplitude Y m Sound pressure amplitude P Ni 2 Sound velocity c ins" Sound velocity amplitude U ins" Specific heat at constant •.4 _ C, J gm degC degC -. 1 Surface tension a dyn cm Temperature Oc Temperature difference degC -1 -I -4 Thermal conductivity K J cm s degC Thermal diffusivity D OM23 - Ultrasonic attenuation a42 m 1s 2 Vapour pressure atmosphere Viscosity dynamic 77 gm cm-is-1 =Poiser-100cP 2 -1 Viscosity kinematic v cm S =Stoke=100cS Wave number k= an-A m 1 Wavelength X A Fig.J Sonoluminescence photographed using an image intensifier camera. 10 Chapter 1 Survey of Sonoluminescence 1.1. Definitions and Historical Review When a liquid is cavitated by a sound field of a few watts per square centimetre intensity a weak luminescence is emitted. This is called sonoluminescence. Cavitation is the process whereby a gas or vapour filled bubble expands and collapses as the net local pressure in the liquid becomes negative and then increases to above atmospheric. Sonoluminescence in tap water can be seen as a faint bluish glow by a dark-adapted eye, but it is stronger in glycerine. However it is more easily detected by a photomultiplier tube on account of its very low intensity. Sonoluminescence was first observed in 1933 by Marinesco and Trillat (1) when photographic plates were blackened on exposure for some hours to water cavitated by an oscillating quartz crystal. However, they ascribed this blackening to an.acceleration of the chemical process of oxy-reduction brought about by the ultrasonic waves. Frenzel and Schultes (2) made similar experiments and believed that the effect was actually due to exposure to light. Adequate reviews of the literature on sonoluminescence have been given by Jarman (3), El'piner (4.) and Finch (5). 1.2. Instrumentation for Observing Sonoluminescence Much of the earlier work was carried out by observing the sonoluminescence with the eye, but all later work has used photo- multiplier tubes. This has enabled a quantitative absolute measure of the light to be made and has led to the discovery that sonolumin- escence occurs as discrete flashes which are periodic with the sound field but that a sonoluminescence pulse does not occur with every sound cycle. (6). Finch (5) has given a table of the types of photo- multiplier tube and of transducer used in studying cavitation by various workers. Quartz crystals working at frequencies up to 2MHz were initially used to produce the cavitation, but more recently magneto - strictive and piezoelectric ceramic transducers working at frequencies from 1 - 30 KHz have been employed. Flynn (7) photographed the light emitted from a field of cavitation in front of a small 25 KHz ferrite transducer using a Westinghouse Astracon light image intensifier camera. (Fig.1). The exposure was for sec, and the decay time of the output phosphor was of the order of a milli-second. This may be a good way of measuring cavitation activity 11 as the phenomenon maybe measured directly without disturbing the cavitation field. Flynn is making a study to determine the relation between the number and density of bright images and the number and acoustic intensity of cavitation events respectively (8). 1.3. Model Bubble Experiment on Sonoluminescence Beccaria (1716 - 1781) observed that glass spheres containing air at reduced pressure emitted luminescence when broken in air. Priestley (9) gave the following description of Beccaria's experi- ments in 1769: "Signor Beccaria observed that hollow glass vessels, of a certain thickness, exhausted of air, gave a light when they were broken in the dark. By a beautiful train of experiments, he found, at length, that the luminous appearance was not occasioned by the breaking of the glass, but by the dashing of the external air against the inside, when it was broke." A model bubble experiment on sonoluminescence at GBttingen (10) was designed to study the collapse of a glass sphere of gas under controllable' conditions of purity, of initial gas pressure, of known gas content, and size of sphere. Schmid used a thin-walled glass sphere of 7 cm diameter which was evacuated, filled with various too gases at low pressures, and then CC1 4 immersed in a liquid. On breaking ill r H20 the glass wall by a striking plate, 1.Luft 1 10 the sphere imploded and a flash of ‘ light was emitted. A high speed I cinematograph record of the im- plosion, which lasted for 4. ms, showed that the walls accelerated t s until the volume of gas was effect- s CO2 ng He lu ively divided into a number of parts h tra each giving rise to strong shock S waves in the liquid and a flash of 01 light near the end of each implosion. Using glycerine as the liquid, a number of experiments were made with (C2H5)20 various filling gases at different CH,, 0 '01 o pressures and the results are shown 10 • 20 30 Torr 60 in Fig.
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