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Ultrafast photo-acoustic spectroscopy of super-cooled liquids

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dc.contributor.advisor Keith A. Nelson. en_US Klieber, Christoph en_US
dc.contributor.other Massachusetts Institute of Technology. Dept. of Chemistry. en_US 2010-08-31T14:49:46Z 2010-08-31T14:49:46Z 2010 en_US 2010 en_US
dc.description Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2010. en_US
dc.description Vita. Cataloged from PDF version of thesis. en_US
dc.description Includes bibliographical references (p. 219-231). en_US
dc.description.abstract Picosecond laser ultrasonic techniques for acoustic wave generation and detection were adapted to probe longitudinal and transverse acoustic waves in liquids at gigahertz frequencies. The experimental effort was designed for the study of supercooled liquids whose slower relaxation dynamics extend to gigahertz frequencies at high temperatures and whose faster dynamics are centered uniquely in the gigahertz frequency range. The experimental approach used a unique laser pulse shaping technique and, in the case of shear acoustic waves, a crystallographically canted metal transducer layer, to generate frequency tunable compressional and shear acoustic waves. Either time-domain coherent Brillouin scattering or interferometry was used to detect the waves in or after propagation through a liquid layer. The study of liquid-state gigahertz acoustic behavior required advances in both the experimental methodology and in the theoretical modeling of the results. A particular challenge was posed by the extraordinarily strong damping of gigahertz-frequency acoustic waves in liquids at some temperature ranges. This demanded the design and construction of a liquid sample cell allowing access to a wide range of liquid thicknesses, from less than a nanometer up to several microns. This was achieved by squeezing the liquid between two specially prepared high quality optical substrates held in a non-parallel configuration by a custom-designed sample holder jig. Several metallic layer materials were used for conversion of optical pulse energy into acoustic waves that were launched into the liquid samples, and different probe geometries were developed to enable access to a wide frequency range. The developed spectroscopic strategies were then applied to the study of two liquids, glycerol and tetramethyl tetraphenyl trisiloxane (DC704). Measurements of the density responses of both liquids from 400 K to below their respective glass transition temperatures were carried out. Longitudinal acoustic waves were either monitored via time-domain Brillouin scattering in the liquid or via interferometry after transmission through variably thick liquid layers, granting access to longitudinal acoustic frequencies from 10 GHz up to about 200 GHz. The information obtained on gigahertz frequency liquid relaxation was pieced together with data from several other techniques to create broadband relaxation spectra (from millihertz up to gigahertz), allowing characterization of the complex structural relaxation dynamics over many orders of magnitude and enabling both empirical modeling and testing of the predictions of the mode-coupling theory of supercooled liquids. The requirements for gigahertz shear wave generation and detection, including the properties of the photo-acoustic transducer materials, the sample and experimental geometry, and the detection material choices, are discussed. Results on shear wave propagation in glycerol and DC704 are presented. The technique for shear wave generation and detection is not limited to the study of viscous liquids but can also be applied to liquids like water, from which initial results are presented. en_US
dc.description.statementofresponsibility by Christoph Klieber. en_US
dc.format.extent 234, [1] p. en_US
dc.language.iso eng en_US
dc.publisher Massachusetts Institute of Technology en_US
dc.rights M.I.T. theses are protected by copyright. They may be viewed from this source for any purpose, but reproduction or distribution in any format is prohibited without written permission. See provided URL for inquiries about permission. en_US
dc.rights.uri en_US
dc.subject Chemistry. en_US
dc.title Ultrafast photo-acoustic spectroscopy of super-cooled liquids en_US
dc.type Thesis en_US Ph.D. en_US
dc.contributor.department Massachusetts Institute of Technology. Dept. of Chemistry. en_US
dc.identifier.oclc 655319384 en_US

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