Brillouin spectroscopy on thin films application to intermediate valence and epitaxial silicides
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1 Research Collection Doctoral Thesis Brillouin spectroscopy on thin films application to intermediate valence and epitaxial silicides Author(s): Mendik, Michael Publication Date: 1993 Permanent Link: Rights / License: In Copyright - Non-Commercial Use Permitted This page was generated automatically upon download from the ETH Zurich Research Collection. For more information please consult the Terms of use. ETH Library
2 Diss.ETH ex. & 2kMail Diss.ETH No BRILLOUIN SPECTROSCOPY ON THIN FILMS: APPLICATION TO INTERMEDIATE VALENCE AND EPITAXIAL SILICIDES A dissertation submitted to the SWISS FEDERAL INSTITUTE OF TECHNOLOGY ZURICH for the degree of Doctor of Natural Sciences presented by MICHAEL MENDIK Dipl.Phys.ETH born July 3th, 1963 citizen of Wadenswil (ZH) accepted on the recommendation of Prof.Dr.P.Wachter, examiner Prof.Dr.G.Giintherodt, co-examiner, / /$/&(M?fi~~
3 ABSTRACT The principal goal of this experimental work is the determination of the (cubic) elastic constants (Cn, C44, C12) of intermediate valent single crystals as well as epitaxial silicides by means of surface acoustic waves. Brillouin spectroscopy (inelastic light scattering) has been applied to detect thermally excited surface acoustic waves and spin waves. The main advantage of light scattering techniques is that small samples or thin films can be measured by a contactless way and under various experimental conditions, e.g. at low temperatures or in magnetic fields. In our work we investigated opaque materials, therefore excitations located in the approximate vicinity of the surface only, such as surface acoustic waves or surface spin waves, could be detected. The velocity of a surface acoustic wave propagating on basal planes of single crystals is depending on the direction of the wavevector in the plane. This directional dependence is called angular dispersion. On the other hand, using the experimentally determined angular dispersion of surface acoustic waves it is possible to compute the whole elastic tensor of the bulk single crystal. A computer program was written to calculate the velocity of a surface acoustic wave propagating along any arbitrary direction on an anisotropic thin film supported by a substrate. This enables to fit the elastic tensor of a single anisotropic thin film. This routine was developed in order to fit the elastic constants of epitaxial thin films that can not be grown with a larger thickness. In the first section we report simulations of surface acoustic waves on thin films that provide informations about the accuracy and reliability of the fit following chapters. applied in the Epitaxial silicides grown on Si: Surface acoustic modes as well as higher order plate modes (Sezawa) were found on epitaxial NiSi2 and CoSii (CaFr-structure) and used to fit the elastic tensor. The main result is, that the elastic properties of CoSi2 and NiSi2 are similar and lie in close agreement with the theoretically calculated properties.
4 For pseudomorphic FeSi, synthezised in the CsCl structure, the measured elastic constants are about 10% lower than theory predicts but still within the typical values for the CsCl structure. Surface spin waves (Damon Eshbach modes) and standing spin waves have been observed on epitaxial ferromagnetic Fe%Si films. The magnetic properties of thick epitaxial films are in agreement with the parameters of single crystals. On the other hand, the magnetization of thin films is depending on the quality of the interface. The motivation for Brillouin scattering measurements on YbX(X=N,PlAs), UTe and TmSeo.toTeQ.iQ single crystals was to find possible negative values for C12. A negative Cu and thus a negative Poisson's ratio are typical for intermediate valence behavior and indicate shrinking of the crystal under uniaxial pressure. For Y6X(X=N,P,As) we could clearly show that C12 remains positive and thus no valence fluctuations are expected. On the other hand, for UTe, which has a negative C12 at room temperature (shown by neutron scattering and ultrasound spectroscopy), we could demonstrate that the elastic properties do not change below the Curie point for ferromagnetic ordering (Tc=106 K) and a negative C12 is highly probable. This coexistence of ferromagnetic ordering and intermediate valent behavior is unusual. For TmSeo.wTeo.40 we found a negative C\i at room temperature which means that this semiconducting compound is intermediate valent in the absence of external pressure and is thus the first example of an intermediate valent semiconductor having a negative elastic constant at ambient conditions.
5 KURZFASSUNG Das Ziel dieser experimentellen Arbeit war, die elastischen Konstanten (Cn, C44, C12) von verschiedenen zwischenvalenten Verbindungen kubischer Einkristalle und epitaktischen Siliziden mit Hilfe Oberf&chenschallwellen zu bestimmen. Zu diesem Zwecke wurde die Technik der Brillouin-spektroskopie (inelastische Lichtstreuung) verwendet da gerade diese die beriihrungs und zerstorungsfreie Messung von kleinen Kristalliten oder Substanzen, die nur in Form diinner epitaktischer Schichten vorkommen, ermoglicht. In unserer Arbeit untersuchten wir vor allem stark absorbierende Materialien. Wegen der geringen Eindringtiefe des Lichtes (etwa 200A) im untersuchten Festkorper tragen hauptsachlich diejenigen akustischen Anregungen zum Streuquerschnitt bei, die an der Oberflache lokalisiert sind. Deshalb konnten nur akustische Oberf&chenwellen detektiert werden. Diese sind jedoch durch die elastischen Eigenschaften des bulk Materials und der Dichte bestimmt. Die Geschwindigkeit einer Oberflachenwelle, die auf einer kristallographischen Symmetrieebene propagiert, ist von der Propagationshc/iftm^ in der Ebene abhangig. Diese Richtungsabhangigkeit wird im folgenden Winkeldispersion genannt. Mit Hilfe der experimentell gemessenen Winkeldispersion von Oberf&chenvteUeii ist es nun moglich den vollstandigen elastischen Tensor des ganzen Fittprozedur zu bestimmen. Bti/fc-Materials mit einer Es wurde eine numerische Prozedur entwickelt die die Geschwindigkeit von akustischen Oberflachenwellen auf dunnen kubischen Filmen in jeder beliebiger Propagationsrichtung iterativ eindeutig berechnet. Diese wurde verwendet, um die elastischen Konstanten einzelner epitaktischer Schichten mit grosst moglicher Genauigkeit zu fitten. Im ersten Abschnitt berichten wir iiber zahlreiche numerische Simulationen an akustischen Oberflachenmoden auf Einkristallen und dunnen epitaktischen Schichten. Damit wird gezeigt, wie die Geschwindigkeit von den elastischen Konstanten im einzelnen abhangt und die Genauigkeit der Fittprozedur wird abgeschatzt.
6 Konstante) Auf Si epitaktisch gewachsene Schichten: Es wurden akustische Oberflachenmoden und hohere Plattenmoden (Sezawa) auf NiSi2 und CoSii (CaF2 Struktur) gefunden und fur die Fittprozedur verwertet. Das Hauptresultat ist, dass die gefundenen elastischen Konstanten fur CoSi2 und NiSi2 ahnlich sind und mit den, vor kurzem publizierten, theoretischen Voraussagen hervorragend iibereinstimmen. Die gefitteten elastischen Konstanten des pseudomorph gewachsenen FeSi (CsCl-Struktur) sind etwa 10% niedriger als die theoretischen Werte, liegen aber im Rahmen der fur CsCl typischen Werte. Auf den epitaktischen ferromagnetischen FesSi Filmen sind sowohl Oberflachen wie auch stehende Spinwellenmoden nachgewiesen worden. Damit konnten zum ersten Mai die magnetischen Parameter (M, g Faktor, exchange - epitaktischer FesSi Filme bestimmt werden. Die Werte fur dicke Schichten stimmen mit denjenigen fur Einkristalle iiberein, wogegen die Magnetisierung von diinnen Schichten stark von der Qualitat des interface Si-FeaSi abhangt. YbX(X=N, P, As), UTe und TmSeo.eoTe0.4o Einkristalle wurden hinsichtlich negativer Werte fur C12 untersucht. Ein negatives C12 (und daraus eine resultierende negative Poisson-Zaht) sind typische Merkmale fiir zwischenvalente Systeme und bedeuten eine Queikontraktion des ganzen Kristalls unter uniachsialem Druck. Es konnte gezeigt werden, dass die Werte fur C12 von YbX positiv sind und somit Ladungsfluktuationen ausgeschlossen sind. Ein klares negatives C12 konnte bereits fruher fur UTe bei Zimmertemperatur mittels Neutronenstreuung und genauer mit Ultraschallabsorptions Messungen nachgewiesen werden. Mit Brillouinstreuung unter dem Curie-Punkt fiir ferromagnetische Ordnung (Tc=106 K) konnte erstmals gezeigt werden, dass sich die elastischen Eigenschaften nicht andern und somit ein negatives C12 durchaus existieren kann. Diese Koexistenz von Ferromagnetismus und zwischenvalentem Verhalten ist ungewohnlich. Fiir Tm5eo.60^0.40 wurde ein negatives C12 bei Zimmertemperatur gefunden. TmSeo.60Teo.40 ist somit das erste Beispiel fiir einen Halbleiter der zwischenvalentes Verhalten zeigt ohne ausseren hydrostatischen Druck.
Brillouin-spectroscopy on
Diss ETH Nr. 12161 Brillouin-spectroscopy on thin films and intermediate valent rare earth compounds Abhandlung zur Erlangung des Titels Doktor der Naturwissenschaften der EidgenOssischen Technischen Hochschule
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