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„Diamonds Are a Girl's Best Friend.“ Marilyn Monroe

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„Diamonds Are a Girl's Best Friend.“ Marilyn Monroe „Diamonds are a girl’s best friend.“ Marilyn Monroe Über die optischen Eigenschaften präsolarer Diamanten Dissertation zur Erlangung des akademischen Grades doctor rerum naturalium (Dr.rer.nat.) vorgelegt dem Rat der Physikalisch-Astronomischen Fakultät der Friedrich-Schiller-Universität Jena von Diplom-Mineralogin Anja Ulrike Braatz geboren am 30.06.1967 in Hannover Gutachter: 1. Prof. Thomas Henning 2. Prof. Elmar K. Jessberger 3. Dr. habil. Ulrich Ott Tag des Rigorosums: 29.8.2000, 31.8.2000, 21.9.2000 Tag der Verteidigung: 14.11.2000 ¢¡ £¥¤ ¦¨§ © £ ¡© ! #"%$'&( *),+"(- ./01 *&32 &4)5&7689 *)5& : 2.1. Murchison . 6 2.2. Allende . 6 ;/0<&=8>0? *@%AB@%"C) D 3.1. Optische Eigenschaften . 7 1 3.1.1. Infraroter Spektralbereich (6000 bis 50 cm E ) . 8 3.1.2. Ultravioletter und visueller Spektralbereich (200 bis 800 nm) . 9 3.2. Elektronenparamagnetische Resonanzabsorption . 10 3.3. Entstehung und Herstellung . 10 3.3.1. Diamantentstehung unter erhöhtem Druck . 11 3.3.2. Diamantentstehung unter niedrigem Druck . 14 :FGH8JI(K¨6L$'@=8M&01 *@%AB@"N)5&=" CO 4.1. Isotopenanomalien . 16 4.2. Chemische Zusammensetzung . 18 4.3. Struktur . 19 4.4. Größe . 19 RQTSN&UAV WK¨XNS(& YZK¨6L$'@N)[ W6L" \]&U8_^=8JI(K¨6L$'@=8M&="`0? *@%AB@%"C)5&U" .Ua P 5.1. Lösen des Hauptteils der Meteoritenmasse . 20 5.2. Entfernen des Schwefels . 22 5.2.1. 1. Methode . 23 5.2.2. 2. Methode . 23 5.3. Oxidation eines Teils der Kohlenstoffverbindungen . 23 5.4. Extraktion der Diamanten . 24 5.4.1. 1. Methode . 24 5.4.2. 2. Methode . 25 5.4.3. 3. Methode . 25 5.5. Entfernen von Graphit . 25 5.6. Entfernen von Oxiden . 26 5.7. Entfernen von Quarzglas . 26 i O/cbL)[ WX(d4Ke)56=fg-U&=S(@%$h)1\]&=8_^=8MI(Ke6i$'@=8M&="`0? *@%AB@%"C)5&=" .]D D/cb!^]&Udj),8M6UKdk6L^ *K[XNSN&lm"C)5&U8JK+(XNS%+%"N-U&U" nAo #"Npq8J@=8M6=)5&="b!^]&Udj),8M@%$sr]&=8M&( ZXNS .]t 7.1. Ziele der Untersuchung . 29 7.2. Meßgerät und Probenaufbereitung . 29 7.3. Spektrenbearbeitung . 31 7.3.1. Berechnung des Massenabsorptionskoeffizienten . 31 7.3.2. Verbinden von Spektren . 31 7.4. Infrarotspektren der verschiedenen Aufbereitungsstufen . 31 7.4.1. Spektren der unbehandelten Meteorite . 32 7.4.2. Spektren nach der Behandlung mit konzentrierter Salz- und Flußsäure 32 7.4.3. Spektren nach der Weiterbehandlung der Probe mit schwefelsaurer Natriumdichromatlösung . 36 7.4.4. Spektren der mit Ammoniak extrahierten Diamanten . 37 7.4.5. Spektren von gereinigten Diamanten . 38 7.5. Analyse der Diamantspektren . 40 1 7.5.1. Absorptionsbanden zwischen 4000 und 3000 cm E . 42 1 7.5.2. Absorptionsbanden zwischen 3000 und 2800 cm E . 43 1 E 7.5.3. Die Absorptionsbande bei u 1750 cm . 44 1 E 7.5.4. Die Absorptionsbande bei u 1620 cm . 44 1 7.5.5. Absorptionsbanden zwischen 1500 und 1300 cm E . 45 1 7.5.6. Absorptionsbanden zwischen 1300 und 1000 cm E . 45 1 7.5.7. Absorptionsbanden zwischen 850 und 700 cm E . 46 1 7.5.8. Absorptionsbanden zwischen 650 und 500 cm E . 47 1 u 7.5.9. Die Absorptionsbande bei 475 cm E . 47 1 E 7.5.10. Die Absorptionsbande bei u 120 cm . 48 7.5.11. Ergebnis . 48 7.6. Simulation der Stickstoffkonfiguration . 49 7.7. Schlußfolgerungen und Zusammenfassung . 52 v/cb!^]&Udj),8M6UKdk6L^ *K[XNSN&wlm"N)5&=8MKk+=XNS+%"(-U&="x nA +%$h),8M@CyU *6L$*&4)z)5&="{+%"=\wy= *K+(&=$s$*&="|b¢^]&]d} ),8M@%$sr]&U8J&( ZXNS : P 8.1. Ziele der Untersuchung . 54 8.2. Meßgerät und Probenaufbereitung . 54 8.3. UV/VIS-Spektren präsolarer Diamanten . 55 8.4. Schlußfolgerungen und Zusammenfassung . 57 t/g$'&Udj),8M6L"(&="%^N@=8M@%AB@N-i"N&4)[ WK¨XNS(&R~g&7K¨6L"(@%"NjK^]&Udj),8M6UKd6L^ *& v P 9.1. Ziele der Untersuchung . 58 9.2. Meßgerät und Probenaufbereitung . 59 9.3. EPR-Spektren präsolarer Diamanten . 60 9.4. Schlußfolgerungen und Zusammenfassung . 63 ii a/9&76irN@=XNSN),+"(-3\&=8_^=8MI(Ke6L$*@=8M&="0? *@%AB@%"C)5&U" nAXNS(&=Ac *K[XNS3+%"%r]&=S(@"=\&=$h)5&=" 2R&4} )5&6]8 ')5&=" O P 10.1. Ziele der Untersuchung . 65 10.2. Meßgerät und Probenaufbereitung . 65 10.3. Untersuchung eines unbehandelten Meteoriten . 65 ]]9&( WyC&=8JK+=XNSN& O]v 11.1. Im Hochtemperaturmassenspektrometer . 68 11.1.1. Ziele der Untersuchung . 68 11.1.2. Meßgerät und Probenaufbereitung . 68 11.1.3. Ergebnis der Analyse . 68 11.2. Im hochauflösenden Transmissionselektronenmikroskop . 69 11.2.1. Ziele der Untersuchung . 69 11.2.2. Meßgerät und Probenaufbereitung . 70 11.2.3. In-situ-Beobachtung der präsolaren Diamanten . 70 11.3. Im Edelgasmassenspektrometer . 71 11.4. Ergebnis . 73 C.i9g"C)5Ke)5&=S%+"(- ^=8MI(Ke6i$'@=8M&=8<0? *@%AB@%"C)5&U" D P 12.1. Folgerungen aus den HRTEM-Messungen . 76 12.2. Folgerungen aus den EPR-Messungen . 77 12.3. Folgerungen aus der Analyse der optischen Spektren . 79 12.4. Mögliche Entstehungsgebiete präsolarer Diamanten . 80 12.4.1. Supernovae . 80 12.4.2. AGB-Sterne . 81 12.4.3. Wolf-Rayet-Sterne . 82 12.4.4. Novae . 83 12.5. Zusammenfassung . 83 C;ib!^]&Udj),8M6UKdk6L^ *K[XNSN&U8F@=XNSNT&= *KgyC6L"01 *@%AB@"N)5&=">@%+%4&=8S(@%$sr>\&7KHbL6L"%"N&U"NK¨7Ke)5&=ABKxv P 13.1. Optische Eigenschaften präsolarer Diamanten . 85 13.1.1. Optische Eigenschaften des Diamantgitters . 85 13.1.2. Der Einfluß der Oberfläche . 89 13.2. Analyse der Spektren verschiedener astronomischer Objekte . 91 13.2.1. Diamanten in der Umgebung von massereichen Protosternen und Herbig- Ae/Be-Sternen? . 91 13.2.2. Diamanten in den Überresten von Supernovaexplosionen? . 93 13.2.3. Diamanten in den zirkumstellaren Staubhüllen von AGB-Sternen? . 94 13.2.4. Diamanten im interstellaren Medium? . 96 13.3. Zusammenfassung . 98 7:M+(Ke@%AAB&="Cp@(K¨Kk+%"N- +"=\>+(Kr$s WX(d t]t iii <2 #"(&=8M@$*6U- WK¨XNS(&+NK¨@%AcAB&="(K¨&4)5N+"(- \&=8_+"N)5&=8MKk+=XNSN)5&="2R&4)5&768 ')5& 7a. A.1. Murchison . 102 A.2. Allende . 103 _<8+%"(\/$'@(-U&="cy&=8MK[XNS] W&\]&U"N&=8<&=8M&XNS%"+%"N-]&=" 7a P B.1. Extraktion der Diamanten: Berechnung der Korngrößen im Bodensatz . 105 B.2. Berechnung der Säulendichten von CHx-Gruppen . 105 B.3. Abschätzung des Stickstoffgehalts in Diamanten anhand der stickstoffindu- zierten Absorptionsbanden . 106 B.4. Abschätzung des mittleren Abstandes der präsolaren Diamanten im Meteoriten 106 iv ¡¦ [§| ¡ Über die Existenz von Diamanten außerhalb unseres Sonnensystems wird schon seit längerer Zeit nachgedacht. So veröffentlichten zum Beispiel Saslaw und Gaustad im Jahr 1969 in der Zeitschrift Nature einen Brief, in dem sie die optischen Eigenschaften von irdischen Diaman- ten mit den beobachteten Extinktionseigenschaften des interstellaren Mediums verglichen und insbesondere im ultravioletten Spektralbereich des Lichts Übereinstimmungen feststellten. Es war zu diesem Zeitpunkt allerdings völlig unklar, woher die Diamanten im interstellaren Me- dium stammen könnten. Zwar wurden schon im 19. Jahrhundert Diamanten in den Meteoriten Novo Urei (Kunz 1888) und Magura (Weinshank 1889) entdeckt, es wurde jedoch angenom- men, daß diese Diamanten unter hohen Drucken und Temperaturen im Innern von Planetoiden entstanden waren, deren Bruchstücke als Meteorite auf die Erde fielen (Saslaw und Gaustad 1969). Daher waren die Ausführungen von Saslaw und Gaustad (1969) nur einer von meh- reren Versuchen, die beobachteten Absorptionseigenschaften des interstellaren Mediums zu erklären. Erst die Entdeckung von Lewis et al. im Jahr 1987, daß die bis dahin als Cδ bezeichnete kohlenstoffhaltige Mineralphase im säureunlöslichen Rest kohlenstoffreicher Meteorite (so- genannter kohliger Chondrite) aus nanometergroßen Diamanten besteht, gab zu neuen Über- legungen über die Existenz von Diamanten außerhalb unseres Sonnensystems Anlaß. Die von Lewis et al. (1987) beschriebenen Diamanten unterscheiden sich nicht nur durch ihre Grö- ße (mittlerer Durchmesser 1-3 nm) von den bis dahin in Meteoriten gefundenen Diamanten, sondern auch durch die Zusammensetzung ihrer Isotope. Die aus den kohligen Chondriten isolierten Diamantproben enthalten Edelgase, deren isotopische Zusammensetzung so stark von der des Sonnensystems abweicht, daß man sich ihr Zustandekommen nur dadurch er- klären kann, daß die Diamanten außerhalb des Sonnensystems gebildet wurden (Lewis et al. 1987). Messungen der isotopischen Zusammensetzung anderer Elemente in den Diamantpro- ben zeigen außerdem eine Stickstoffanomalie (die Proben sind sehr arm an 15N; Lewis et al. 1987) und eine Anreicherung der Diamantproben mit Deuterium (Carey et al. 1987; Virag et al. 1989). Aufgrund der geringen Größe der Diamanten war es bisher nicht möglich, einzel- ne Diamantkristalle chemisch zu analysieren. Massenspektroskopische Untersuchungen von Russell et al. (1996) zeigen jedoch, daß der Stickstoff mit großer Sicherheit ein chemischer Bestandteil der Diamanten ist. Lewis et al. 1987 bezeichneten die von ihnen gefundenen Diamanten als „interstellar“, weil sie nicht aus dem Sonnensystem stammen. Andere Autoren, zum Beispiel Alexander et al. (1990), verwenden die Bezeichnung „präsolar“, weil ihrer Ansicht nach die Diaman- ten schon vor der Bildung des Sonnensystems existierten. Da die Bezeichnung „interstellare Diamanten“ zu der Annahme führen könnte, daß die Diamanten im interstellaren Medium ge- 1 bildet wurden, jedoch die Herkunft der von Lewis et al. entdeckten Diamanten noch ungeklärt ist, werden in dieser Arbeit die aus kohligen Chondriten isolierten Diamanten als „präsolare Diamanten“ bezeichnet. Im Zeitraum zwischen den Überlegungen von Saslaw und Gaustad (1969) und der Ent- deckung der präsolaren Diamanten durch Lewis et al. (1987) wurde eine neue Methode zur Herstellung von Diamanten bei niedrigen Drücken entwickelt, die sogenannte CVD-Synthese (CVD = Chemical Vapor Deposition). Dadurch wurde eine Entstehung von Diamanten auch außerhalb von planetoiden Körpern vorstellbar. Eine Beschreibung der CVD-Synthese von Diamant befindet sich im Abschnitt 3.3 dieser Arbeit. Einen Überblick über die Entwicklung der CVD-Synthese von Diamanten bietet der Artikel von Angus und Hayman (1988).
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