Ammonothermal Synthesis of Functional Ternary and Multinary

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Ammonothermal Synthesis of Functional Ternary and Multinary Dissertation zur Erlangung des Doktorgrades der Fakultät für Chemie und Pharmazie der Ludwig-Maximilians-Universität München Ammonothermal Synthesis of Functional Ternary and Multinary Nitrides Jonas Häusler aus Ingolstadt, Deutschland 2018 Erklärung Diese Dissertation wurde im Sinne von § 7 der Promotionsordnung vom 28. November 2011 von Herrn Prof. Dr. Wolfgang Schnick betreut. Eidesstattliche Versicherung Diese Dissertation wurde eigenständig und ohne unerlaubte Hilfe erarbeitet. München, den 24.04.2018 .................................... (Jonas Häusler) Dissertation eingereicht am 01.03.2018 1. Gutachter Prof. Dr. W. Schnick 2. Gutachter Prof. Dr. R. Niewa Mündliche Prüfung am 17.04.2018 Acknowledgements Acknowledgements Ich möchte mich herzlich bei Herrn Prof. Dr. Schnick für die Möglichkeit bedanken, meine Dissertation in seinem Arbeitskreis anfertigen zu können. Die hervorragenden Arbeitsbedingungen und die Freiheiten bei der Umsetzung neuer Ideen waren perfekte Voraussetzungen für die eigenständige Gestaltung meiner Promotion. Die Bearbeitung eines neuen Themenbereichs in der Arbeitsgruppe stellte außerdem eine besonders spannende und zugleich abwechslungsreiche Herausforderung dar. Ich möchte mich darüber hinaus für die zahlreichen positiven Anregungen und Gespräche bedanken und für die vielen Gelegenheiten, an Fachtagungen sowie an der ersten Summerschool für ammonothermale Kristallzucht in Erlangen und Santa Barbara teilnehmen zu können. Ganz besonderer Dank gilt zudem Herrn Prof. Dr. Rainer Niewa für Übernahme des Koreferats meiner Dissertation sowie für die tolle Zusammenarbeit in unserer Forschergruppe und die große Hilfsbereitschaft bei jeglichen Diskussionen und Fragestellungen. Herrn Prof. Dr. Wolfgang Beck, Herrn Prof. Dr. Hans-Christian Böttcher, Herrn Prof. Dr. Konstantin Karaghiosoff und Herrn Prof. Dr. Joost Wintterlin danke ich herzlich für ihre Bereitschaft, als Teil der Prüfungskommission meiner Doktorarbeit zur Verfügung zu stehen. Vielen Dank an meine Laborkollegen Peter Wagatha, Mathias Mallmann, Niklas Cordes, Philipp Strobel, Kerstin Gottschling, Claudia Lermer und an meine Schreibstubenkollegen Eva Bertschler und Otto Zeman für die tolle Zeit und vielen spaßigen Abende. Danke auch an Christian Maak, Lukas Neudert, Lucien Eisenburger, Robin Niklaus und Eugenia Elzer, an Fabian Kessler und Jonathan Sappl, an Philipp Pust, Sebastian Schmiechen und Nicole Braml und natürlich an alle anderen Mitglieder des Arbeitskreises für die schöne Zeit und die vielen lustigen Schafkopf-, Film-, und Pokerrunden. Ich möchte mich außerdem bei den Mitgliedern der Ammonothermal-Subgroup, Mathias Mallmann und Niklas Cordes, für die gute Zusammenarbeit in den letzten Jahren bedanken. Ebenfalls danke ich Philipp Pust und Sebastian Schmiechen für die Unterstützung und Hilfestellungen mit den Hochdruckautoklaven. Acknowledgements Darüber hinaus bedanke ich mich bei allen weiteren Beteiligten der DFG-Forschergruppe Ammono-FOR. Ohne die zahlreichen Kooperationen mit den Projektpartnern wäre diese Arbeit nicht möglich gewesen. Ich möchte mich dabei besonders bei Anna Kimmel, Thomas Steigerwald und Benjamin Hertweck für die große Hilfsbereitschaft bei Problemen jeglicher Art und die hervorragende Zusammenarbeit sowie bei Saskia Schimmel für die tolle Kooperation und die Röntgenmessungen bedanken. Herzlichen Dank auch an Prof. Rainer Niewa, Prof. Peter Wellmann und Prof. Eberhard Schlücker für die hervorragenden Anregungen und hilfreichen Gespräche bei unseren Forschergruppentreffen. Ich bedanke mich natürlich auch bei Lukas Neudert, Lucien Eisenburger, Robin Niklaus, Prof. Ján Minár und Prof. Oliver Oeckler für die tolle Zusammenarbeit, aus der einige schöne Publikationen hervorgingen. Vielen Dank auch an meine Praktikanten Stefan Strangmüller, Andreas Baumann, Gabriel Kiefl, Mathias Mallmann und David Schmidl, die alle einen hervorragenden Beitrag zu meiner Arbeit geleistet haben. Großer Dank gilt auch Wolfgang Wünschheim, Thomas Miller und Olga Lorenz für die Hilfe bei allen technischen und organisatorischen Fragen. Durch euch war es möglich, sich ganz auf die eigene Forschung zu konzentrieren. Außerdem bedanke ich mich bei Christian Minke für die unzähligen REM-Messungen. Darüber hinaus möchte ich mich herzlich bei den Organisatoren der Summerschool in Erlangen und Santa Barbara, Anna Kimmel, Siddha Pimputkar und allen weiteren Mithelfern, bedanken. Ich habe dort eine Menge toller Erfahrungen gesammelt und viele unglaublich nette Leute kennengelernt. Besonders die Gruppenausflüge waren wirklich einmalige Erlebnisse! Ebenso danke ich natürlich auch allen anderen Mitgliedern der Arbeitskreise Schnick, Oeckler, Hoch, Johrendt und Lotsch für die super Arbeitsatmosphäre und die tolle Zeit im 2. Stock. Meiner Freundin Martina und meinen Eltern und kann ich garnicht genug danken. Ohne eure Unterstützung wäre all das nie möglich gewesen! „ ― Table of Contents Table of Contents 1 Introduction ............................................................................................................... 1 2 Ammonothermal Synthesis of Nitrides: Recent Developments and Future Perspectives ............................................................................................................13 2.1 Introduction ........................................................................................................14 2.2 Ammonothermal synthesis of nitrides ................................................................16 2.2.1 Binary nitrides .............................................................................................16 2.2.1.1 Overview .................................................................................................16 2.2.1.2 Group 13 nitrides.....................................................................................17 2.2.2 Ternary nitrides ...........................................................................................22 2.2.3 Quaternary and multinary nitrides ...............................................................28 2.2.4 Oxonitrides .................................................................................................33 2.3 Advance of autoclave technologies ....................................................................35 2.3.1 Autoclaves and liner concepts ....................................................................35 2.3.2 In situ autoclave technologies .....................................................................38 2.3.2.1 In situ X-ray imaging ...............................................................................38 2.3.2.2 In situ spectroscopy ................................................................................39 2.3.2.3 In situ ultrasonic velocity measurements .................................................40 2.4 Future challenges and perspectives ..................................................................40 2.5 Conclusions .......................................................................................................42 2.6 References ........................................................................................................43 3 Ammonothermal Synthesis of Earth-abundant Nitride Semiconductors ZnSiN2 and ZnGeN2 and Dissolution Monitoring by In Situ X-ray Imaging ..................................53 3.1 Introduction ........................................................................................................54 3.2 Results and Discussion .....................................................................................55 3.2.1 Synthesis ....................................................................................................55 3.2.2 Powder X-ray diffraction (PXRD) ................................................................56 3.2.3 Scanning/transmission electron microscopy (SEM/TEM) ............................59 Table of Contents 3.2.4 UV/Vis spectroscopy .................................................................................. 60 3.2.5 Dissolution monitoring by in situ X-ray imaging .......................................... 62 3.3 Conclusions ...................................................................................................... 65 3.4 Experimental Section ........................................................................................ 66 3.4.1 Ammonothermal synthesis ......................................................................... 66 3.4.2 Powder X-ray diffraction ............................................................................. 67 3.4.3 Electron microscopy ................................................................................... 67 3.4.4 UV/VIS spectroscopy ................................................................................. 68 3.4.5 Dissolution monitoring by in situ X-ray imaging .......................................... 68 3.5 References ........................................................................................................ 69 4 Ammonothermal Synthesis and Optical Properties of Ternary Nitride Semiconductors Mg-IV-N2, Mn-IV-N2 and Li-IV2-N3 (IV = Si, Ge) ...................................................... 71 4.1 Introduction ....................................................................................................... 72 4.2 Results and Discussion ..................................................................................... 73 4.2.1 Synthesis ..................................................................................................
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