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Modelling the DGEBA-EDA Poly-Epoxy Reactivity Towards Copper Experimental and Numerical Approach Andreas Gavrielides

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Modelling the DGEBA-EDA Poly-Epoxy Reactivity Towards Copper Experimental and Numerical Approach Andreas Gavrielides Modelling the DGEBA-EDA poly-epoxy reactivity towards copper experimental and numerical approach Andreas Gavrielides To cite this version: Andreas Gavrielides. Modelling the DGEBA-EDA poly-epoxy reactivity towards copper experimental and numerical approach. Materials. Université Paul Sabatier - Toulouse III, 2017. English. NNT : 2017TOU30300. tel-01988563 HAL Id: tel-01988563 https://tel.archives-ouvertes.fr/tel-01988563 Submitted on 21 Jan 2019 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. 5)µ4& &OWVFEFMPCUFOUJPOEV %0$503"5%&-6/*7&34*5²%&506-064& %ÏMJWSÏQBS Université Toulouse 3 Paul Sabatier (UT3 Paul Sabatier) 1SÏTFOUÏFFUTPVUFOVFQBS Andreas GAVRIELIDES le mardi 28 novembre 2017 5JUSF Modélisation du poly-époxy DGEBA-EDA et de sa réactivité vis à vis du cuivre: approche expérimentale et numérique Modelling the DGEBA-EDA poly-epoxy and its reactivity towards copper: experimental and numerical approach ²DPMFEPDUPSBMF et discipline ou spécialité ED SDM : Sciences et génie des matériaux - CO034 6OJUÏEFSFDIFSDIF CIRIMAT UMR CNRS 5085 %JSFDUFVSUSJDF T EFʾÒTF Pr. Corinne LACAZE-DUFAURE Dr. Thomas DUGUET Jury: Dominique COSTA, Directrice de Recherche, Chimie ParisTech, Paris, Rapporteur Tzonka MINEVA, Directrice de Recherche, Institut Charles Gerhardt, Montpellier, Rapporteur Patrice RAYNAUD, Directeur de Recherche, LAPLACE, Toulouse, Examinateur Frederic MERCIER, Chargé de Recherche, Université Grenoble Alpes, Examinateur Corinne LACAZE-DUFAURE, Professeur, CIRIMAT, Toulouse, Directrice de thèse Thomas DUGUET, Chargé de Recherche, CIRIMAT, Toulouse, Co-directeur de thèse Yohann LEDRU, Ingénieur Docteur, MECANO-ID, Toulouse, Invité Acknowledgements I would like to start by expressing my sincere gratitude to my supervisors Professor Corinne Lacaze-Dufaure and Dr. Thomas Duguet who trusted me with these project and gave me the opportunity to work with them. They are both great scientific minds and excellent characters and truly passionate about anything they are involved and the advancement of science. They were always there for me and without our valuable discussions and their dedication to the success of this project, this thesis would not have been feasible. The knowledge they have instilled in me will stay forever and I am grateful for the supplies they have provided for the open road that lies ahead of me. They have not only provided the knowledge but also the skills necessary to achieve my dreams. I will cherish our moments and hope in the future that our roads will once again converge. I would like to thank Professor Paul S. Bagus for his enormous help with the Hartree-Fock ΔSCF calculations which are a part of this thesis and for providing us with some very interesting results on the calculation of XPS spectra. Professor Doros Theodorou and PhD student Mr. Orestis Ziogos had a big impact on this project as our discussions both in Athens (National Technical University of Athens) as well as following discussions after returning back to France helped us accelerate the calculations on the Molecular Dynamics front. To both Professor Theodorou and Professor Andreas Boudouvis, I would like to say a big thank you for directing me in the path of executing a PhD thus giving me three of my best years. I would also like to thank the members of the SURF team of which I was a proud member during my 3-year PhD course and would like to extend special thanks to Dr. Maëlenn Aufray for our very helpful discussions and Mr. Jérôme Esvan for his valuable help in the experimental XPS spectra acquisition as well as the mounting of the metal evaporator on the UHV chamber. I am also lucky to have met and discussed with Dr. Constantin Vahlas in numerous occasions. Through our discussions I managed to change my character in a way I am sure will help me for years to come. My PhD thesis could not have been executed if not for my two wonderful parents Kleanthis and Marina which were there for me from the beginning and continue to support me until this very day. I owe them everything and they have shaped me throughout the years. My two brothers Pavlos and Alexandros were also there when I needed them and I am sure they will grow to be excellent. To my grandparents Pavlos, Virginia, Andreas and Alexandra I need to express my gratitude which cannot be contained in words as they are pillars of my life and have been there in all of my moments even from a distance. They have sacrificed a lot for me and this PhD is dedicated to their memory. Finally I would like to thank all of my friends that were right beside me, from my childhood years, to the 5 wonderful years in Athens and the 3 amazing years in France. They have stood by me in every moment, both good and bad and without them there would be no point in anything. This PhD thesis is finally dedicated to everyone who is not afraid to pursue their dreams no matter how impossible they may seem. I want you to know that if you put your mind on anything you can do it and even if you fail, persist and you can only win. Things will come around even in unpredictable ways. As far as the financial support of this thesis is concerned I would like to thank the French Ministère de l’Enseignement supérieur et de la Recherche for providing the funds for the execution of this thesis. Table of Contents Introduction générale ............................................................................................................................ 1 Chapter 1: Objectives and methods ..................................................................................................... 5 1.1 Introduction ....................................................................................................................................... 5 1.2 Why poly-epoxy polymers and what is the benefit of their surface metallization? .......................... 5 1.3 Calculations on polymers: ................................................................................................................. 8 1.3.1 Quantum calculations ................................................................................................................. 9 1.3.1.1 The Schrödinger’s equation ................................................................................................. 9 1.3.1.2 The Born-Oppenheimer approximation ............................................................................ 10 1.3.1.3 The Hartree-Fock method.................................................................................................. 12 1.3.1.4 Density functional theory (DFT) calculations ................................................................... 13 1.3.2 Classical Calculations ............................................................................................................... 21 1.3.2.1 Molecular Mechanics (MM) basics ................................................................................... 21 1.3.2.1 The molecular Dynamics (MD) method ............................................................................ 26 1.4 Computational Facilities.................................................................................................................. 31 1.5 Conclusion ....................................................................................................................................... 32 Chapter 2: Experimental formation of model poly-epoxy surfaces and characterizations .......... 37 2.1 Introduction ..................................................................................................................................... 37 2.2 Pristine (non-metallized) poly-epoxy surface ................................................................................. 38 2.2.1 Synthesis protocol of a pristine low-roughness poly-epoxy surface ........................................ 38 2.2.2. Characterizations ..................................................................................................................... 39 2.2.2.1 Bulk Characterizations ...................................................................................................... 39 2.2.2.2 Surface Characterizations .................................................................................................. 47 2.3 Metallized poly-epoxy surface ........................................................................................................ 56 2.3.1 Protocol for metallizing a poly-epoxy surface in ambient temperature with Cu ...................... 56 2.3.2 AFM results .............................................................................................................................. 58 2.3.3 XPS results ............................................................................................................................... 59 2.4 Conclusion ....................................................................................................................................... 60 Chapter 3: HF and DFT computations for the simulation of XPS spectra .................................... 63 3.1 Introduction
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