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Synchrotron Radiation Spectroscopy of Molecular Dynamics Beyond the Valence Shell

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Synchrotron Radiation Spectroscopy of Molecular Dynamics Beyond the Valence Shell Synchrotron radiation spectroscopy of molecular dynamics beyond the valence shell EMILIO MELERO GARCÍA Doctoral Thesis Stockholm, Sweden 2006 TRITA-FYS 2006:13 AlbaNova University Center, KTH Physics Department ISSN 0280-316X Section of Atomic and Molecular Physics ISRN KTH/FYS/- -06:13- -SE SE-106 91 Stockholm ISBN 91-7178-294-X SWEDEN Akademisk avhandling som med tillstånd av Kungl Tekniska högskolan framlägges till offentlig granskning för avläggande av doktorsexamen i fysik torsdagen den 20 April 2006 klockan 10.00 i AlbaNova University Center, SE-106 91 Stockholm. © Emilio Melero García, April 2006 Tryck: Universitetsservice US AB iii Abstract This thesis presents experimental results on molecular spectroscopy of gas phase mole- cules using synchrotron radiation. It deals mainly with dynamical processes following res- onant excitation of electrons from core and inner-valence shells of the following systems H2O, H2,SF6 and CD4. In order to reach these deep electrons and excite them photons in the energy range from 25 to 550 eV were used, depending on the particular system. Two experimental techniques are used. Photon induced fluorescence spectroscopy is used to study the fluorescence emission of fragments after the decay of resonant core- excited states for the water molecule, and after doubly excited states and resonant ex- citations of inner-shell electrons for H2 and SF6 respectively. Only the emission in the visible and near infrared range (300-900nm) and the Lyman-α transitions are measured. Energy resolved electron-ion coincidence is used for the study of the fragmentation of CD4 and SF6 after selective ionisation of one of the outer-valence orbitals. In the case of CD4 the fragmentation is compared for the cases in which the ionisation is done directly, or through participator Auger decay of different resonantly core-excited states. List of papers This thesis is composed of 7 peer-reviewed papers published in international jour- nals. Here I list the references of Papers I-VII • PAPER I Fluorescence Emission of Excited Hydrogen Atoms after Core Excitation of Water Vapor, E. Melero García, A. Kivimäki, L. G. M. Pettersson, J. Álvarez Ruiz, M. Coreno, M. de Simone, R. Richter, and K. C. Prince. Phys. Rev. Letters 96, (2006) 063003. • PAPER II Fluorescence emission following core excitations in the water molecule,A. Kivimäki, M. Coreno, R. Richter, J. Álvarez Ruiz, E. Melero García, M. de Simone, V. Feyer, G. Vall-llosera and K. C. Prince. J. Phys. B: At. Mol. Opt. Phys. 39, (2006) 1101. • PAPER III Fluorescence study of doubly excited states of molecular hydrogen, E. Melero García, J. Álvarez Ruiz, S. Menmuir, E. Rachlew, P. Erman, A. Kivimäki, M. Glass-Maujean, R. Richter and M. Coreno. J. Phys. B: At. Mol. Opt. Phys. 39, (2006) 205. • PAPER IV Synchrotron radiation induced fluorescence spectroscopy of SF6, J. Álvarez Ruiz, E. Melero García, A. Kivimäki, M. Coreno, P. Erman, E. Rachlew and R. Richter. J. Phys. B: At. Mol. Opt. Phys. 38 (2005) 387. v vi LIST OF PAPERS • PAPER V Core-excitation-induced dissociation in CD4 after participator Auger decay, J. Rius i Riu, E. Melero García, J. Álvarez Ruiz, P. Erman, P. Hatherly, E. Rachlew, and M. Stankiewicz. Phys. Rev. A 68, (2003) 022715. • PAPER VI An energy resolved electron-ion coincidence study near the S 2p thresholds of the SF6 molecule, A. Kivimäki, J. Álvarez Ruiz, P. Erman, P. Hatherly, E. Melero García, E. Rachlew, J. Rius i Riu and M. Stankiewicz. J. Phys. B: At.Mol.Opt.Phys.36 (2003) 781. • PAPER VII Experimental station for gas phase fluorescence spectroscopy, M. Stankiewicz, E. Melero García, J. Álvarez Ruiz, P. Erman, P. Hatherly, A. Kivimäki, E. Rachlew and J. Rius i Riu. Rev. Sci. Inst. 75, (2004) 2402. Except for Paper V I have always been involved in the measurements of all experiments during the experimental session. My additional contributions to the different Papers were as follows: In Paper I I analysed all the data and was in charge of writing the manuscript in discussion with the rest of coauthors. In Paper II I did a bit of the preliminar data analysis. In Paper III I did part of the data analysis and I was in charge of writing the manuscript in discussion with the rest of coauthors. In Paper IV I did part of the data analysis and discussed and co-wrote the man- uscript together with the first author. In Paper V I discussed and co-wrote the manuscript together with the first author. In Paper VII I co-designed the new optic cell and co-wrote the manuscript always together with the first author. Also analysed the preliminary data shown in the text. vii During my PhD studies I have also contributed to the following papers which are not included as part of the thesis - Neutral dissociation of superexcited states in nitric oxide, E. Melero Gar- cía, J. Álvarez Ruiz, P. Erman, A. Kivimäki, E. Rachlew, J. Rius i Riu, M. Stankiewicz and L. Veseth, Chem. Phys. 293,(2003) 65. + - Autoionization of superexcited states in N2 to the N2 B state, J. Álvarez Ruiz, M. Coreno, P. Erman, A. Kivimäki, E. Melero García, K. C. Prince, M. de Simone, E. Rachlew, R. Richter, J. Rius i Riu and L. Veseth, Chem. Phys. Letters 372, (2003) 139. σ1Σ+ π1Π 1Σ+ - Selective excitation of the np u and np u to the E, F g emission systems in molecular hydrogen using synchrotron radiation, J. Álvarez Ruiz, P. Erman, A. Kivimäki, E. Melero García, E. Rachlew, J. Rius i Riu and M. Stankiewicz, Chem. Phys. Letters 388, (2004) 31. - The npσ, π to EF emission systems in D2, studied by selective excitation,G. Vall-llosera, J. Álvarez Ruiz, P. Erman, E. Melero García, E. Rachlew, S. Menmuir and M. Stankiewicz, J. Phys. B: At. Mol. Opt. Phys. 38, (2005) 659. - Relaxation dynamics of SF6 studied by energy resolved electron-ion coinci- dence technique, M. Stankiewicz, J. Rius i Riu, J. Álvarez Ruiz, P. Erman, P. Hatherly, A. Kivimäki, E. Melero García and E. Rachlew, J. Electron Spec- trosc. Relat. Phenom. 137-140, (2004) 369. Acknowledgements Once again I face the empty paper with the will of expressing the due thanks and acknowledgements that the people responsible for this thesis deserve. And once again the paper looks back at me and challenges me to try to pour my heart into words, and to do it in much less than the million of pages I would certainly need to fairly give credit to everyone for this thesis and all these years. And I realise again that it is a futile effort, but a necessary one. I will probably not mention many of the great people I have known during these wonderful years. It is true that, although proud as I am of the work I am presenting here, and as self-conscious as I am of the enormous experience and knowledge that I have gathered about science, it is in my personal me that I carry my greatest reward and profit of these years. Therefore I have many to thank to. Those of you that can not find your names explicitly written here please believe me when I say that I carry you all with me. Starting thus with the beginning I would like to first thank the people that made possible in first instance that I came here. Specially I would like to thank my supervisor, Professor Elisabeth Rachlew, for giving me the opportunity of coming here and for teaching me so much without you maybe realising it sometimes. Also thanks to Peter Erman and to Agneta Falk for helping me whenever I needed it. It is a must to thank the people at my group Mattias (Jag ska aldrig glömde vår diskussioner; nästa gång fästa vi världen ok?), Sheena and specially Gemma (La única con la que he conseguido no engordar durante un beamtime!! mucha suerte maca!). Thank you so much for the friendship and companionship I have received from you. I wish you all the good luck for your future endeavours. Also to past members of the group, Bob and Ofelia, thank you very much. Outside the building where I work I have met with all sort of great people I would like to take the opportunity and say thank you to some of them: Bea, Mónica, Pello, Bea la pelirroja, Mercedes, Txemari, the Sons and Daughters of Erik, the staff of the OLEOLE restaurant (best tapas bar in Stockholm, Hantverkargatan 23), Edo and Elma (For being such a fantastic people), Fredrik and Pilar (thanks for that weekend in the wild!!) and many more... Thank you all so much!! Also from Spain Jose de la Vega deserves special mention for still being there despite the distance. Warm regards also to Sandra, Cuco, Maribel, Juani, Nati, Nacho and the rest of my friends in Córdoba. Many thanks also to the fantastic staff of the MAX-Laboratory (Helena, Martin, ix x ACKNOWLEDGEMENTS Mikael, and a long etc). It has been a pleasure to meet you and I hope we will see each other soon in the future. Also thanks to my colleagues from ELETTRA, Marcello, Monica, Robert and Kevin. From Lappis the list is neverending. Three years of living there give a lot of opportunities for meeting people. Thank you to all the little families that I have formed during these years and that have been key for my personal development and that have given me the love so that I could call Sweden my home (including, but not at all the only ones, Samer, Merche, Juancar, Marian, Óskar, my querido frente andaluz and well... I hope you know who you all are.
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