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glusac - PHOTOPHYSICS OF PLATINUM-ACETYLIDES By KSENIJA...

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PHOTOPHYSICS OF PLATINUM-ACETYLIDES By KSENIJA HASKINS-GLUSAC A DISSERTATION PRESENTED TO THE GRADUATE SCHOOL OF THE UNIVERSITY OF FLORIDA IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY UNIVERSITY OF FLORIDA 2003
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To the curious minds out there.
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ACKNOWLEDGEMENTS The years of graduate studies have been the most wonderful period of my life. During this period, I have grown both as a scientist and as a person. Here, I would like to acknowledge all those that helped this adventure be so pleasant by shining the light on my path and making sure that I am not lost. I thank my advisor, Dr. Kirk S. Schanze. He introduced me to photochemistry, the field that I grew to love and plan to investigate in years to come. Even more significantly, Kirk always encouraged me to think, create and not feel bad if I am wrong. I thank my committee members, Dr. Lisa McElwee-White, Dr. Michael Scott, Dr. John Reynolds and Dr. Stephen Schulman. Special gratitude I owe to Lisa and Michael. In many occasions they offered valuable help and advice related to chemistry, my future and my personal dilemmas. I thank all those that directly collaborated with me on my thesis projects. Dr. Khalil Abboud and Dr. Ion Ghiviriga conducted the X-ray and 2D NMR characterization of Pt- stilbene complex. Dr. Shujun Jiang and Thomas Cardiolaccia synthesized Pt-oligomer series. Dr. Mauricio Pinto synthesized polymers and model compounds presented in Chapter 4. I thank the members of Schanze research team. They have been great friends and coworkers for the last 4 years. Dr. Yao Liu has been my “junior” advisor. He showed me many aspects of physical chemistry, how to use instruments and how to be patient (that iii
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wonderful virtue of East). I will especially miss Eric Silverman and Garry Cunningham, these two “walking encyclopedias” have been great friends. I thank my parents, Ljubica and Dejan, for making me what I am today. I thank my husband, Will. He brought the colors to my life. Without him, none of this would have a meaning. iv
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TABLE OF CONTENTS page ACKNOWLEDGEMENTS. .............................................................................................. iii LIST OF TABLES. ........................................................................................................... vii LIST OF FIGURES . ........................................................................................................ viii ABSTRACT. ..................................................................................................................... xii CHAPTER 1 INTRODUCTION. ....................................................................................................... 1 Interaction of Light with Matter . .................................................................................. 1 Photons and Electrons: Particle-Wave Nature . ..................................................... 1 Absorption of Light . .............................................................................................. 2 Decay Processes of the Excited State. ................................................................... 3 Singlet-triplet splitting. ................................................................................... 5 Radiative decay (fluorescence and phosphorescence) . .................................. 9 Radiationless transitions (internal conversion and intersystem crossing) . ............................................................................. 10 Energy transfer . ............................................................................................ 13 Electron transfer . .......................................................................................... 16 Platinum Acetylides. ................................................................................................... 18 Synthetic approach . ............................................................................................. 18 Excited state properties. ....................................................................................... 19 2 PLATINUM-STILBENES . ........................................................................................ 29 Introduction. ................................................................................................................ 29 Results and Discussion . .............................................................................................. 33 Crystal Structure. ................................................................................................. 33 UV-Visible Absorption Spectroscopy. ................................................................ 34 Photoluminescence Spectroscopy . ...................................................................... 35 Transient Absorption Spectroscopy . ................................................................... 40 Photochemical Measurements. ............................................................................ 43 Photophysical Model: Pt(P) 2 ( C C Ar) 2 Complexes. ...................................... 45 Photophysical Model: Pt(bpy)( C C Ar) 2 Complexes . ................................... 48 Conlusions . ................................................................................................................. 50 Experimental. .............................................................................................................. 52 Syntheses. ............................................................................................................ 52 X-Ray Diffraction Analysis. ................................................................................ 57 v
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Photophysical Measurements. ............................................................................. 58 Photoisomerization Studies. ................................................................................ 60 3 PLATINUM OLIGOMERS .
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