Augulis, Ramunas

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Proceedings - University of Groningen

   University of GroningenMolecular aggregates, dendrimers, and motorsAugulis, RamunasIMPORTANT NOTE: You are advised to consult the publisher's version (publisher's PDF) if you wish to cite fromit. Please check the document version below.Document VersionPublisher's PDF, also known as Version of recordPublication date:2008Link to publication in University of Groningen/UMCG research databaseCitation for published version (APA):Augulis, R. (2008). Molecular aggregates, dendrimers, and motors: optical dynamics and control. s.n.CopyrightOther than for strictly personal use, it is not permitted to download or to forward/distribute the text or part of it without the consent of theauthor(s) and/or copyright holder(s), unless the work is under an open content license (like Creative Commons).The publication may also be distributed here under the terms of Article 25fa of the Dutch Copyright Act, indicated by the “Taverne” license.More information can be found on the University of Groningen website: https://www.rug.nl/library/open-access/self-archiving-pure/taverne-amendment.Take-down policyIf you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediatelyand investigate your claim.Downloaded from the University of Groningen/UMCG research database (Pure): http://www.rug.nl/research/portal. For technical reasons thenumber of authors shown on this cover page is limited to 10 maximum.Download date: 03-06-2022 Molecular Aggregates, Dendrimers, and Motors: Optical Dynamics and Control  Zernike Institute for Advanced Materials Ph.D. thesis series 2008-27 ISSN 1570-1530 ISBN printed version: 978-90-367-3641-1 ISBN electronic version: 978-90-367-3642-8  The work described in this thesis was performed in the group “Optical Condensed Matter Physics” (part of the Zernike Institute for Advanced Materials) of the University of Groningen, the Netherlands.  Printed by: Facultair Bedrijf RuG, Groningen  RIJKSUNIVERSITEIT GRONINGEN Molecular Aggregates, Dendrimers, and Motors: Optical Dynamics and Control Proefschrift  ter verkrijging van het doctoraat in de Wiskunde en Natuurwetenschappen aan de Rijksuniversiteit Groningen op gezag van de Rector Magnificus, dr. F. Zwarts, in het openbaar te verdedigen op maandag 24 november 2008 om 16.15 uur    door  Ramūnas Augulis geboren op 6 februari 1979 te Kaunas, Litouwen Promotores:    Prof. dr. Ir. P. H. M. van Loosdrecht     Prof. dr. J. Knoester Copromotor:   Dr. A. Pugžlys  Beoordelingscommissie: Prof. dr. L. Valkūnas      Prof. dr. V. Sundström     Prof. dr. P. F. Barbara ISBN: 978-90-367-3641-1 (printed version) ISBN: 978-90-367-3642-8 (electronic version) i Contents CHAPTER 1   INTRODUCTION ..........................................................................................1 I. MOTIVATION................................................................................................................. 1 II. THESIS OVERVIEW ....................................................................................................... 2 REFERENCES .................................................................................................................... 3 CHAPTER 2   OPTICAL ENERGY TRANSPORT AND INTERACTIONS BETWEEN THE EXCITATIONS IN A COUMARIN – PERYLENE BISIMIDE DENDRIMER .....7 ABSTRACT ....................................................................................................................... 7 I. INTRODUCTION ............................................................................................................. 7 II. MATERIALS AND METHODS.......................................................................................... 9 III. RESULTS AND DISCUSSION ....................................................................................... 10 A. Donor-acceptor ET in C4P: qualitative description ...................................................10 B. ET at low excitation density.........................................................................................13 C. Analytical description of ET dynamics in C4P at high excitation density ..................16 D. ET at high excitation density: experimental results ....................................................19 E. Control of the ET rate: pre-pump – pump – probe experiment...................................21 IV. SUMMARY AND CONCLUSIONS ................................................................................. 23 REFERENCES .................................................................................................................. 23 CHAPTER 3   CYLINDRICAL AGGREGATES OF 5,5',6,6'-TETRA- CHLOROBENZIMIDACARBOCYANINE AMPHIPILIC DERIVATIVES: STRUCTURE RELATED OPTICAL PROPERTIES AND EXCITON DYNAMICS...27 ABSTRACT ..................................................................................................................... 27 I. INTRODUCTION ........................................................................................................... 27 II. OPTICAL PROPERTIES OF CYLINDRICAL AGGREGATES ................................................ 29 III. EXCITON DYNAMICS................................................................................................. 33 IV. CONCLUSIONS .......................................................................................................... 38 REFERENCES .................................................................................................................. 39 CHAPTER 4   TEMPERATURE-DEPENDENT RELAXATION OF EXCITONS IN TUBULAR MOLECULAR AGGREGATES: FLUORESCENCE DECAY AND STOKES SHIFT.....................................................................................................................41 ABSTRACT ..................................................................................................................... 41 I. INTRODUCTION ........................................................................................................... 41 II. SAMPLE PREPARATION AND EXPERIMENTAL SETUP.................................................... 43 III. EXPERIMENTAL RESULTS.......................................................................................... 43 A. Steady-state spectra.....................................................................................................43 B. Spectrally resolved fluorescence decay.......................................................................45 C. Dynamic stokes shift of the fluorescence spectrum .....................................................47 IV. MODEL CALCULATIONS............................................................................................ 50 Α. Aggregate structure and absorption spectrum ............................................................50 Β. Modeling the spectral dynamics ..................................................................................53 V. SUMMARY AND CONCLUDING REMARKS.................................................................... 56 REFERENCES AND NOTES................................................................................................ 57 CONTENTS  ii CHAPTER 5   RELAXATION OF EXCITONS IN TUBULAR MOLECULAR AGGREGATES AT LOW TEMPERATURES: TIME-RESOLVED TRANSIENT ABSORPTION DYNAMICS ................................................................................................61 ABSTRACT ..................................................................................................................... 61 I. INTRODUCTION ........................................................................................................... 61 II. EXPERIMENT.............................................................................................................. 62 III. RESULTS AND DISCUSSION ....................................................................................... 63 IV. CONCLUSIONS .......................................................................................................... 66 REFERENCES .................................................................................................................. 66 CHAPTER 6   LEVEL REPULSION IN LINEAR MOLECULAR J-AGGREGATES 69 ABSTRACT ..................................................................................................................... 69 I. INTRODUCTION ........................................................................................................... 69 II. SAMPLE PREPARATION AND EXPERIMENTAL SETUPS.................................................. 70 III. THEORETICAL BACKGROUND ................................................................................... 71 A. Hidden structure of the Lifshits tail .............................................................................71 B. Relaxation model .........................................................................................................73 C. Inter-segment vs. intra-segment relaxation.................................................................74 IV. EXPERIMENTAL RESULTS AND DISCUSSION .............................................................. 75 A. Continuous wave experiments .....................................................................................75 B. Time-resolved experiments ..........................................................................................77 C. Data extraction procedure ..........................................................................................81 D. Discussion ...................................................................................................................83 V. SUMMARY AND CONCLUDING REMARKS.................................................................... 85 REFERENCES .................................................................................................................. 85 CHAPTER 7   EXCITON SPECTRA AND MICROSCOPIC STRUCTURE OF  SELF-ASSEMBLED PORPHYRIN NANOTUBES...........................................................89 ABSTRACT ..................................................................................................................... 89 I. INTRODUCTION ........................................................................................................... 89 II. MATERIALS AND METHODS........................................................................................ 91 A. Preparation of TPPS4 aggregates ...............................................................................91 B. Cryo-electron microscopy ...........................................................................................91 C. Absorption and linear dichroism spectroscopy...........................................................92 III. EXPERIMENTAL RESULTS.......................................................................................... 92 IV. MODEL..................................................................................................................... 94 A. The cylindrical geometry .............................................................................................95 B. Hamiltonian and spectra .............................................................................................97 C. Ordered aggregate and optical selection rules ...........................................................99 D. Effects of disorder .....................................................................................................100 V. COMPARISON TO EXPERIMENT................................................................................. 101 A. Parameters ................................................................................................................101 B. Results........................................................................................................................103 VI. CONCLUSIONS ........................................................................................................ 105 APPENDIX: EXPRESSIONS FOR THE ABSORPTION SPECTRA ............................................ 106 REFERENCES AND NOTES.............................................................................................. 107 CHAPTER 8   LIGHT-DRIVEN ROTARY MOLECULAR MOTORS:  AN ULTRAFAST OPTICAL STUDY...............................................................................111 ABSTRACT ................................................................................................................... 111 CONTENTS   iii I. INTRODUCTION ......................................................................................................... 111 II. EXPERIMENTS AND RESULTS.................................................................................... 113 A. Experimental setup and samples ...............................................................................113 B. Experimental results ..................................................................................................113 C. Interpretation of the results.......................................................................................115 III. SUMMARY AND CONCLUSIONS ............................................................................... 117 REFERENCES ................................................................................................................ 117 SYNOPSIS ............................................................................................................................119 SANTRAUKA ......................................................................................................................121 LITERATŪROS SĄRAŠAS ............................................................................................... 124 SAMENVATTING ..............................................................................................................127 REFERENTIES ............................................................................................................... 130 ACKNOWLEDGEMENTS ................................................................................................133 CURRICULUM VITAE......................................................................................................137 LIST OF PUBLICATIONS ................................................................................................139 

Molecular aggregates, dendrimers, and motors:optical dynamics and control

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Molecular aggregates, dendrimers, and motors:optical dynamics and control

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Proceedings - University of Groningen