Ultrafast Spectroscopy of Model Biological Membranes

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1 Ultrafast Spectroscopy of Model Biological Membranes

2 Ultrafast Spectroscopy of Model Biological Membranes Proefschrift ter verkrijging van de graad van Doctor aan de Universiteit Leiden, op gezag van de Rector Magnificus, Prof. Mr. Dr. Paul F. van der Heijden, volgens besluit van het College voor Promoties in het openbaar te verdedigen op Woensdag 2 September 2009 klokke uur door Avishek Ghosh geboren op 20 Augustus 1979 te London, U.K.

3 Promotiecommissie Promotor: Prof. Dr. Mischa Bonn Overige leden: Prof. Dr. Aart Kleyn Prof. Dr. Huib J Bakker Prof. Dr. Marc Koper Dr. Jens Bredenbeck Dr. Sander Woutersen Prof. Dr. Jaap Brouwer Prof. Dr. Geert-Jan Kroes Prof. dr. Marc C. van Hemert

4 This thesis is based on the following publications: 1. Avishek Ghosh, Marc Smits, Jens Bredenbeck, Niels Dijkhuizen and Mischa Bonn. Femtosecond time-resolved and 2D vibrational sum frequency spectroscopy to study structural dynamics at interfaces. Rev. Sci. Instrum. 79, (2008) 2. Marc Smits, Avishek Ghosh, Martin Sterrer, Michiel Muller, Mischa Bonn. Ultrafast Vibrational Energy Transfer between Surface and Bulk Water at the Air-Water Interface. Phys. Rev. Lett. 98, (2007) 3. Avishek Ghosh, Marc Smits, Jens Bredenbeck, Mischa Bonn. Membrane-bound water is energetically decoupled from nearby bulk water: An ultrafast surfacespecific investigation. J. Am. Chem. Soc. 129, (31), (2007) 4. Avishek Ghosh, Marc Smits, Maria Sovago, Jens Bredenbeck, Michiel Muller, Mischa Bonn. Ultrafast vibrational dynamics of interfacial water. Chem. Phys. 350, (1-3), (2008) 5. Avishek Ghosh, Maria Sovago, R. Kramer Campen and Mischa Bonn. Structure and dynamics of interfacial water in model lung surfactants. Faraday Discuss. 141, 1-15 (2008) 6. Marc Smits, Avishek Ghosh, Jens Bredenbeck, Susumu Yamamoto, Michiel Mller and Mischa Bonn. Ultrafast energy flow in model biological membranes. New J. Phys. 9, 390 (2007) 7. Avishek Ghosh, R.K. Campen and Mischa Bonn. Ultrafast vibrational dynamics of water at various lipid-water interfaces. (in preparation) Other Publications: Jens Bredenbeck, Avishek Ghosh, Marc Smits, Mischa Bonn. Ultrafast Two Dimensional-Infrared Spectroscopy of a Molecular Monolayer. J. Am. Chem. Soc. 130 (7), (2008) Jens Bredenbeck, Avishek Ghosh, Marc Smits, Han-Kwang Nienhuys and Mischa Bonn. Interface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy. Acc. Chem. Res. (in press) (Web published: May 14, 2009). contributed equally to this work

5 Contents Chapter 1 Introduction Interfaces - A General Perspective Interfaces in Biology Membranes and Interfacial Water Challenges in probing interfacial water Vibrational Sum Frequency Generation (VSFG) Spectroscopy - The Surface Probe Concepts in Nonlinear Polarization Sum Frequency Generation Vibrational Sum Frequency Generation at Interfaces Properties of χ (2) and surface-sensitivity of VSFG VSFG - A surface-specific IR probe Time-Resolved SFG Spectroscopy Thesis Outline Chapter 2 Experimental Technique Introduction Generation of Mid-IR and Visible upconversion pulses for VSFG Instrumentation at Sample Detection Schemes and Data Acquisition Software and Electronics Getting Started Chapter 3 Ultrafast Energy Transfer between Interfacial and Bulk Water at the Air-Water Interface Introduction Static and Time-resolved VSFG experiments Results and Discussion Static SFG Results Time-resolved SFG Results Conclusions Chapter 4 Ultrafast Dynamics of Water at various lipid-water interfaces Introduction Surface-specific Vibrational Spectroscopy: Frequency- and Time-Resolved Sum Frequency Generation

6 Contents 4.3 Experimental Section Results and Discussion Frequency-resolved SFG experiments Time-resolved SFG experiments DPTAP/H 2 O Interface DMPS/H 2 O Interface DPPC/H 2 O and DPPE/H 2 O Interface Conclusion Chapter 5 Structure and Dynamics of Water at Model Human Lung Surfactant interfaces Introduction Lung Surfactants and Interfacial Water Frequency- and Time-Resolved SFG on model lung surfactant monolayers on water Results and Analysis Frequency-resolved VSFG measurements Time-resolved SFG measurements Discussion Frequency-resolved SFG measurements Time-resolved SFG measurements Conclusions Chapter 6 Ultrafast energy flow in model biological membranes Introduction Time-resolved Surface Spectroscopy Steady-state Sum Frequency Generation Time-resolved Sum Frequency Generation Experiment Sample preparation Results Static SFG Spectra Time Resolved SFG Spectra DPPC DOPC Heat transfer across the monolayer Data Analysis Discussion Conclusions and Outlook Bibliography 91 Summary 104 Samenvatting 108 Dankwoord 112 Curriculum Vitae 114