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UNIVERSITY of CALIFORNIA Santa Barbara Bio-Inspired Adhesion UNIVERSITY OF CALIFORNIA Santa Barbara Bio-Inspired Adhesion, Friction and Lubrication A dissertation submitted in partial satisfaction of the requirements for the degree Doctor of Philosophy in Chemical Engineering by Saurabh Basudeb Das Committee in charge: Professor Jacob N. Israelachvili, Chair Professor Todd M. Squires Professor Michael J. Gordon Professor Kimberly L. Turner December 2014 The dissertation of Saurabh Basudeb Das is approved. _____________________________________________ Professor Todd M. Squires _____________________________________________ Professor Michael J. Gordon _____________________________________________ Professor Kimberly L. Turner _____________________________________________ Professor Jacob N. Israelachvili, Chair December 2014 Bio-Inspired Adhesion, Friction and Lubrication Copyright © 2014 Saurabh Basudeb Das iii ACKNOWLEDGEMENTS During my stint as a doctoral researcher at UCSB, I investigated multiple problems in interfacial science and engineering along with collaborators from mechanical engineering, materials science, chemistry, and molecular and marine biology. All this would have not been possible without the support and guidance of my PhD advisor Prof. Jacob Israelachvili. He encouraged and cultivated a collaborative research environment in his group and this has immensely contributed to my success as a PhD student. He taught me to ask the right questions and I express my gratitude and respect to him for enabling me to grow as a Scientist. I would also like to thank my many other lab members who supported me from a professional perspective. I am grateful to Travers Anderson, Stephen Donaldson, Xavier Banquy, Wren Greene and Jing Yu who taught me the SFA technique. I worked together with Nadine Martinez, Nick Cadirov and Kollbe Ahn on many different projects and resolved technical and scientific challenges efficiently in matters of weeks. I am thankful to Wei Wei and Dusty Miller for providing mussel foot proteins and peptides. I greatly appreciate the company of my very close friends (and colleague) Himanshu Mishra and Yair Kaufman for their support and advice. I am thankful to Sandy Chen, Alex Schrader and Dong Woog Lee who made work for me a fun-filled and an entertaining experience. Many thanks to Kai Kristiansen and Greg Carver who helped me troubleshoot technical problems with the instruments in the lab. Nancy Emerson was my guardian in the States and I appreciate all her support for numerous occasions. Prof. Herbert Waite gave countless suggestions and insightful thoughts into the biochemistry aspect of my research. I want to thank my committee members, Prof. Todd Squires, Prof. Mike Gordon and Prof. iv Kim Turner for taking the time to review my research progress annually and providing helpful suggestions. I dedicate this Dissertation to my parents and cannot thank them enough for all of their love and support during my PhD studies and throughout my life. I am grateful to all of my local and international friends at UCSB with whom I share many sweet memories for years to come, esp., with Rodrigo Nery Azevedo and Aviel Chaimovich. Finally I thank the funding agencies: Procter & Gamble, Institute of Collaborative Biotechnologies, National Institute of Health and The Department of Energy. v VITA of SAURABH BASUDEB DAS December, 2014 EDUCATION 2009 Bachelor of Chemical Engineering Chemical Engineering University Institute of Chemical Technology, Mumbai 2014 Doctor of Philosophy Chemical Engineering University of California, Santa Barbara PEER-REVIEWED JOURNAL ARTICLES Das, S.; Rodriguez, N. R. M.; Wei, W.; Waite, J. H.; Israelachvili, J. N. Peptide length and Dopa Contribution to Metal Mediated Chelation of Peptides. Submitted 2014. Das, S.; Miller, D. R.; Kaufman, Y.; Rodriguez, N. R. M.; Israelachvili, J.; Waite, J. H. Tough Coating proteins: Subtle Sequence Variation Modulates Cohesion. Submitted 2014. Das, S.; Miller, D. R.; Huang, K. Y.; Han, S.; Israelachvili, J.; Waite, J. H. Mussel-Inspired Complex Coacervate Provide Enhanced Wear Protection to Surfaces. Submitted 2014. Das, S.; Cadirov, N.; Chary, S.; Kaufman, Y.; Hogan, J.; Turner, K.; Israelachvili, J. Stick- slip Friction of Gecko Mimetic Flaps on Smooth and Rough Surfaces. Submitted 2014. Das, S.; Ahn, B. K.; Rodriguez, N. R. M.; Rinstadt, R.; Kaufman, Y.; Kesselman, E.; Mirshafian, R.; Lipshutz, B.; Talmon, Y.; Israelachvili, J.; Waite, J. H. Small Molecular Underwater Adhesives Inspired by Mussel Foot Proteins. Submitted 2014. Rodriguez, N. R. M.; Das, S.; Kaufman, Y.; Israelachvili, J.; Waite, J. H. Interfacial pH During Mussel Adhesive Plaque Formation. Submitted 2014. Rodriguez, N. R. M.; Das, S.; Kaufman, Y.; Wei, W.; Israelachvili, J.; Waite, J. H. Mussel adhesive protein provides cohesive matrix for collagen type-1α. Biomaterials (accepted) 2014. vi Lee, D. W.; Banquy, X.; Das, S.; Cadirov, N.; Jay, G.; Israelachvili, J. Effects of Molecular Weight of Grafted Hyaluronic Acid on Wear Initiation. Acta Biomater 2014, 10 (5), 1817- 1823. Banquy, X.; Lee, D. W.; Das, S.; Hogan, J.; Israelachvili, J. N. Shear-Induced Aggregation of Mammalian Synovial Fluid Components under Boundary Lubrication Conditions. Adv Funct Mater 2014, 24 (21), 3152-3161. Rapp, M.; Donaldson, S.; Gebbie, M.; Das, S.; Kaufman, Y.; Gizaw, Y.; Koenig, P. H.; Israelachvili, J. Hydrophobic, Electrostatic, and Dynamic Polymer Forces at Silicone Surfaces Modified with Long-Chain Bolaform Surfactants. Small 2014, in press. Yu, J.; Kan, Y. J.; Rapp, M.; Danner, E.; Wei, W.; Das, S.; Miller, D. R.; Chen, Y. F.; Waite, J. H.; Israelachvili, J. N. Adaptive Hydrophobic and Hydrophilic Interactions of Mussel Foot Proteins with Organic Thin Films. P Natl Acad Sci USA 2013, 110 (39), 15680-15685. Nicklisch, S. C. T.; Das, S.; Rodriguez, N. R. M.; Waite, J. H.; Israelachvili, J. N. Antioxidant Efficacy and Adhesion Rescue by a Recombinant Mussel Foot Protein-6. Biotechnol Progr 2013, 29 (6), 1587-1593. Israelachvili, J. N.; Kristiansen, K.; Gebbie, M. A.; Lee, D. W.; Donaldson, S. H.; Das, S.; Rapp, M. V.; Banquy, X.; Valtiner, M.; Yu, J. The Intersection of Interfacial Forces and Electrochemical Reactions. J Phys Chem B 2013, 117 (51), 16369-16387. Israelachvili, J.; Donaldson, S.; Das, S.; Gebbie, M.; Rapp, M. Interactions of Soft-particles (vesicles, etc.) in Complex Fluid Systems. Abstr Pap Am Chem S 2013, 246. Donaldson, S. H.; Das, S.; Gebbie, M. A.; Rapp, M.; Jones, L. C.; Roiter, Y.; Koenig, P. H.; Gizaw, Y.; Israelachvili, J. N. Asymmetric Electrostatic and Hydrophobic-Hydrophilic Interaction Forces between Mica Surfaces and Silicone Polymer Thin Films. Acs Nano 2013, 7 (11), 10094-10104. Donaldson, S.; Valtiner, M.; Kristiansen, K.; Royne, A.; Gebbie, M.; Rapp, M.; Das, S.; Chmelka, B.; Israelachvili, J. Development of a General Interaction Potential for Hydrophobic and Hydrophilic Interactions. Abstr Pap Am Chem S 2013, 246. Das, S.; Donaldson, S. H.; Kaufman, Y.; Israelachvili, J. N. Interaction of Adsorbed Polymers with Supported Cationic Bilayers. Rsc Adv 2013, 3 (43), 20405-20411. Das, S.; Chary, S.; Yu, J.; Tamelier, J.; Turner, K. L.; Israelachvili, J. N. JKR Theory for the Stick Slip Peeling and Adhesion Hysteresis of Gecko Mimetic Patterned Surfaces with a Smooth Glass Surface. Langmuir 2013, 29 (48), 15006-15012. Das, S.; Banquy, X.; Zappone, B.; Greene, G. W.; Jay, G. D.; Israelachvili, J. N. Synergistic Interactions between Grafted Hyaluronic Acid and Lubricin Provide Enhanced Wear Protection and Lubrication. Biomacromolecules 2013, 14 (5), 1669-1677. vii Yu, J.; Chary, S.; Das, S.; Tamelier, J.; Turner, K. L.; Israelachvili, J. N. Friction and Adhesion of Gecko-Inspired PDMS Flaps on Rough Surfaces. Langmuir 2012, 28 (31), 11527-11534. Yu, J.; Chary, S.; Das, S.; Tamelier, J.; Pesika, N. S.; Turner, K. L.; Israelachvili, J. N. Gecko-Inspired Dry Adhesive for Robotic Applications. Adv Funct Mater 2011, 21 (16), 3010-3018. Tamelier, J.; Chary, S.; Turner, K.; Yu, J.; Das, S.; Israelachvili, J. Millimeter Size Patch Behavior of Gecko-Inspired Reversible Adhesive. 2011 Ieee Sensors 2011, 1819-1822. BOOK CHAPTER Greene, G. W.; Lee, D. W.; Yu, J.; Das, S.; Banquy, X.; Israelachvili, J. N., Lubrication and Wear Protection of Natural (Bio)Systems. In Polymer Adhesion, Friction, and Lubrication, John Wiley & Sons, Inc.: 2013; pp 83-133. SELECTED CONFERENCE PRESENTATIONS Das, S., Miller, D., Kaufman, Y., Martinez, N., Isralelachvili, J.N., Waite, H., “Tough Coating proteins: Subtle Sequence Variation Modulates Cohesion”, 2nd International Conference on Biological and Biomimetic Adhesives, Istanbul, Turkey, 2014. Das, S.; Chary, S.; Tamelier, J.; Hogan, H.; Yu, J.; Turner, K.; Israelachvili, J., "Frictional Adhesion and Stick-slip Friction of Patterned Surfaces with Smooth and Rough Glass Surfaces", International Nanotribology Forum, Kochi, Kerala, Jan 2014. Das, S.; Yu, J.; Chary, S.; Tamelier, J.; Turner, K.; Israelachvili, J., “A Modified JKR Theory for the Adhesion of Patterened Surfaces Against Smooth Glass Surface”, Gordon Research Conference of Adhesion, South Hadley MA, July 2013. Das, S.; Donaldson Jr., S.; Israelachvili, J., “Polyacrylamide Induced Thinning and Increase in Head Group Area of Supported Cationic Bilayers”, AIChE, Pittsburgh PA, Nov 2012. Das, S.; Banquy, X.; Zappone, B.; Greene, G.; Jay, G.; Israelachvili, J., “Synergistic Interactions between Grafted Hyaluronic acid and Lubricin Provide Enhanced Wear Protection and Lubrication”, Gordon Research Conference of Tribolgy, Waterville ME, July 2012. Das, S.; Yu, J.; Chary,
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