Bio-inspired self-assembly. Anant K. Paravastu Department of Chemical and Biomedical Engineering Florida A&M University and Florida State University

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1 Bio-inspired self-assembly Anant K. Paravastu Department of Chemical and Biomedical Engineering Florida A&M University and Florida State University

2 Self-assembly in biology Multi-scale extracellular matrices membranes and vesicles organelles cells tissue organs organisms Multi-component Environment responsive Self-healing 37 C, atmospheric pressure, water

3 Research thrusts to date Materials science biomimetics biomedical engineering: drug delivery, gene delivery, artificial extracellular matrices, bioimaging, sensing Study of disease protein misfolding virus capsid assembly

4 Molecular building blocks DNA Amphiphilic molecules Peptides and proteins Bio-inspired molecules peptoids FMOC-FF Hybrid molecules peptide amphiphiles protein-polymer hybrids Larger Materials with bio-inorganic interfaces

5 Recent advances: DNA Gates, E. P.; Dearden, A. M.; Woolley, A. T. Crit. Rev. Anal. Chem. 2014, 44, Mohri, K.; Nishikawa, M.; Takahashi, Y.; Takakura, Y. Eur. J. Pharm. Sci , Tintoré, M.; Eritja, R.; Fábrega, C. Chembiochem. 2014, 15,

6 Recent advances: amphiphilic molecules Barclay, T. G.; Constantopoulos, K.; Matisons, J. Chem Rev. 2014, 114, Hill, J. P.; Shrestha, L. K.; Ishihara, S.; Ji, Q.; Ariga, K. Molecules. 2014, 19,

7 Recent advances: peptides/proteins Woolfson, D.N.; Mahmoud, Z.N. Chem. Soc. Rev., 2010, 39, 3464.

8 Recent advances: peptides/proteins Matson, J.B.; Zha, R. H.; Stupp, S. I. Curr. Opin. Solid State Mater. Sci. 2001, 15, Likjestrom, V.; Mikkila, J.; Kostiainen, M.A. Nat. Comm. 2014, 5, 1-9

9 Recent advances: Bioinspired/hybrid molecules Scanlon, S.; Aggeli, A. Nanotoday, 2008, 3, 3-4. Vandermeulen, G. W. M.; Klok, H. Macromol. Biosci. 2004, 4,

10 Observations Most work seems to be application driven Most literature is about properties, not mechanisms Little discussion of manufacturing and scalability Each application could be accomplished by multiple material designs Empiricism outpaces understanding Computational/theoretical methods may be key to progress

11 Materials Synthesis Challenges How do we better address heterogeneity in the synthesis of well defined building blocks for self-assembly? As materials complexity increases (e.g. increasing # of constituents) will combinatorial materials synthesis become more important? How do we achieve nanomanufacturing of materials at scales relevant for applications? Cormier, A.R.; Ruiz-Orta, C.; Alamo, R.G.; Paravastu, A.K. Biomacromolecules 2012, 13, 1794.

12 Challenges in Self-Assembly Structures As the # of constituents in self-assembly increases how do we address the question of pathway complexity? Out of the large # of possible directions how do we best explore non-equilibrium derived self-assembly structures? Moving beyond static structures how can meaningful dynamically responsive structures be designed from self-assembly? Self-assembly of Alzheimer s b-amyloid: Roychaudhuri, R., D.B. Teplow, et. al. J. Biol. Chem. 2009, 284, 4749.

13 Challenges associated with Order in Self-Assembled Structures What are the fundamental issues associated with defect control in self-assembled structure? Can we mimic nature to generate defect-free or defect-repair structures? How can we generate hierarchical structures with simple methodologies? Ma, J.; Wang, J.; Ai, X.; Zhang, S. Biotech. Adv. 2014, George, A.; Ravindran, S. Nano Today, 2010, 5, 254.

14 Challenges with Characterizing Dynamics in Self-Assembled Structures As the complexity of self-assembled structure increases how can we keep up with understanding the associated dynamical features of such systems? What novel methods need to be developed to better characterize the dynamics of complex self-assembled systems? Considering the complexity of self-assembled systems, is there a meaningful role for materials by design efforts? Yokoi, H., T. Kinoshita, and S. G. Zhang. Proc. Natl. Acad. Sci USA 2005, 102, Cheng, L., Englander, O.E., Paravastu, A.K., Oates, W.S. J. Chem. Phys. 2011, 135,

15 DNA self-assembly: Bath, J. ; Turberfield A. J. Nat. Nanotechnol. 2007, 2, Bell, N. A.W.; Keyser, U. F. FEBS. Lett , Gates, E. P.; Dearden, A. M.; Woolley, A. T. Crit. Rev. Anal. Chem. 2014, 44, Mohri, K.; Nishikawa, M.; Takahashi, Y.; Takakura, Y. Eur. J. Pharm. Sci , Tintoré, M.; Eritja, R.; Fábrega, C. Chembiochem. 2014, 15, Wang, Z.G.; Ding, B. Acc. Chem. Res. 2014, 47, Amphiphilic molecules: Barclay, T. G.; Constantopoulos, K.; Matisons, J. Chem Rev. 2014, 114, Hill, J. P.; Shrestha, L. K.; Ishihara, S.; Ji, Q.; Ariga, K. Molecules. 2014, 19, Peptide Amphiphiles: Tan, A.; Rajadas, J.; Seifalian, A. M. J. Control. Release. 2012, 163, Trent, A.; Marullo R.; Lin, Brian.; Black, Matthew.; Tirrell, Matthew. Soft Matter, 2011, 7, He, B.; Yuan, Xiao.; Jiang, Dianming. RSC Adv. 2014, 4, FMOC-FF self-assembly and applications: Scanlon, S.; Aggeli, A. Nanotoday, 2008, 3, 3-4. Protein folding and mis-folding: Dobson, C.M. Sem Cell. Dev. Biol. 2004, 15, 3-16.

16 Natural Protein Self-Assembly: Daamena,W.F.; Veerkampa, J.H.; van Hestb, J.C.M.; van Kuppevelt, T.H. Biomaterials. 2007, 28, Peptide nanotubes (including FMOC-FF): Gao, X.; Matsui, H. Adv. Mater. 2005, Designer peptide self-assembly: Matson, J.B.; Zha, R. H.; Stupp, S. I. Curr. Opin. Solid State Mater. Sci. 2001, 15, Woolfson, D.N.; Mahmoud, Z.N. Chem. Soc. Rev., 2010, 39, Plamer, L. C.; Stupp, S. I. Acc. Chem. Res. 2008, 41, Rajagopal, K. Schneider, J. P.; Curr. Opin. Struct. Biol. 2004, 14, Zhang, S. Biotechnol. Adv. 2002, 2, Zhang, S.; Marini, D. M.; Hwang, W.; Santoso, S. Biopolymers. Curr. Opin. Chem. Biol. 2002, 6, Panda, J.J.; Chauhan, V.S.; Polym. Chem. 2014, 5, Hierarchical biological self-assembly: Ma, J.; Wang, J.; Ai, X.; Zhang, S. Biotech. Adv. 2014, George, A.; Ravindran, S. Nano Today, 2010, 5, 254.