Jeffrey D. Hartgerink
Professor of Chemistry and Professor of Bioengineering
Supramolecular chemistry is an emerging sub-discipline of chemistry that primarily concerns itself with non-covalent intermolecular interactions. These relatively weak forces are used in large number to create nanometer sized objects in a massively parallel fashion. The inspiration for this area of research comes primarily from advances in our understanding of biological systems and the miraculous structures found therein. Great strides have been made to mimic both the structures found in biological systems and the approaches that biology uses to create these structures. Although many of these advances are truly remarkable, and many may find practical application in the future, a situation has arisen where we are able to produce materials which have no easy method of manipulation or organization into higher order structures. It is analogous to being able to produce a wheel and an axle and having no way to connect them to one another, let alone to a cart. Alternatively one could compare this stage of supramolecular chemistry to traditional organic synthesis of a century ago when the number of chemical transformation and protecting groups were severely limited. In order to bring supramolecular chemistry to a new level of sophistication methods by which two or more supramolecular objects can be coupled or organized must be developed.
My research is directed at solving this problem by employing a second step of self-assembly, covalent capture and / or mineralization to create complex and functional assemblies. Three projects are starting in my lab which address this. The first uses the self-assembly of ?coiled-coils? (a pair of alpha-helical peptides wound around one another) as a framework for the secondary self-assembly of a conductive organic matrix to form wires with nanometer dimensions. These wires, unlike most other approaches to nanoscale electronics, may be able to organize themselves in neural networks that can readily interface with traditional electronics. The second project is geared toward the synthesis of an artificial extracellular matrix (ECM) for use as a drug and cell delivery vehicle and tissue regeneration therapies. This biomimetic material will be prepared through two steps of self-assembly followed by covalent capture. The third project targets the synthesis of novel catalysts and magnetic materials. The preparation of these materials uses the mechanisms involved in biomineralization that allow biology to create an amazing diversity of inorganic and composite materials such as shells, teeth and bone.
V. A. Kumar, N. L. Taylor, A. A. Jalan, L. K. Hwang, B. K. Wang, Jeffery D. Hartgerink “A Novel Synthetic Collagen Mimic for Hemostasis” Biomacromolecules 2014, 15, 1484−1490. DOI: dx.doi.org/10.1021/bm500091e.
D. Zhang, O. Neumann, H. Wang, V. M. Yuwono, A. Barhoumi, M. Perham, J. D. Hartgerink, P. Wittung-Stafshede and N. J. Halas "Gold Nanoparticles Can Induce the Formation of Protein-based Aggregates at Physiological pH" Nano Lett., 9 (2009) : 666-671.
A. A. Jalan, K. A. Jochim, J. D. Hartgerink “Rational Design of a Non-canonical “Sticky-ended” ABC-Collagen Triple Helix” J. Am. Chem. Soc., 2014, 136, 7535-7538. DOI: dx.doi.org/10.1021/ja5001246.
J. S. Colombo, A. N. Moore, J. D. Hartgerink, R. N. D’Souza “Scaffolds to Control Inflammation and Facilitate Dental Pulp Regeneration” J. Endodontics, 2014, 40, S6-S12. DOI: dx.doi.org/10.1016/j.joen.2014.01.019.
B. Sarkar, L. E. R. O’Leary, J. D. Hartgerink “Self-Assembly of Fiber-Forming Collagen Mimetic Peptides Controlled by Triple-Helical Nucleation” J. Am. Chem. Soc., 2014, 136, 14417-14424. DOI: dx.doi.org/10.1021/ja504377s.
L. Aulisa, H. Dong and J. D. Hartgerink "Self-Assembly of Multidomain Peptides: Sequence Variation Allows Control over Cross-Linking and Viscoelasticity" Biomacromolecules, 10 (2009) : 2694-2698.
M. K. Kang, J. Colombo, R.N. D'Souza, J. D. Hartgerink “Sequence effects of self-assembling MultiDomain Peptide Hydrogels on encapsulated SHED cells” Biomacromolecules, 2014, 15, 2004-2011. DOI:dx.doi.org/10.1021/bm500075r.
J. A. Fallas, V. Gauba and J. D. Hartgerink "Solution structure of an ABC collagen heterotrimer reveals a single-register helix stabilized by electrostatic interactions" J. Biol. Chem., 284 (2009) : 26851-26859.
N. C. Wickremasinghe, V. A. Kumar, J. D. Hartgerink “Two-Step Self-Assembly of Liposome-Multidomain Peptide Nanofiber Hydrogel for Time-Controlled Release” Biomacromolecules, 2014 15, 3587-3595. DOI: dx.doi.org/10.1021/bm500856c.
Amanda M. Acevedo-Jake, Abhishek A. Jalan, and Jeffrey D. Hartgerink “Comparative NMR Analysis of Collagen Triple Helix Organization from N- to C-Termini” Biomacromolecules, 2014 available online. DOI: dx.doi.org/10.1021/bm501281a.
A. A. Jalan, B. Demeler, J. D. Hartgerink Hydroxyproline-Free Single Composition ABC Collagen. J. Am. Chem. Soc., 135 2013: 6014-6017
A. A. Jalan, J. D. Hartgerink Pairwise interactions in collagen and the design of heterotrimeric helices. Curr. Opin. Chem. Biol., 17 2013: 960-967
E. L. Bakota, O. Sensoy, B. Ozgur, M. Sayar, J. D. Hartgerink Self-Assembling Multidomain Peptide Fibers with Aromatic Cores. Biomacromolecules, 14 2013: 1370-1378
A. A. Jalan, J. D. Hartgerink Simultaneous Control of Composition and Register of an AAB-Type Collagen Heterotrimer. Biomacromolecules, 14 2013: 179-185
K. M. Galler, J. D. Hartgerink, A. C. Cavender, G. Schmalz, and R. N. D'Souza A Customized Self-Assembling Peptide Hydrogel for Dental Pulp Engineeering. Tissue Eng. Part A, 18 2012: 176-184
J. A. Fallas and J. D. Hartgerink Computational design of self-assembling register-specific collagen heterotrimers. Nat. Commun., 3 2012: 1087
J. A. Fallas, M. A. Lee, A. A. Jalan, and J. D. Hartgerink Rational Design of Single-Composition ABC Collagen Heterotrimers. J. Am. Chem. Soc., 134 2012: 1430-1433
F. Wei, J. A. Fallas, J. D. Hartgerink Sequence Position and Side Chain Length Dependence of Charge Pair Interactions in Collagen Triple Helices. Macromol. Rapid Commun., 33 2012: 1445-1452
J. A. Fallas, J. Dong, Y. J. Tao, and J. D. Hartgerink Structural Insights into Charge Pair Interactions in Triple Helical Collagen-like Proteins. J. Biol. Chem., 287 2012: 8039-8047
E. L. Bakota, L. Aulisa, K. M. Galler and J. D. Hartgerink Enzymatic Cross-Linking of a Nanofibrous Peptide Hydrogel. Biomacromolecules, 12 2011: 82-87
E. L. Bakota, Y. Wang, F. R. Danesh and J. D. Hartgerink Injectable Multidomain Peptide Nanofiber Hydrogel as a Delivery Agent for Stem Cell Secretome. Biomacromolecules, 12 2011: 1651-1657
W. C. Pomerantz, V. M. Yuwono, R. Drake, J. D. Hartgerink, N. L. Abbott and S. H. Gellman Lyotropic Liquid Crystals Formed from ACHC-Rich β-Peptides. J. Am. Chem. Soc., 133 2011: 13604-13613
L. E. R. O'Leary, J A. Fallas, E. L. Bakota, M. K. Kang and J. D. Hartgerink Multi-hierarchical self-assembly of a collagen mimetic peptide fro triple helix to nanofiber and hydrogel. Nat. Chem., 3 2011: 821-828
Y. Wang, E. Bakota, B. H. J. Chang, M. Entman, J. D. Hartgerink, and F. R. Danesh Peptide Nanofibers Preconditioned with Stem Cell Secretome Are Renoprotective. J. Am. Soc. Nephrology, 22 2011: 704-717
L. E. R. O'Leary, J. A. Fallas and J. D. Hartgerink Positive and Negative Design Leads to Compositional Control in AAB Collagen Heterotrimers. J. Am. Chem. Soc., 133 2011: 5432-5443
K. M. Galler, R. N. D'Souza, J. D. Hartgerink, and G. Schmalz Scaffolds for Dental Pulp Tissue Engineering. Adv. Dent. Res., 23 2011: 333-339
K. M. Galler, R. N. D'Souza and J. D. Hartgerink Biomaterials and their Potential Applications for Dental Tissue Engineering. J. Mater. Chem., 20 2010: 8730-8746
E. L. Bakota, L. Aulisa, D. A. Tsyboulski, R. B. Weisman and J. D. Hartgerink Multidomain Peptides as Single-Walled Carbon Nanotube Surfactants in Cell Culture. Biomacromolecules, 10 2010: 2201-2206
L. E. Russell, J. A. Fallas and J. D. Hartgerink Selective Assembly of a High Stability AAB Collagen Heterotrimer. J. Am. Chem. Soc., 132 2010: 3242-3243
K. M. Galler, L. Aulisa, K. R. Regan, R. N. D'Souza and J. D. Hartgerink Self-assembling Multidomain Peptide Hydrogels: Designed Susceptibility to Enzymatic Cleavage Allows Enhanced Cell Migration and Spreading. J. Am. Chem. Soc., 132 2010: 3217-3223
J. A. Fallas, L. E. R. O'Leary and J. D. Hartgerink Synthetic collagen mimics: self-assembly of homotrimers, heterotrimers and higher order structures. Chem. Soc. Rev., 39 2010: 3510-3527
F. Wei, D. Zhang, N. J. Halas and J. D. Hartgerink Aromatic amino acids provide characteristic motifs in the Raman and SERS spectroscopy of Peptides. J. Phys. Chem. B, 113 2008: 9158-9164
C. L. Pizzey, W. C. Pomerantz, B.-J. Sung, V. M. Yuwono, S. H. Gellman, J. D. Hartgerink, A. Yethiraj, N. L. Abbott Characterization of nanofibers formed by self-assembly of beta-peptide oligomers using small angle x-ray scattering. J. Chem. Phys., 129 2008: 095103
W. C. Pomerantz, V. M. Yuwono, C. L. Pizzey, J. D. Hartgerink, N. L. Abbott, S. H. Gellman Nanofibers and Lyotropic Liquid Crystals from a Class of Self-Assembling Beta-Peptides. Angew. Chem. Int. Ed., 47 2008: 1241-1244
K. M. Galler, A. Cavender, V. Yuwono, H. Dong, S. Shi, G. Schmalz, J. D. Hartgerink and R. N. D'Souza Self-Assembling Peptide Amphiphile Nanofibers as a Scaffold for Dental Stem Cells. Tissue Eng., 14 2008: 2051-2058
D. Tsyboulski, E. Bakota, L. Witus, J-D. Rocha, J. D. Hartgerink, R. B. Weisman Self-Assembling Peptide Coatings Designed for Highly Luminescent Suspensions of Single-Walled Carbon Nanotubes. J. Am. Chem. Soc., 130 2008: 17134-17140
H. Dong, S. E. Paramonov and J. D. Hartgerink Self-assembly of alpha-helica coiled-coil nanofibers. J. Am. Chem. Soc., 130 2008: 13691-13695
V. Gauba and J. D. Hartgerink Synthetic Collagen Heterotrimers: Structural Mimics of Wild Type and Mutant Collagen Type I. J. Am. Chem. Soc., 130 2008: 7509-7515
H-W. Jun, S. E. Paramonov, H. Dong, N. Forraz, C. McGuckin, and J. D. Hartgerink Tuning the mechanical and bioresponsive properties of peptide-amphiphile nanofiber networks. J. Biomater. Sci. Polymer Edn., 19 2008: 665-676
V. Gauba and J. D. Hartgerink Recent Advances in Supramolecular Polymers. Physical Properties of Polymers Handbook, 2nd Ed 2007: 715-722
V. Gauba and J. D. Hartgerink Self-Assembled heterotrimeric collagen triple helices directed through electrostatic interactions. J. Am. Chem. Soc., 129 2007: 2683-2690
H. Dong, S. E. Paramonov, L. Aulisa, E. L. Bakota and J. D. Hartgerink Self-assembly of Multi-domain Peptides: Balancing Molecular Frustration Controls Conformation and Nanostructure. J. Am. Chem. Soc., 129 2007: 12468-12472
V. Gauba and J. D. Hartgerink Surprisingly High Stability of Collagen ABC Heterotrimer: Evaluation of Side Chain Charge Pairs. J. Am. Chem. Soc., 10 2007
S. E. Paramonov, H-W. Jun, J. D. Hartgerink Self-assembly of peptide-amphiphile nanofibers: the roles of hydrogen bonding and amphiphilic packing. J. Am. Chem. Soc., 128 2006: 7219-7298