Nanoscale dynamics and aging of fibrous peptide-based gels

Dudukovic, Nikola A.; Zukoski, Charles F.

doi:10.1063/1.4899905

Nanoscale dynamics and aging of fibrous peptide-based gels

Journal Article · Tue Oct 28 00:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4899905· OSTI ID:1875822

Dudukovic, Nikola A. ^[1]; Zukoski, Charles F. ^[2]

Univ. of Illinois at Urbana-Champaign, IL (United States); University of Illinois
Univ. at Buffalo, NY (United States)

Solutions of the aromatic dipeptide derivative molecule fluorenylmethoxycarbonyl-diphenylalanine (Fmoc-FF) in dimethyl sulfoxide produce fibrous gels when mixed with water. We study the evolution of density fluctuations of this three-component system using X-ray photon correlation spectroscopy (XPCS) and compare these results to the macroscopic rheology of the gels and optical observations of the microstructure evolution. At the investigated scattering angles, the intensity autocorrelation functions do not follow behavior expected for simple diffusion of individual Fmoc-FF molecules localized within cages of nearest neighbors. Instead, the dynamics are associated with density fluctuations on length scales of ~10–100 nm arising from disaggregation and reformation of fibers, leading to an increasingly uniform network. This process is correlated with the growth of the elastic modulus, which saturates at long times. Autocorrelation functions and relaxation times acquired from XPCS measurements are consistent with relaxation rates of structures at dynamic equilibrium. Furthermore, this study provides further support to the concept of exploring peptide-based gelators as valence-limited patchy particles capable of forming equilibrium gels.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: FG02-07ER46471; AC02-06CH11357

OSTI ID:: 1875822

Alternate ID(s):: OSTI ID: 1224252
OSTI ID: 22310771
OSTI ID: 1163382

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 16 Vol. 141; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (37)

Nanostructured Hydrogels for Three-Dimensional Cell Culture Through Self-Assembly of Fluorenylmethoxycarbonyl–Dipeptides Jayawarna, V.; Ali, M.; Jowitt, T. A. Advanced Materials, Vol. 18, Issue 5 https://doi.org/10.1002/adma.200501522	journal	March 2006
Rigid, Self-Assembled Hydrogel Composed of a Modified Aromatic Dipeptide Mahler, A.; Reches, M.; Rechter, M. Advanced Materials, Vol. 18, Issue 11 https://doi.org/10.1002/adma.200501765	journal	June 2006
Fmoc-Diphenylalanine Self Assembles to a Hydrogel via a Novel Architecture Based on π–π Interlocked β-Sheets Smith, A. M.; Williams, R. J.; Tang, C. Advanced Materials, Vol. 20, Issue 1 https://doi.org/10.1002/adma.200701221	journal	January 2008
Use of a gel-forming dipeptide derivative as a carrier for antigen presentation Vegners, Rolands; Shestakova, Irina; Kalvinsh, Ivars Journal of Peptide Science, Vol. 1, Issue 6 https://doi.org/10.1002/psc.310010604	journal	November 1995
Anomalous dynamical light scattering in soft glassy gels Bouchaud, J. -P.; Pitard, E. The European Physical Journal E, Vol. 6, Issue 3 https://doi.org/10.1007/s101890170005	journal	November 2001
Introducing chemical functionality in Fmoc-peptide gels for cell culture Jayawarna, Vineetha; Richardson, Stephen M.; Hirst, Andrew R. Acta Biomaterialia, Vol. 5, Issue 3 https://doi.org/10.1016/j.actbio.2009.01.006	journal	March 2009
XPCS: Nanoscale motion and rheology Leheny, Robert L. Current Opinion in Colloid & Interface Science, Vol. 17, Issue 1 https://doi.org/10.1016/j.cocis.2011.11.002	journal	February 2012
Reversible gels of patchy particles Sciortino, Francesco; Zaccarelli, Emanuela Current Opinion in Solid State and Materials Science, Vol. 15, Issue 6 https://doi.org/10.1016/j.cossms.2011.07.003	journal	December 2011
Self-Assembled Fmoc-Peptides as a Platform for the Formation of Nanostructures and Hydrogels Orbach, Ron; Adler-Abramovich, Lihi; Zigerson, Sivan Biomacromolecules, Vol. 10, Issue 9 https://doi.org/10.1021/bm900584m	journal	September 2009
The Rheological and Structural Properties of Fmoc-Peptide-Based Hydrogels: The Effect of Aromatic Molecular Architecture on Self-Assembly and Physical Characteristics Orbach, Ron; Mironi-Harpaz, Iris; Adler-Abramovich, Lihi Langmuir, Vol. 28, Issue 4 https://doi.org/10.1021/la204426q	journal	December 2011
Mechanical Properties of Self-Assembled Fmoc-Diphenylalanine Molecular Gels Dudukovic, Nikola A.; Zukoski, Charles F. Langmuir, Vol. 30, Issue 15 https://doi.org/10.1021/la500589f	journal	April 2014
Fmoc-Diphenylalanine Self-Assembly Mechanism Induces Apparent p K _a Shifts Tang, Claire; Smith, Andrew M.; Collins, Richard F. Langmuir, Vol. 25, Issue 16 https://doi.org/10.1021/la900653q	journal	August 2009
Controlled Release from Modified Amino Acid Hydrogels Governed by Molecular Size or Network Dynamics Sutton, Sam; Campbell, Neil L.; Cooper, Andrew I. Langmuir, Vol. 25, Issue 17 https://doi.org/10.1021/la9011058	journal	September 2009
Dynamic Signatures of Microphase Separation in a Block Copolymer Melt Determined by X-ray Photon Correlation Spectroscopy and Rheology Patel, Amish J.; Mochrie, Simon; Narayanan, Suresh Macromolecules, Vol. 43, Issue 3 https://doi.org/10.1021/ma902343m	journal	February 2010
Fabrication of novel biomaterials through molecular self-assembly Zhang, Shuguang Nature Biotechnology, Vol. 21, Issue 10 https://doi.org/10.1038/nbt874	journal	September 2003
Universal non-diffusive slow dynamics in aging soft matter Cipelletti, Luca; Ramos, Laurence; Manley, S. Faraday Discussions, Vol. 123 https://doi.org/10.1039/b204495a	journal	September 2002
Peptide-based stimuli-responsive biomaterials Mart, Robert J.; Osborne, Rachel D.; Stevens, Molly M. Soft Matter, Vol. 2, Issue 10 https://doi.org/10.1039/b607706d	journal	January 2006
Designing peptide based nanomaterials Ulijn, Rein V.; Smith, Andrew M. Chemical Society Reviews, Vol. 37, Issue 4 https://doi.org/10.1039/b609047h	journal	January 2008
Relationship between molecular structure, gelation behaviour and gel properties of Fmoc-dipeptides Adams, Dave J.; Mullen, Leanne M.; Berta, Marco Soft Matter, Vol. 6, Issue 9 https://doi.org/10.1039/b921863g	journal	January 2010
Amino acid based smart hydrogel: formation, characterization and fluorescence properties of silver nanoclusters within the hydrogel matrix Roy, Subhasish; Banerjee, Arindam Soft Matter, Vol. 7, Issue 11 https://doi.org/10.1039/c1sm05034f	journal	January 2011
Tuneable mechanical properties in low molecular weight gels Chen, Lin; Raeburn, Jaclyn; Sutton, Sam Soft Matter, Vol. 7, Issue 20 https://doi.org/10.1039/c1sm05827d	journal	January 2011
Fmoc-diphenylalanine hydrogels: understanding the variability in reported mechanical properties Raeburn, Jaclyn; Pont, Guillaume; Chen, Lin Soft Matter, Vol. 8, Issue 4 https://doi.org/10.1039/c1sm06929b	journal	January 2012
Self-sustaining, fluorescent and semi-conducting co-assembled organogel of Fmoc protected phenylalanine with aromatic amines Bairi, Partha; Roy, Bappaditya; Routh, Parimal Soft Matter, Vol. 8, Issue 28 https://doi.org/10.1039/c2sm25673h	journal	January 2012
Polymer nanocomposites: polymer and particle dynamics Kim, Daniel; Srivastava, Samanvaya; Narayanan, Suresh Soft Matter, Vol. 8, Issue 42 https://doi.org/10.1039/c2sm26325d	journal	January 2012
Gel formation and aging in weakly attractive nanocolloid suspensions at intermediate concentrations Guo, Hongyu; Ramakrishnan, S.; Harden, James L. The Journal of Chemical Physics, Vol. 135, Issue 15 https://doi.org/10.1063/1.3653380	journal	October 2011
Colloidal gels: equilibrium and non-equilibrium routes Zaccarelli, Emanuela Journal of Physics: Condensed Matter, Vol. 19, Issue 32 https://doi.org/10.1088/0953-8984/19/32/323101	journal	July 2007
Connecting nanoscale motion and rheology of gel-forming colloidal suspensions Guo, Hongyu; Ramakrishnan, S.; Harden, James L. Physical Review E, Vol. 81, Issue 5 https://doi.org/10.1103/PhysRevE.81.050401	journal	May 2010
Nanoparticle Motion within Glassy Polymer Melts Guo, Hongyu; Bourret, Gilles; Corbierre, Muriel K. Physical Review Letters, Vol. 102, Issue 7 https://doi.org/10.1103/PhysRevLett.102.075702	journal	February 2009
Thermal Jamming of a Colloidal Glass Agarwal, Praveen; Srivastava, Samanvaya; Archer, Lynden A. Physical Review Letters, Vol. 107, Issue 26 https://doi.org/10.1103/PhysRevLett.107.268302	journal	December 2011
Crowded, Confined, and Frustrated: Dynamics of Molecules Tethered to Nanoparticles Agarwal, Praveen; Kim, Sung A.; Archer, Lynden A. Physical Review Letters, Vol. 109, Issue 25 https://doi.org/10.1103/PhysRevLett.109.258301	journal	December 2012
Structure and Transport Anomalies in Soft Colloids Srivastava, Samanvaya; Archer, Lynden A.; Narayanan, Suresh Physical Review Letters, Vol. 110, Issue 14 https://doi.org/10.1103/PhysRevLett.110.148302	journal	April 2013
Dynamics of Block Copolymer Micelles Revealed by X-Ray Intensity Fluctuation Spectroscopy Mochrie, S. G. J.; Mayes, A. M.; Sandy, A. R. Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1275	journal	February 1997
Universal Aging Features in the Restructuring of Fractal Colloidal Gels Cipelletti, Luca; Manley, S.; Ball, R. C. Physical Review Letters, Vol. 84, Issue 10 https://doi.org/10.1103/PhysRevLett.84.2275	journal	March 2000
Relationship between Structural and Stress Relaxation in a Block-Copolymer Melt Patel, Amish J.; Narayanan, Suresh; Sandy, Alec Physical Review Letters, Vol. 96, Issue 25 https://doi.org/10.1103/PhysRevLett.96.257801	journal	June 2006
Phase Diagram of Patchy Colloids: Towards Empty Liquids Bianchi, Emanuela; Largo, Julio; Tartaglia, Piero Physical Review Letters, Vol. 97, Issue 16 https://doi.org/10.1103/PhysRevLett.97.168301	journal	October 2006
Casting Metal Nanowires Within Discrete Self-Assembled Peptide Nanotubes Reches, M. Science, Vol. 300, Issue 5619 https://doi.org/10.1126/science.1082387	journal	April 2003
Evolution of dynamics and structure during formation of a cross-linked polymer gel Czakkel, O.; Madsen, A. EPL (Europhysics Letters), Vol. 95, Issue 2 https://doi.org/10.1209/0295-5075/95/28001	journal	June 2011

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