Self-assembly pathways and polymorphism in peptide-based nanostructures

Nanoscale
Nikola A DudukovicCharles F Zukoski

Abstract

Dipeptide derivative molecules can self-assemble into space-filling nanofiber networks at low volume fractions (<1%), allowing the formation of molecular gels with tunable mechanical properties. The self-assembly of dipeptide-based molecules is reminiscent of pathological amyloid fibril formation by naturally occurring polypeptides. Fluorenylmethoxycarbonyl-diphenylalanine (Fmoc-FF) is the most widely studied such molecule, but the thermodynamic and kinetic phenomena giving rise to Fmoc-FF gel formation remain poorly understood. We have previously presented evidence that the gelation process is a first order phase transition characterized by low energy barriers to nucleation, short induction times, and rapid quasi-one-dimensional crystal growth, stemming from solvent-solute interactions and highly specific molecular packing. Here, we discuss the phase behavior of Fmoc-FF in different solvents. We find that Fmoc-FF gel formation can be induced in apolar solvents, in addition to previously established pathways in aqueous systems. We further show that in certain solvent systems anisotropic crystals (nanofibers) are an initial metastable state, after which macroscopic crystal aggregates with no preferred axis of growth are formed. ...Continue Reading

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Citations

Apr 27, 2018·Chemical Society Reviews·Danielle M Raymond, Bradley L Nilsson
Feb 6, 2019·Nanoscale·Ana M Fuentes-CaparrósDave J Adams
Sep 4, 2019·Angewandte Chemie·Tom GutermanEhud Gazit
Jun 10, 2020·Nanoscale·Santanu PanjaDave J Adams
Jan 12, 2020·Materials Science & Engineering. C, Materials for Biological Applications·Rashmi Jain, Sangita Roy
Jan 10, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Enric Mayans, Carlos Alemán
Oct 3, 2018·The Journal of Physical Chemistry Letters·Takeshi YamamotoShuichi Hiraoka

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Methods Mentioned

BETA
biosensing
NMR
Confocal microscopy

Software Mentioned

MATLAB

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