skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Super-resolution microscopy reveals structural diversity in molecular exchange among peptide amphiphile nanofibres

Abstract

The dynamic behaviour of supramolecular systems is an important dimension of their potential functions. Here, we report on the use of stochastic optical reconstruction microscopy to study the molecular exchange of peptide amphiphile nanofibres, supramolecular systems known to have important biomedical functions. Solutions of nanofibres labelled with different dyes (Cy3 and Cy5) were mixed, and the distribution of dyes inserting into initially single-colour nanofibres was quantified using correlative image analysis. Our observations are consistent with an exchange mechanism involving monomers or small clusters of molecules inserting randomly into a fibre. Different exchange rates are observed within the same fibre, suggesting that local cohesive structures exist on the basis of beta-sheet discontinuous domains. The results reported here show that peptide amphiphile supramolecular systems can be dynamic and that their intermolecular interactions affect exchange patterns. Lastly, this information can be used to generate useful aggregate morphologies for improved biomedical function.

Authors:
 [1];  [2]; ORCiD logo [3];  [4];  [2];  [4]
  1. Northwestern Univ., Evanston, IL (United States); Eindhoven Univ. of Technology, Eindhoven (The Netherlands); King's College London, London (United Kingdom)
  2. Eindhoven Univ. of Technology, Eindhoven (The Netherlands)
  3. Eindhoven Univ. of Technology, Eindhoven (The Netherlands); Institute for Bioengineering of Catalonia (IBEC), Barcelona (Spain)
  4. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Dutch Ministry of Education, Culture and Science (Gravity program); European Research Council (ERC); Marie Curie FP7-PEOPLE-IOF program
OSTI Identifier:
1261783
Alternate Identifier(s):
OSTI ID: 1820968
Grant/Contract Number:  
FG02-00ER45810
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 99 GENERAL AND MISCELLANEOUS; cells; multivalency; dynamics; medicine; vesicles; adhesion; systems; probes; biophysical chemistry; microscopy; structural biology; Biophysical chemistry Microscopy Structural biology

Citation Formats

da Silva, Ricardo M. P., van der Zwaag, Daan, Albertazzi, Lorenzo, Lee, Sungsoo S., Meijer, E. W., and Stupp, Samuel I.. Super-resolution microscopy reveals structural diversity in molecular exchange among peptide amphiphile nanofibres. United States: N. p., 2016. Web. https://doi.org/10.1038/ncomms11561.
da Silva, Ricardo M. P., van der Zwaag, Daan, Albertazzi, Lorenzo, Lee, Sungsoo S., Meijer, E. W., & Stupp, Samuel I.. Super-resolution microscopy reveals structural diversity in molecular exchange among peptide amphiphile nanofibres. United States. https://doi.org/10.1038/ncomms11561
da Silva, Ricardo M. P., van der Zwaag, Daan, Albertazzi, Lorenzo, Lee, Sungsoo S., Meijer, E. W., and Stupp, Samuel I.. Thu . "Super-resolution microscopy reveals structural diversity in molecular exchange among peptide amphiphile nanofibres". United States. https://doi.org/10.1038/ncomms11561. https://www.osti.gov/servlets/purl/1261783.
@article{osti_1261783,
title = {Super-resolution microscopy reveals structural diversity in molecular exchange among peptide amphiphile nanofibres},
author = {da Silva, Ricardo M. P. and van der Zwaag, Daan and Albertazzi, Lorenzo and Lee, Sungsoo S. and Meijer, E. W. and Stupp, Samuel I.},
abstractNote = {The dynamic behaviour of supramolecular systems is an important dimension of their potential functions. Here, we report on the use of stochastic optical reconstruction microscopy to study the molecular exchange of peptide amphiphile nanofibres, supramolecular systems known to have important biomedical functions. Solutions of nanofibres labelled with different dyes (Cy3 and Cy5) were mixed, and the distribution of dyes inserting into initially single-colour nanofibres was quantified using correlative image analysis. Our observations are consistent with an exchange mechanism involving monomers or small clusters of molecules inserting randomly into a fibre. Different exchange rates are observed within the same fibre, suggesting that local cohesive structures exist on the basis of beta-sheet discontinuous domains. The results reported here show that peptide amphiphile supramolecular systems can be dynamic and that their intermolecular interactions affect exchange patterns. Lastly, this information can be used to generate useful aggregate morphologies for improved biomedical function.},
doi = {10.1038/ncomms11561},
journal = {Nature Communications},
number = 1,
volume = 7,
place = {United States},
year = {2016},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Supramolecular Chemistry and Self-Assembly in Organic Materials Design
journal, September 2013

  • Stupp, Samuel I.; Palmer, Liam C.
  • Chemistry of Materials, Vol. 26, Issue 1
  • DOI: 10.1021/cm403028b

Correlation Functions Quantify Super-Resolution Images and Estimate Apparent Clustering Due to Over-Counting
journal, February 2012


The use of Nile Red to monitor the aggregation behavior in ternary surfactant-water-organic solvent systems
journal, January 2005

  • Stuart, Marc C. A.; van de Pas, John C.; Engberts, Jan B. F. N.
  • Journal of Physical Organic Chemistry, Vol. 18, Issue 9
  • DOI: 10.1002/poc.919

Cellular Motility Driven by Assembly and Disassembly of Actin Filaments
journal, February 2003


Control of Vesicular Trafficking by Rho GTPases
journal, September 2003


Cell death versus cell survival instructed by supramolecular cohesion of nanostructures
journal, February 2014

  • Newcomb, Christina J.; Sur, Shantanu; Ortony, Julia H.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4321

Control of Vesicular Trafficking by Rho GTPases
journal, May 2003


Control of Vesicular Trafficking by Rho GTPases
journal, May 2003


Consequences of chirality on the dynamics of a water-soluble supramolecular polymer
journal, February 2015

  • Baker, Matthew B.; Albertazzi, Lorenzo; Voets, Ilja K.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7234

Atomistic Molecular Dynamics Simulations of Peptide Amphiphile Self-Assembly into Cylindrical Nanofibers
journal, March 2011

  • Lee, One-Sun; Stupp, Samuel I.; Schatz, George C.
  • Journal of the American Chemical Society, Vol. 133, Issue 10
  • DOI: 10.1021/ja110966y

Antitumor Activity of Peptide Amphiphile Nanofiber-Encapsulated Camptothecin
journal, October 2011

  • Soukasene, Stephen; Toft, Daniel J.; Moyer, Tyson J.
  • ACS Nano, Vol. 5, Issue 11
  • DOI: 10.1021/nn203343z

High-Affinity Peptide-Based Collagen Targeting Using Synthetic Phage Mimics: From Phage Display to Dendrimer Display
journal, August 2009

  • Helms, Brett A.; Reulen, Sanne W. A.; Nijhuis, Sebastiaan
  • Journal of the American Chemical Society, Vol. 131, Issue 33
  • DOI: 10.1021/ja902285m

Supramolecular Nanofibers of Peptide Amphiphiles for Medicine
journal, August 2013

  • Webber, Matthew J.; Berns, Eric J.; Stupp, Samuel I.
  • Israel Journal of Chemistry, Vol. 53, Issue 8
  • DOI: 10.1002/ijch.201300046

Energy landscapes and functions of supramolecular systems
journal, January 2016

  • Tantakitti, Faifan; Boekhoven, Job; Wang, Xin
  • Nature Materials, Vol. 15, Issue 4
  • DOI: 10.1038/nmat4538

Equilibrium Chain Exchange Kinetics of Diblock Copolymer Micelles:  Tuning and Logarithmic Relaxation
journal, June 2006

  • Lund, Reidar; Willner, Lutz; Richter, Dieter
  • Macromolecules, Vol. 39, Issue 13
  • DOI: 10.1021/ma060328y

Sub-diffraction-limit imaging by stochastic optical reconstruction microscopy (STORM)
journal, August 2006

  • Rust, Michael J.; Bates, Mark; Zhuang, Xiaowei
  • Nature Methods, Vol. 3, Issue 10
  • DOI: 10.1038/nmeth929

Tunable Mechanics of Peptide Nanofiber Gels
journal, March 2010

  • Greenfield, Megan A.; Hoffman, Jessica R.; Olvera de la Cruz, Monica
  • Langmuir, Vol. 26, Issue 5
  • DOI: 10.1021/la9030969

Microspectroscopic imaging tracks the intracellular processing of a signal transduction protein: fluorescent-labeled protein kinase C beta I.
journal, August 1996

  • Bastiaens, P. I.; Jovin, T. M.
  • Proceedings of the National Academy of Sciences, Vol. 93, Issue 16
  • DOI: 10.1073/pnas.93.16.8407

Molecular Mechanisms Controlling Actin Filament Dynamics in Nonmuscle Cells
journal, June 2000

  • Pollard, Thomas D.; Blanchoin, Laurent; Mullins, R. Dyche
  • Annual Review of Biophysics and Biomolecular Structure, Vol. 29, Issue 1
  • DOI: 10.1146/annurev.biophys.29.1.545

Cellular Motility Driven by Assembly and Disassembly of Actin Filaments
journal, February 2003


Multicolor Super-Resolution Imaging with Photo-Switchable Fluorescent Probes
journal, September 2007


Selective Adhesion, Lipid Exchange and Membrane-Fusion Processes between Vesicles of Various Sizes Bearing Complementary Molecular Recognition Groups
journal, June 2001


Self-Assembly of Peptide−Amphiphile Nanofibers:  The Roles of Hydrogen Bonding and Amphiphilic Packing
journal, June 2006

  • Paramonov, Sergey E.; Jun, Ho-Wook; Hartgerink, Jeffrey D.
  • Journal of the American Chemical Society, Vol. 128, Issue 22
  • DOI: 10.1021/ja060573x

Selective Adhesion, Lipid Exchange and Membrane-Fusion Processes between Vesicles of Various Sizes Bearing Complementary Molecular Recognition Groups
journal, June 2001


The actin cytoskeleton in rapid steroid hormone actions: Actin Cytoskeleton and Steroid Hormones
journal, March 2014

  • Stournaras, Christos; Gravanis, Achilles; Margioris, Andrew N.
  • Cytoskeleton, Vol. 71, Issue 5
  • DOI: 10.1002/cm.21172

Cellular Motility Driven by Assembly and Disassembly of Actin Filaments
journal, May 2003


Super-resolution fluorescence imaging of organelles in live cells with photoswitchable membrane probes
journal, August 2012

  • Shim, S. -H.; Xia, C.; Zhong, G.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 35
  • DOI: 10.1073/pnas.1201882109

Probing Exchange Pathways in One-Dimensional Aggregates with Super-Resolution Microscopy
journal, May 2014


Tubulin post-translational modifications: encoding functions on the neuronal microtubule cytoskeleton
journal, August 2010


Shape-Dependent Targeting of Injured Blood Vessels by Peptide Amphiphile Supramolecular Nanostructures
journal, February 2015

  • Moyer, Tyson J.; Kassam, Hussein A.; Bahnson, Edward S. M.
  • Small, Vol. 11, Issue 23
  • DOI: 10.1002/smll.201403429

Actin Structure and Function
journal, June 2011


Super-Resolution Fluorescence Microscopy
journal, June 2009


Spatiotemporal control and superselectivity in supramolecular polymers using multivalency
journal, July 2013

  • Albertazzi, L.; Martinez-Veracoechea, F. J.; Leenders, C. M. A.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 30
  • DOI: 10.1073/pnas.1303109110

Equilibrium exchange kinetics in n-alkyl–PEO polymeric micelles: single exponential relaxation and chain length dependence
journal, January 2012

  • Zinn, Thomas; Willner, Lutz; Lund, Reidar
  • Soft Matter, Vol. 8, Issue 3
  • DOI: 10.1039/c1sm06809a

25th Anniversary Article: Supramolecular Materials for Regenerative Medicine
journal, February 2014


Multivalency as a Chemical Organization and Action Principle
journal, September 2012

  • Fasting, Carlo; Schalley, Christoph A.; Weber, Marcus
  • Angewandte Chemie International Edition, Vol. 51, Issue 42
  • DOI: 10.1002/anie.201201114

Lipid transfer between phosphatidylcholine vesicles and human erythrocytes: exponential decrease in rate with increasing acyl chain length
journal, June 1985

  • Ferrell, James E.; Lee, Kong Joo; Huestis, Wray H.
  • Biochemistry, Vol. 24, Issue 12
  • DOI: 10.1021/bi00333a007

Self-assembly for the synthesis of functional biomaterials
journal, February 2013


Pathway Selection in Peptide Amphiphile Assembly
journal, June 2014

  • Korevaar, Peter A.; Newcomb, Christina J.; Meijer, E. W.
  • Journal of the American Chemical Society, Vol. 136, Issue 24
  • DOI: 10.1021/ja503882s

Tuning Supramolecular Rigidity of Peptide Fibers through Molecular Structure
journal, May 2010

  • Pashuck, E. Thomas; Cui, Honggang; Stupp, Samuel I.
  • Journal of the American Chemical Society, Vol. 132, Issue 17
  • DOI: 10.1021/ja908560n

Conformational preferences of amino acids in globular proteins
journal, October 1978


Selective Differentiation of Neural Progenitor Cells by High-Epitope Density Nanofibers
journal, February 2004

  • Silva, Gabriel A.; Czeisler, Catherine; Niece, Krista L.
  • Science, Vol. 303, Issue 5662, p. 1352-1355
  • DOI: 10.1126/science.1093783

Supramolecular crafting of cell adhesion
journal, November 2007


Equilibrium exchange kinetics in n-alkyl–PEO polymeric micelles: single exponential relaxation and chain length dependence
journal, January 2012

  • Zinn, Thomas; Willner, Lutz; Lund, Reidar
  • Soft Matter, Vol. 8, Issue 3
  • DOI: 10.1039/C1SM06809A

    Works referencing / citing this record:

    Host Materials Transformable in Tumor Microenvironment for Homing Theranostics
    journal, February 2017


    Into the Dynamics of a Supramolecular Polymer at Submolecular Resolution
    journal, July 2017

    • Bochicchio, Davide; Salvalaglio, Matteo; Pavan, Giovanni M.
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/s41467-017-00189-0

    Reversible self-assembly of superstructured networks
    journal, October 2018


    Quantification of functional crosslinker reaction kinetics via super-resolution microscopy of swollen microgels
    journal, January 2019

    • Karanastasis, Apostolos A.; Kenath, Gopal S.; Sundararaman, Ravishankar
    • Soft Matter, Vol. 15, Issue 45
    • DOI: 10.1039/c9sm01618j

    A stochastic view on surface inhomogeneity of nanoparticles
    journal, April 2019


    Super-resolution Fluorescence Imaging for Materials Science
    journal, August 2017


    Quenched Stochastic Optical Reconstruction Microscopy (qSTORM) with Graphene Oxide
    journal, November 2018


    Quantifying Guest-Host Dynamics in Supramolecular Assemblies to Analyze Their Robustness
    journal, December 2018

    • Bastings, Maartje M. C.; Hermans, Thomas M.; Spiering, A. J. H.
    • Macromolecular Bioscience, Vol. 19, Issue 1
    • DOI: 10.1002/mabi.201800296

    Tuning the matrix metalloproteinase-1 degradability of peptide amphiphile nanofibers through supramolecular engineering
    journal, January 2019

    • Shi, Yejiao; Ferreira, Daniela S.; Banerjee, Jayati
    • Biomaterials Science, Vol. 7, Issue 12
    • DOI: 10.1039/c9bm00949c

    Designing stable, hierarchical peptide fibers from block co-polypeptide sequences
    journal, January 2019

    • van Rijt, Mark M. J.; Ciaffoni, Adriano; Ianiro, Alessandro
    • Chemical Science, Vol. 10, Issue 39
    • DOI: 10.1039/c9sc00800d

    Supramolecular materials based on AIE luminogens (AIEgens): construction and applications
    journal, January 2020

    • Li, Jie; Wang, Jianxing; Li, Haoxuan
    • Chemical Society Reviews, Vol. 49, Issue 4
    • DOI: 10.1039/c9cs00495e

    Molecular modelling of supramolecular polymers
    journal, January 2018


    Functional Control of Peptide Amphiphile Assemblies via Modulation of Internal Cohesion and Surface Chemistry Switch
    journal, August 2018

    • Lu, Sheng; Cui, Weijia; Li, Jason
    • Chemistry - A European Journal, Vol. 24, Issue 52
    • DOI: 10.1002/chem.201803026

    Supramolecular Copolymerization as a Strategy to Control the Stability of Self-Assembled Nanofibers
    journal, May 2018

    • Thota, Bala N. S.; Lou, Xianwen; Bochicchio, Davide
    • Angewandte Chemie, Vol. 130, Issue 23
    • DOI: 10.1002/ange.201802238

    Supramolecular Copolymerization as a Strategy to Control the Stability of Self-Assembled Nanofibers
    journal, May 2018

    • Thota, Bala N. S.; Lou, Xianwen; Bochicchio, Davide
    • Angewandte Chemie International Edition, Vol. 57, Issue 23
    • DOI: 10.1002/anie.201802238

    Controllable hierarchical self-assembly of porphyrin-derived supra-amphiphiles
    journal, March 2019


    Peptide supramolecular materials for therapeutics
    journal, January 2018

    • Sato, Kohei; Hendricks, Mark P.; Palmer, Liam C.
    • Chemical Society Reviews, Vol. 47, Issue 20
    • DOI: 10.1039/c7cs00735c