Abstract
A large variety of functional self-assembled supramolecular nanostructures have been reported over recent decades. The experimental approach to these systems initially focused on the design of molecules with specific interactions that lead to discrete geometric structures, and more recently on the kinetics and mechanistic pathways of self-assembly. However, there remains a major gap in our understanding of the internal conformational dynamics of these systems and of the links between their dynamics and function. Molecular dynamics simulations have yielded information on the molecular fluctuations of supramolecular assemblies, yet experimentally it has been difficult to obtain analogous data with subnanometre spatial resolution. Using site-directed spin labelling and electron paramagnetic resonance spectroscopy, we measured the conformational dynamics of a self-assembled nanofibre in water through its 6.7 nm cross-section. Our measurements provide unique insight for the design of supramolecular functional materials.
Original language | English (US) |
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Pages (from-to) | 812-816 |
Number of pages | 5 |
Journal | Nature materials |
Volume | 13 |
Issue number | 8 |
DOIs | |
State | Published - Aug 2014 |
Funding
This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the US Department of Energy under Award # DE-FG02-00ER45810. J.B.M. acknowledges a postdoctoral fellowship through the National Institutes of Health National Research Service Award # 1F32AR06195501. J.H.O. acknowledges an IBNAM-Baxter early career award. EPR experiments were carried out at The Medical College of Wisconsin, National Biomedical EPR Center, supported by National Institutes of Health Grant P41 EB001980, and also at Northwestern University under support of the National Heart, Lung and Blood Institute of the National Institutes of Health (NIH-HL-13531). X-ray diffraction experiments were carried out at beamline 5ID-D of the Advanced Photon Source at Argonne National Laboratory. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work also made use of Northwestern University’s Biological Imaging Facility (BIF) for electron microscopy and the Integrated Molecular Structure Education and Research Center (IMSERC) for mass spectrometry and FTIR spectroscopy. The authors acknowledge S. Han for helpful discussions and M. Seniw for illustrations.
ASJC Scopus subject areas
- General Chemistry
- General Materials Science
- Condensed Matter Physics
- Mechanics of Materials
- Mechanical Engineering