Mapping the energy landscapes of supramolecular assembly by thermal hysteresis

Robert W. Harkness V, Nicole Avakyan, Hanadi F. Sleiman and Anthony K. Mittermaier ()
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Robert W. Harkness V: McGill University
Nicole Avakyan: McGill University
Hanadi F. Sleiman: McGill University
Anthony K. Mittermaier: McGill University

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Understanding how biological macromolecules assemble into higher-order structures is critical to explaining their function in living organisms and engineered biomaterials. Transient, partly-structured intermediates are essential in many assembly processes and pathway selection, but are challenging to characterize. Here we present a simple thermal hysteresis method based on rapid, non-equilibrium melting and annealing measurements that maps the rate of supramolecular assembly as a function of temperature and concentration. A straightforward analysis of these surfaces provides detailed information on the natures of assembly pathways, offering temperature resolution beyond that accessible with conventional techniques. Validating the approach using a tetrameric guanine quadruplex, we obtain strikingly good agreement with previous kinetics measurements and reveal temperature-dependent changes to the assembly pathway. In an application to the recently discovered co-assembly of polydeoxyadenosine (poly(A)) and cyanuric acid, we show that fiber elongation is initiated when an unstable complex containing three poly(A) monomers acquires a fourth strand.

Date: 2018
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DOI: 10.1038/s41467-018-05502-z

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