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Nat Commun. 2014 Dec 16;5:5793. doi: 10.1038/ncomms6793.

A dynamic supramolecular polymer with stimuli-responsive handedness for in situ probing of enzymatic ATP hydrolysis.

Author information

1
New Chemistry Unit, Supramolecular Chemistry Laboratory, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Bangalore 560064, India.
2
Laboratory for Chemistry of Novel Materials, Center for Innovation and Research in Materials and Polymers, University of Mons-UMONS, 20, Place du Parc, Mons B-7000, Belgium.

Abstract

Design of artificial systems, which can respond to fluctuations in concentration of adenosine phosphates (APs), can be useful in understanding various biological processes. Helical assemblies of chromophores, which dynamically respond to such changes, can provide real-time chiroptical readout of various chemical transformations. Towards this concept, here we present a supramolecular helix of achiral chromophores, which shows chiral APs responsive tunable handedness along with dynamically switchable helicity. This system, composing of naphthalenediimides with phosphate recognition unit, shows opposite handedness on binding with ATP compared with ADP or AMP, which is comprehensively analysed with molecular dynamic simulations. Such differential signalling along with stimuli-dependent fast stereomutations have been capitalized to probe the reaction kinetics of enzymatic ATP hydrolysis. Detailed chiroptical analyses provide mechanistic insights into the enzymatic hydrolysis and various intermediate steps. Thus, a unique dynamic helical assembly to monitor the real-time reaction processes via its stimuli-responsive chiroptical signalling is conceptualized.

PMID:
25511998
DOI:
10.1038/ncomms6793
[Indexed for MEDLINE]

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