TY - JOUR
T1 - Effects of Knot Tightness at the Molecular Level
AU - Zhang, Liang
AU - Lemonnier, Jean-Francois
AU - Acocella, Angela
AU - Calvaresi, Matteo
AU - Zerbetto, Francesco
AU - Leigh, David
N1 - Funding Information:
ACKNOWLEDGMENTS. We thank the China 1000 Talents Plan, East China Normal University, the Engineering and Physical Sciences Research Council (EP/P027067/1) and the European Research Council, Advanced Grant 339019 for funding, and the University of Manchester for a President’s Doctoral Scholar Award (to L.Z.). D.A.L. is a China 1000 Talents “Topnotch Talent” Professor and Royal Society Research Professor.
Publisher Copyright:
© National Academy of Sciences. All rights reserved.
Copyright:
Copyright 2019 Elsevier B.V., All rights reserved.
PY - 2019/1/25
Y1 - 2019/1/25
N2 - Three 819 knots in closed-loop strands of different lengths (approximately 20, 23 and 26 nm) were used to experimentally assess the consequences of knot tightness at the molecular level. Through the use of 1H nuclear magnetic resonance (NMR), diffusion ordered spectroscopy (DOSY), circular dichroism (CD), collision induced dissociation mass spectrometry (CID-MS) and molecular dynamics (MD) simulations on the different sized knots, we find that the structure, dynamics and reactivity of the molecular chains are dramatically affected by the tightness of the knotting. The tautness of entanglement causes differences in conformation, enhances the expression of topological chirality, weakens covalent bonds, inhibits decomplexation events and changes absorption properties. Understanding the effects of tightening nanoscale knots may usefully inform the design of knotted and entangled molecular materials.
AB - Three 819 knots in closed-loop strands of different lengths (approximately 20, 23 and 26 nm) were used to experimentally assess the consequences of knot tightness at the molecular level. Through the use of 1H nuclear magnetic resonance (NMR), diffusion ordered spectroscopy (DOSY), circular dichroism (CD), collision induced dissociation mass spectrometry (CID-MS) and molecular dynamics (MD) simulations on the different sized knots, we find that the structure, dynamics and reactivity of the molecular chains are dramatically affected by the tightness of the knotting. The tautness of entanglement causes differences in conformation, enhances the expression of topological chirality, weakens covalent bonds, inhibits decomplexation events and changes absorption properties. Understanding the effects of tightening nanoscale knots may usefully inform the design of knotted and entangled molecular materials.
U2 - 10.1073/pnas.1815570116
DO - 10.1073/pnas.1815570116
M3 - Article
C2 - 30683725
SN - 0027-8424
VL - 116
SP - 2452
EP - 2457
JO - Proceedings of the National Academy of Sciences
JF - Proceedings of the National Academy of Sciences
IS - 7
ER -