Observing and Controlling the Folding Pathway of DNA Origami at the Nanoscale

ACS Nano
Jonathan Lee Tin WahAndré Estevez-Torres

Abstract

DNA origami is a powerful method to fold DNA into rationally designed nanostructures that holds great promise for bionanotechnology. However, the folding mechanism has yet to be fully resolved, principally due to a lack of data with single molecule resolution. To address this issue, we have investigated in detail, using atomic force microscopy, the morphological evolution of hundreds of individual rectangular origamis in solution as a function of temperature. Significant structural changes were observed between 65 and 55 °C both for folding and melting, and six structural intermediates were identified. Under standard conditions, folding was initiated at the edges of the rectangle and progressed toward the center. Melting occurred through the reverse pathway until the structures were significantly disrupted but ended through a different pathway involving out-of-equilibrium chainlike structures. Increasing the relative concentration of center to edge staples dramatically modified the folding pathway to a mechanism progressing from the center toward the edges. These results indicate that the folding pathway is determined by thermodynamics and suggest a way of controlling it.

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Citations

Oct 4, 2019·Nanoscale·Eddie G Sanchez-RuedaArmando Hernandez-Garcia
Dec 22, 2019·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Taiki WatanabeShin-Ichiro M Nomura
Apr 30, 2020·Nucleic Acids Research·Jacob M MajikesJ Alexander Liddle
Dec 24, 2018·The Journal of Chemical Physics·Alexander CumberworthDaan Frenkel
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Dec 13, 2017·Nanotechnology·P Lourdu Xavier, Arun Richard Chandrasekaran
Dec 2, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Andreas JaekelBarbara Saccà
Feb 11, 2021·ACS Nano·Jacob M MajikesJ Alexander Liddle
Feb 23, 2021·Advanced Functional Materials·So Yeon AhnSoong Ho Um
May 14, 2021·Chemical Communications : Chem Comm·Joshua A JohnsonCarlos E Castro
Jun 13, 2017·Chemical Reviews·Fan HongHao Yan
Sep 14, 2017·ACS Nano·Deepak K AgrawalRebecca Schulman
Dec 15, 2020·Bioconjugate Chemistry·Willem E M NotebornThomas H Sharp
Feb 14, 2020·ACS Nano·Huan H CaoTao Ye

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