Programming crystallization kinetics of self- assembled DNA crystals with 5-methylcytosine modification

• 成果类型: Article
• 署名作者: Chen, Jielin; Dai, Zheze; Lv, Hui; Jin, Zhongchao; Tang, Yuqing; Xie, Xiaodong; Shi, Jiye; Wang, Fei; Li, Qian; Liu, Xiaoguo; Fan, Chunhai
• 署名单位: Shanghai Jiao Tong University; Shanghai Jiao Tong University; Zhangjiang Laboratory; Chinese Academy of Sciences; Shanghai Institute of Applied Physics, CAS
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-15412
• DOI: 10.1073/pnas.2312596121
• 发表日期: 2024-03-12
• 关键词: methylation; stacking; DESIGN

摘要

Self- assembled DNA crystals offer a precise chemical platform at the angstrom-scale for DNA nanotechnology, holding enormous potential in material separation, catalysis, and DNA data storage. However, accurately controlling the crystallization kinetics of such DNA crystals remains challenging. Herein, we found that atomiclevel 5- methylcytosine (5mC) modification can regulate the crystallization kinetics of DNA crystal by tuning the hybridization rates of DNA motifs. We discovered that by manipulating the axial and combination of 5mC modification on the sticky ends of DNA tensegrity triangle motifs, we can obtain a series of DNA crystals with controllable morphological features. Through DNA - PAINT and FRET- labeled DNA strand displacement experiments, we elucidate that atomiclevel 5mC modification enhances the affinity constant of DNA hybridization at both the single- molecule and macroscopic scales. This enhancement can be harnessed for kinetic- driven control of the preferential growth direction of DNA crystals. The 5mC modification strategy can overcome the limitations of DNA sequence design imposed by limited nucleobase numbers in various DNA hybridization reactions. This strategy provides a new avenue for the manipulation of DNA crystal structure, valuable for the advancement of DNA and biomacromolecular crystallography.