3D Columnar Phase of Stacked Short DNA Organized by Coherent Membrane Undulations

Nathan F. Bouxsein, Cecília Leal, Christopher S. McAllister, Youli Li, Kai K. Ewert, Charles E. Samuel, Cyrus R. Safinya

Research output: Contribution to journalArticle

Abstract

We report on the discovery of a new organized lipid-nucleic acid phase upon intercalation of blunt duplexes of short DNA (sDNA) within cationic multilayer fluid membranes. End-to-end interactions between sDNA leads to columnar stacks. At high membrane charge density, with the inter-sDNA column spacing (dsDNA) comparable but larger than the diameter of sDNA, a 2D columnar phase (i.e., a 2D smectic) is found similar to the phase in cationic liposome-DNA complexes with long lambda-phage DNA. Remarkably, with increasing dsDNA as the membrane charge density is lowered, a transition is observed to a 3D columnar phase of stacked sDNA. This occurs even though direct DNA-DNA electrostatic interactions across layers are screened by diffusing cationic lipids near the phosphate groups of sDNA. Softening of the membrane bending rigidity (κ), which further promotes membrane undulations, significantly enhances the 3D columnar phase. These observations are consistent with a model by Schiessel and Aranda-Espinoza where local membrane undulations, due to electrostatically induced membrane wrapping around sDNA columns, phase lock from layer-to-layer, thereby precipitating coherent "crystal-like" undulations coupled to sDNA columns with long-range position and orientation order. The finding that this new phase is stable at large dsDNA and enhanced with decreasing κ is further supportive of the model where the elastic cost of membrane deformation per unit area around sDNA columns (∈ κh2/dsDNA 4, h2 = sum of square of amplitudes of the inner and outer monolayer undulations) is strongly reduced relative to the favorable electrostatic attractions of partially wrapped membrane around sDNA columns. The findings have broad implications in the design of membrane-mediated assembly of functional nanoparticles in 3D.

Original languageEnglish (US)
Pages (from-to)11891-11901
Number of pages11
JournalLangmuir
Volume35
Issue number36
DOIs
StatePublished - Sep 10 2019

    Fingerprint

ASJC Scopus subject areas

  • Materials Science(all)
  • Condensed Matter Physics
  • Surfaces and Interfaces
  • Spectroscopy
  • Electrochemistry

Cite this

Bouxsein, N. F., Leal, C., McAllister, C. S., Li, Y., Ewert, K. K., Samuel, C. E., & Safinya, C. R. (2019). 3D Columnar Phase of Stacked Short DNA Organized by Coherent Membrane Undulations. Langmuir, 35(36), 11891-11901. https://doi.org/10.1021/acs.langmuir.9b01726