Dataset Information

Complex three-dimensional self-assembly in proxies for atmospheric aerosols.

ABSTRACT: Aerosols are significant to the Earth's climate, with nearly all atmospheric aerosols containing organic compounds that often contain both hydrophilic and hydrophobic parts. However, the nature of how these compounds are arranged within an aerosol droplet remains unknown. Here we demonstrate that fatty acids in proxies for atmospheric aerosols self-assemble into highly ordered three-dimensional nanostructures that may have implications for environmentally important processes. Acoustically trapped droplets of oleic acid/sodium oleate mixtures in sodium chloride solution are analysed by simultaneous synchrotron small-angle X-ray scattering and Raman spectroscopy in a controlled gas-phase environment. We demonstrate that the droplets contained crystal-like lyotropic phases including hexagonal and cubic close-packed arrangements of spherical and cylindrical micelles, and stacks of bilayers, whose structures responded to atmospherically relevant humidity changes and chemical reactions. Further experiments show that self-assembly reduces the rate of the reaction of the fatty acid with ozone, and that lyotropic-phase formation also occurs in more complex mixtures more closely resembling compositions of atmospheric aerosols. We suggest that lyotropic-phase formation likely occurs in the atmosphere, with potential implications for radiative forcing, residence times and other aerosol characteristics.

SUBMITTER: Pfrang C

PROVIDER: S-EPMC5701067 | biostudies-literature | 2017 Nov

REPOSITORIES: biostudies-literature

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Complex three-dimensional self-assembly in proxies for atmospheric aerosols.

Pfrang C C Rastogi K K Cabrera-Martinez E R ER Seddon A M AM Dicko C C Labrador A A Plivelic T S TS Cowieson N N Squires A M AM

Nature communications 20171123 1

Aerosols are significant to the Earth's climate, with nearly all atmospheric aerosols containing organic compounds that often contain both hydrophilic and hydrophobic parts. However, the nature of how these compounds are arranged within an aerosol droplet remains unknown. Here we demonstrate that fatty acids in proxies for atmospheric aerosols self-assemble into highly ordered three-dimensional nanostructures that may have implications for environmentally important processes. Acoustically trappe ...[more]

PMID: 29170428

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Project description:Nucleic acids (DNA and RNA) are widely used to construct nanometre-scale structures with ever increasing complexity, with possible application in fields such as structural biology, biophysics, synthetic biology and photonics. The nanostructures are formed through one-pot self-assembly, with early kilodalton-scale examples containing typically tens of unique DNA strands. The introduction of DNA origami, which uses many staple strands to fold one long scaffold strand into a desired structure, has provided access to megadalton-scale nanostructures that contain hundreds of unique DNA strands. Even larger DNA origami structures are possible, but manufacturing and manipulating an increasingly long scaffold strand remains a challenge. An alternative and more readily scalable approach involves the assembly of DNA bricks, which each consist of four short binding domains arranged so that the bricks can interlock. This approach does not require a scaffold; instead, the short DNA brick strands self-assemble according to specific inter-brick interactions. First-generation bricks used to create three-dimensional structures are 32 nucleotides long, consisting of four eight-nucleotide binding domains. Protocols have been designed to direct the assembly of hundreds of distinct bricks into well formed structures, but attempts to create larger structures have encountered practical challenges and had limited success. Here we show that DNA bricks with longer, 13-nucleotide binding domains make it possible to self-assemble 0.1-1-gigadalton, three-dimensional nanostructures from tens of thousands of unique components, including a 0.5-gigadalton cuboid containing about 30,000 unique bricks and a 1-gigadalton rotationally symmetric tetramer. We also assembled a cuboid that contains around 10,000 bricks and about 20,000 uniquely addressable, 13-base-pair 'voxels' that serves as a molecular canvas for three-dimensional sculpting. Complex, user-prescribed, three-dimensional cavities can be produced within this molecular canvas, enabling the creation of shapes such as letters, a helicoid and a teddy bear. We anticipate that with further optimization of structure design, strand synthesis and assembly procedure even larger structures could be accessible, which could be useful for applications such as positioning functional components.

Dataset Information

Complex three-dimensional self-assembly in proxies for atmospheric aerosols.

Publications

Complex three-dimensional self-assembly in proxies for atmospheric aerosols.

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