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Three-dimensional femtosecond snapshots of isolated faceted nanostructures.

ABSTRACT: The structure and dynamics of isolated nanosamples in free flight can be directly visualized via single-shot coherent diffractive imaging using the intense and short pulses of x-ray free-electron lasers. Wide-angle scattering images encode three-dimensional (3D) morphological information of the samples, but its retrieval remains a challenge. Up to now, effective 3D morphology reconstructions from single shots were only achieved via fitting with highly constrained models, requiring a priori knowledge about possible geometries. Here, we present a much more generic imaging approach. Relying on a model that allows for any sample morphology described by a convex polyhedron, we reconstruct wide-angle diffraction patterns from individual silver nanoparticles. In addition to known structural motives with high symmetries, we retrieve imperfect shapes and agglomerates that were not previously accessible. Our results open unexplored routes toward true 3D structure determination of single nanoparticles and, ultimately, 3D movies of ultrafast nanoscale dynamics.

SUBMITTER: Colombo A

PROVIDER: S-EPMC9946342 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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Three-dimensional femtosecond snapshots of isolated faceted nanostructures.

Colombo Alessandro A Dold Simon S Kolb Patrice P Bernhardt Nils N Behrens Patrick P Correa Jonathan J Düsterer Stefan S Erk Benjamin B Hecht Linos L Heilrath Andrea A Irsig Robert R Iwe Norman N Jordan Jakob J Kruse Björn B Langbehn Bruno B Manschwetus Bastian B Martinez Franklin F Meiwes-Broer Karl-Heinz KH Oldenburg Kevin K Passow Christopher C Peltz Christian C Sauppe Mario M Seel Fabian F Tanyag Rico Mayro P RMP Treusch Rolf R Ulmer Anatoli A Walz Saida S Fennel Thomas T Barke Ingo I Möller Thomas T von Issendorff Bernd B Rupp Daniela D

Science advances 20230222 8

The structure and dynamics of isolated nanosamples in free flight can be directly visualized via single-shot coherent diffractive imaging using the intense and short pulses of x-ray free-electron lasers. Wide-angle scattering images encode three-dimensional (3D) morphological information of the samples, but its retrieval remains a challenge. Up to now, effective 3D morphology reconstructions from single shots were only achieved via fitting with highly constrained models, requiring a priori knowl ...[more]

PMID: 36812315

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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

Three-dimensional femtosecond snapshots of isolated faceted nanostructures.

Publications

Three-dimensional femtosecond snapshots of isolated faceted nanostructures.

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