Shape-induced crystallization of binary DNA-functionalized nanocubes

Yunhan Zhang*, Giuliana Giunta, Haojun Liang, Marjolein Dijkstra*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Leveraging the anisotropic shape of DNA-functionalized nanoparticles holds potential for shape-directed crystallization of a wide collection of superlattice structures. Using coarse-grained molecular dynamics simulations, we study the self-assembly of a binary mixture of cubic gold nanoparticles, which are functionalized by complementary DNA strands. We observe the spontaneous self-assembly of simple cubic (SC), plastic body-centered tetragonal (pBCT), and compositionally disordered plastic body-centered tetragonal (d-pBCT) phases due to hybridization of the DNA strands. We systematically investigate the effect of length, grafting density, as well as rigidity of the DNA strands on the self-assembly behavior of cubic nanoparticles. We measure the potential of mean force between DNA-functionalized nanocubes for varying rigidity of the DNA strands and DNA lengths. Using free-energy calculations, we find that longer and flexible DNA strands can lead to a phase transformation from SC to the pBCT phase due to a gain in entropy arising from the orientational degrees of freedom of the nanocubes in the pBCT phase. Our results may serve as a guide for self-assembly experiments on DNA-functionalized cubic nanoparticles.

Original languageEnglish
Article number184902
Number of pages15
JournalJournal of Chemical Physics
Volume158
Issue number18
DOIs
Publication statusPublished - 14 May 2023

Bibliographical note

Funding Information:
We thank Tor Sewring and Edwin A. Bedolla Montiel for useful discussions. We are grateful for the financial support from the Chinese Scholarship Council (CSC) and the Program of the National Natural Science Foundation of China (Grant No. 21991132, 22073090). In additional we acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. ERC-2019-ADG 884902, SoftML).

Publisher Copyright:
© 2023 Author(s).

Funding

We thank Tor Sewring and Edwin A. Bedolla Montiel for useful discussions. We are grateful for the financial support from the Chinese Scholarship Council (CSC) and the Program of the National Natural Science Foundation of China (Grant No. 21991132, 22073090). In additional we acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. ERC-2019-ADG 884902, SoftML).

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