Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 113, Issue 38, Pages 10485-10490Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1611808113
Keywords
nanomaterials; anisotropic nanoparticles; colloidal crystallization; DNA; broken symmetry
Categories
Funding
- Air Force Office of Scientific Research Multidisciplinary University Research Initiative [FA9550-11-1-0275]
- National Science Foundation (NSF) Materials Research Science and Engineering Center (MRSEC) program at the Materials Research Center of Northwestern University (NU) [DMR-1121262]
- Non-equilibrium Energy Research Center, an Energy Frontier Research Center - Department of Energy (DoE), Office of Science, and Office of Basic Energy Sciences [DE-SC0000989]
- National Science Foundation Graduate Research Fellowship
- Natural Sciences and Engineering Research Council of Canada [PGS-D 6799-459278-2014]
- China Scholarship Council [201306310060]
- International Institute of Nanotechnology
- DoE [DE-AC02-06CH11357]
- MRSEC program (NSF Grant) at the Materials Research Center [DMR-1121262]
- International Institute for Nanotechnology (IIN)
- State of Illinois, through the IIN
- NU Office for Research
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In this work, we present a joint experimental and molecular dynamics simulations effort to understand and map the crystallization behavior of polyhedral nanoparticles assembled via the interaction of DNA surface ligands. In these systems, we systematically investigated the interplay between the effects of particle core (via the particle symmetry and particle size) and ligands (via the ligand length) on crystallization behavior. This investigation revealed rich phase diagrams, previously unobserved phase transitions in polyhedral crystallization behavior, and an unexpected symmetry breaking in the ligand distribution on a particle surface. To understand these results, we introduce the concept of a zone of anisotropy, or the portion of the phase space where the anisotropy of the particle is preserved in the crystallization behavior. Through comparison of the zone of anisotropy for each particle we develop a foundational roadmap to guide future investigations.
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