Dendrimer Ligand Directed Nanoplate Assembly

Journal Article · 22 November 2019 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.9b07348 · OSTI ID:1599291

Elbert, Katherine C.  ^[1]; Vo, Thi ^[2]; Krook, Nadia M.  ^[1]; Zygmunt, William ^[2]; Park, Jungmi ^[1]; Yager, Kevin G.  ^[3]; Composto, Russell J.  ^[1]; Glotzer, Sharon C. ^[2]; Murray, Christopher B. ^[1]

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1. Univ. of Pennsylvania, Philadelphia, PA (United States)
2. Univ. of Michigan, Ann Arbor, MI (United States)
3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Many studies on nanocrystal (NC) self-assembly into ordered superlattices have focused mainly on attractive forces between the NCs, whereas the role of organic ligands on anisotropic NCs is only in its infancy. Herein, we report the use of a series of dendrimer ligands to direct the assembly of nanoplates into 2D and 3D geometries. It was found that the dendrimer-nanoplates consistently form a directionally offset architecture in 3D films. We present a theory to predict ligand surface distribution and Monte Carlo simulation results that characterize the ligand shell around the nanoplates. Bulky dendrimer ligands create a nontrivial corona around the plates that changes with ligand architecture. When this organic–inorganic effective shape is used in conjunction with thermodynamic perturbation theory to predict both lattice morphology and equilibrium relative orientations between NCs, a lock-and-key type of mechanism is found for the 3D assembly. We observe excellent agreement between our experimental results and theoretical model for 2D and 3D geometries, including the percent of offset between the layers of NCs. Furthermore, such level of theoretical understanding and modeling will help guide future design frameworks to achieve targeted assemblies of NCs

• Research Organization: Brookhaven National Laboratory (BNL), Upton, NY (United States)
• Sponsoring Organization: National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
• Grant/Contract Number: SC0012704
• OSTI ID: 1599291
• Report Number(s): BNL--213620-2020-JAAM
• Journal Information: ACS Nano, Journal Name: ACS Nano Journal Issue: 12 Vol. 13; ISSN 1936-0851
• Publisher: American Chemical Society (ACS)Copyright Statement
• Country of Publication: United States
• Language: English