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Epitaxy: Programmable Atom Equivalents Versus Atoms

Wang, Mary X. and Seo, Soyoung E. and Gabrys, Paul A. and Fleischman, Dagny and Lee, Byeongdu and Kim, Youngeun and Atwater, Harry A. and Macfarlane, Robert J. and Mirkin, Chad A. (2017) Epitaxy: Programmable Atom Equivalents Versus Atoms. ACS Nano, 11 (1). pp. 180-185. ISSN 1936-0851. doi:10.1021/acsnano.6b06584.

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The programmability of DNA makes it an attractive structure-directing ligand for the assembly of nanoparticle (NP) superlattices in a manner that mimics many aspects of atomic crystallization. However, the synthesis of multilayer single crystals of defined size remains a challenge. Though previous studies considered lattice mismatch as the major limiting factor for multilayer assembly, thin film growth depends on many interlinked variables. Here, a more comprehensive approach is taken to study fundamental elements, such as the growth temperature and the thermodynamics of interfacial energetics, to achieve epitaxial growth of NP thin films. Both surface morphology and internal thin film structure are examined to provide an understanding of particle attachment and reorganization during growth. Under equilibrium conditions, single crystalline, multilayer thin films can be synthesized over 500 × 500 μm2 areas on lithographically patterned templates, whereas deposition under kinetic conditions leads to the rapid growth of glassy films. Importantly, these superlattices follow the same patterns of crystal growth demonstrated in atomic thin film deposition, allowing these processes to be understood in the context of well-studied atomic epitaxy and enabling a nanoscale model to study fundamental crystallization processes. Through understanding the role of epitaxy as a driving force for NP assembly, we are able to realize 3D architectures of arbitrary domain geometry and size.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Lee, Byeongdu0000-0003-2514-8805
Kim, Youngeun0000-0002-5936-6520
Atwater, Harry A.0000-0001-9435-0201
Mirkin, Chad A.0000-0002-6634-7627
Additional Information:© 2016 American Chemical Society. ACS AuthorChoice - This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. Received: September 29, 2016; Accepted: November 23, 2016; Publication Date (Web): December 5, 2016. This work was supported by the following awards: AFOSR FA9550-11-1-0275 and FA9550-12-1-0280; the Department of Defense National Security Science and Engineering Faculty Fellowship N00014-15-1-0043; and the Center for Bio-Inspired Energy Science (CBES), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences under award DE-SC0000989-0002. This work was also supported by the National Science Foundation’s (NSF) MRSEC program (DMR-1121262) and made use of its Shared Facilities at the Materials Research Center of Northwestern University, specifically the EPIC facility of the NUANCE Center, which also receives support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205). X-ray experiments were carried out at beamline 12-ID-B at the Advanced Photon Source (APS), a U.S. DOE Office of Science User Facility operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. EBL was performed at the Kavli Nanoscience Institute’s shared instrumentation center. FIB-SEM was performed at the Shared Experimental Facilities supported in part by the MRSEC Program of the NSF (DMR-1419807). M.X.W. acknowledges support from the National Science Foundation Graduate Research Fellowship, a Ryan Fellowship, and the Northwestern University International Institute for Nanotechnology. S.E.S. acknowledges support from the Center for Bio-Inspired Energy Sciences Fellowship and the Northwestern University International Institute for Nanotechnology. Y.K. acknowledges support from a Ryan Fellowship and the Northwestern University International Institute for Nanotechnology. M.X.W. and S.E.S. contributed equally. The authors declare no competing financial interest.
Group:Kavli Nanoscience Institute
Funding AgencyGrant Number
Air Force Office of Scientific Research (AFOSR)FA9550-11-1-0275
Air Force Office of Scientific Research (AFOSR)FA9550-12-1-0280
National Security Science and Engineering Faculty FellowshipN00014-15-1-0043
Department of Energy (DOE)DE-SC0000989-0002
Department of Energy (DOE)DE-AC02-06CH11357
NSF Graduate Research FellowshipUNSPECIFIED
Ryan FellowshipUNSPECIFIED
Northwestern UniversityUNSPECIFIED
Subject Keywords:DNA, epitaxy, nanoparticles, self-assembly, thin film
Issue or Number:1
Record Number:CaltechAUTHORS:20161206-142155188
Persistent URL:
Official Citation:Epitaxy: Programmable Atom Equivalents Versus Atoms Mary X. Wang, Soyoung E. Seo, Paul A. Gabrys, Dagny Fleischman, Byeongdu Lee, Youngeun Kim, Harry A. Atwater, Robert J. Macfarlane, and Chad A. Mirkin ACS Nano 2017 11 (1), 180-185 DOI: 10.1021/acsnano.6b06584
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:72602
Deposited By: Tony Diaz
Deposited On:06 Dec 2016 22:51
Last Modified:11 Nov 2021 05:04

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