Covalently Linked, Two-Dimensional Quantum Dot Assemblies

Ritchhart, Andrew; Monahan, Madison; Mars, Julian; Toney, Michael F.; De Yoreo, James J.; Cossairt, Brandi M.

doi:10.1021/acs.langmuir.0c01668

Covalently Linked, Two-Dimensional Quantum Dot Assemblies

Journal Article · Wed Jul 29 00:00:00 EDT 2020 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.0c01668· OSTI ID:1781113

Ritchhart, Andrew ^[1]; Monahan, Madison ^[2]; Mars, Julian ^[3]; ^[3]; ^[4]; ^[2]

Univ. of Washington, Seattle, WA (United States); University of Washington
Univ. of Washington, Seattle, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of Washington, Seattle, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Using nanoscale building blocks to construct hierarchical materials is a radical new branch point in materials discovery that promises new structures and emergent functionality. Understanding the design principles that govern nanoparticle assembly is critical to moving this field forward. By exploiting mixed ligand environments to target patchy nanoparticle surfaces, we have demonstrated a novel method of colloidal quantum dot (QD) assembly that gives rise to 2D structures. The equilibration of solutions of spherical and quasispherical QDs, including CdS, CdSe, and InP, with 2,2'-bipyridine-5,5'-diacrylic acid resulted in the preferential formation of 2D assemblies over the course of days as determined by transmission electron microscopy analysis. Small-angle X-ray scattering confirms the existence of the QD assemblies in solution. The dependence of the assembly on linker properties (length and rigidity), linker concentration, and total concentration was investigated, together with the data point to a mechanism involving ligand redistribution to create a patchy surface that maximizes the steric repulsion of neighboring QDs. By operating in an underexchanged regime, the arising patchiness results in enthalpically preferred directions of cross-linking that can be accessed by thermal equilibration.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Washington, Seattle, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); European Union (EU)

Grant/Contract Number:: SC0019288; AC02-76SF00515

OSTI ID:: 1781113

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 33 Vol. 36; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Covalently Linked, Two-Dimensional Quantum Dot Assemblies

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