Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices

Ondry, Justin C.; Philbin, John P.; Lostica, Michael; Rabani, Eran; Alivisatos, A. Paul

doi:10.1021/acsnano.0c07202

Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices

Journal Article · Tue Dec 29 23:00:00 EST 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c07202· OSTI ID:1839253

^[1]; Philbin, John P. ^[2]; Lostica, Michael ^[3]; ^[4]; ^[5]

Univ. of California, Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Harvard Univ., Cambridge, MA (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel)
Univ. of California, Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

By combining colloidal nanocrystal synthesis, self-assembly, and solution phase epitaxial growth techniques, we developed a general method for preparing single dot thick atomically attached quantum dot (QD) superlattices with high-quality translational and crystallographic orientational order along with state-of-the-art uniformity in the attachment thickness. The procedure begins with colloidal synthesis of hexagonal prism shaped core/shell QDs (e.g., CdSe/CdS), followed by liquid subphase self-assembly and immobilization of superlattices on a substrate. Solution phase epitaxial growth of additional semiconductor material fills in the voids between the particles, resulting in a QD-in-matrix structure. The photoluminescence emission spectra of the QD-in-matrix structure retains characteristic 0D electronic confinement. Importantly, annealing of the resulting structures removes inhomogeneities in the QD–QD inorganic bridges, which our atomistic electronic structure calculations demonstrate would otherwise lead to Anderson-type localization. The piecewise nature of this procedure allows one to independently tune the size and material of the QD core, shell, QD–QD distance, and the matrix material. These four choices can be tuned to control many properties (degree of quantum confinement, quantum coupling, band alignments, etc.) depending on the specific applications. Lastly, cation exchange reactions can be performed on the final QD-in-matrix, as demonstrated herein with a CdSe/CdS to HgSe/HgS conversion.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1839253

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 2 Vol. 15; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited By (3)

Course materials and datasets for the Alivisatos group-based undergraduate research program Calvin, Jason; Ondry, Justin; Dahl, Jakob Zenodo https://doi.org/10.5281/zenodo.5555924	other	January 2021
Course materials and datasets for the Alivisatos group-based undergraduate research program Calvin, Jason; Ondry, Justin; Dahl, Jakob Zenodo https://doi.org/10.5281/zenodo.5672504	other	January 2021
Course materials and datasets for the Alivisatos group-based undergraduate research program Calvin, Jason; Ondry, Justin; Dahl, Jakob Dryad https://doi.org/10.6078/d1hd9g	dataset	January 2021

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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lattices
nanocrystal superlattices
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oriented attachment
physical and chemical processes
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self-assembly
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Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices

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