Colloidal dispersions of sterically and electrostatically stabilized PbS quantum dots: the effect of stabilization mechanism on structure factors, second virial coefficients, and film-forming properties

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Hauptverfasser: Jeong, Ahhyun, Portner, Josh, Tanner, Christian P. N., Ondry, Justin C., Zhou, Chenkun, Mi, Zehan, Tazoui, Youssef A., Wall, Vivian R. K., Ginsberg, Naomi S., Talapin, Dmitri V.
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Veröffentlicht: 2024
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author Jeong, Ahhyun
Portner, Josh
Tanner, Christian P. N.
Ondry, Justin C.
Zhou, Chenkun
Mi, Zehan
Tazoui, Youssef A.
Wall, Vivian R. K.
Ginsberg, Naomi S.
Talapin, Dmitri V.
author_facet Jeong, Ahhyun
Portner, Josh
Tanner, Christian P. N.
Ondry, Justin C.
Zhou, Chenkun
Mi, Zehan
Tazoui, Youssef A.
Wall, Vivian R. K.
Ginsberg, Naomi S.
Talapin, Dmitri V.
contents Electrostatically stabilized nanocrystals (NCs) and, in particular, quantum dots (QDs) hold promise for forming strongly coupled superlattices due to their compact and electronically conductive surface ligands. However, studies on the colloidal dispersion and interparticle interactions of electrostatically stabilized sub-10 nm NCs have been limited, hindering the optimization of colloidal stability and self-assembly. In this study, we employed small-angle X ray scattering (SAXS) experiments to investigate the interparticle interactions and arrangement of PbS QDs with thiostannate ligands (PbS-Sn2S64-) in polar solvents. The study reveals significant deviations from ideal solution behavior in electrostatically stabilized QD dispersions. Our results demonstrate that PbS-Sn2S64- QDs exhibit long-range interactions within the solvent, in contrast to the short-range steric repulsion characteristic of PbS QDs with oleate ligands (PbS-OA). Introducing highly charged multivalent electrolytes screens electrostatic interactions between charged QDs, reducing the length scale of the repulsive interactions. Furthermore, we calculate the second virial (B2) coefficients from SAXS data, providing insights into how surface chemistry, solvent, and size influence pair potentials. Finally, we explore the influence of long-range interparticle interactions of PbS-Sn2S64- QDs on the morphology of films produced by drying or spin-coating colloidal solutions. The long-range repulsive term of PbS-Sn2S64- QDs promotes the formation of amorphous films, and screening the electrostatic repulsion by addition of an electrolyte enables the formation of a crystalline film. These findings highlight the critical role of NC-NC interactions in tailoring the properties of functional nanomaterials.
format Preprint
id arxiv_https___arxiv_org_abs_2404_18915
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Colloidal dispersions of sterically and electrostatically stabilized PbS quantum dots: the effect of stabilization mechanism on structure factors, second virial coefficients, and film-forming properties
Jeong, Ahhyun
Portner, Josh
Tanner, Christian P. N.
Ondry, Justin C.
Zhou, Chenkun
Mi, Zehan
Tazoui, Youssef A.
Wall, Vivian R. K.
Ginsberg, Naomi S.
Talapin, Dmitri V.
Soft Condensed Matter
Materials Science
Electrostatically stabilized nanocrystals (NCs) and, in particular, quantum dots (QDs) hold promise for forming strongly coupled superlattices due to their compact and electronically conductive surface ligands. However, studies on the colloidal dispersion and interparticle interactions of electrostatically stabilized sub-10 nm NCs have been limited, hindering the optimization of colloidal stability and self-assembly. In this study, we employed small-angle X ray scattering (SAXS) experiments to investigate the interparticle interactions and arrangement of PbS QDs with thiostannate ligands (PbS-Sn2S64-) in polar solvents. The study reveals significant deviations from ideal solution behavior in electrostatically stabilized QD dispersions. Our results demonstrate that PbS-Sn2S64- QDs exhibit long-range interactions within the solvent, in contrast to the short-range steric repulsion characteristic of PbS QDs with oleate ligands (PbS-OA). Introducing highly charged multivalent electrolytes screens electrostatic interactions between charged QDs, reducing the length scale of the repulsive interactions. Furthermore, we calculate the second virial (B2) coefficients from SAXS data, providing insights into how surface chemistry, solvent, and size influence pair potentials. Finally, we explore the influence of long-range interparticle interactions of PbS-Sn2S64- QDs on the morphology of films produced by drying or spin-coating colloidal solutions. The long-range repulsive term of PbS-Sn2S64- QDs promotes the formation of amorphous films, and screening the electrostatic repulsion by addition of an electrolyte enables the formation of a crystalline film. These findings highlight the critical role of NC-NC interactions in tailoring the properties of functional nanomaterials.
title Colloidal dispersions of sterically and electrostatically stabilized PbS quantum dots: the effect of stabilization mechanism on structure factors, second virial coefficients, and film-forming properties
topic Soft Condensed Matter
Materials Science
url https://arxiv.org/abs/2404.18915