Shape Control of Colloidal Semiconductor Nanocrystals through Thermodynamically Driven Aggregative Growth

Cassidy, James; Harankahage, Dulanjan; Ojile, Jack; Porotnikov, Dmitry; Walker, Lexie; Montemurri, Michael; Narvaez, Bianca L.; Khon, Dmitriy; Forbes, Malcolm D. E.; Zamkov, Mikhail

doi:10.1021/acs.chemmater.2c00265

Shape Control of Colloidal Semiconductor Nanocrystals through Thermodynamically Driven Aggregative Growth

Journal Article · Wed Feb 16 23:00:00 EST 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c00265· OSTI ID:1865406

Cassidy, James ^[1]; Harankahage, Dulanjan ^[2]; Ojile, Jack ^[3]; Porotnikov, Dmitry ^[2]; Walker, Lexie ^[2]; Montemurri, Michael ^[2]; Narvaez, Bianca L. ^[2]; Khon, Dmitriy ^[4]; ^[2]; ^[2]

Bowling Green State Univ., OH (United States); BGSU
Bowling Green State Univ., OH (United States)
St. Mary's Univ., San Antonio, TX (United States)
St. Mary’s Univ., San Antonio, TX (United States)

The optoelectronic properties of colloidal semiconductor nanocrystals (NCs) can be manipulated by changing their geometric shapes. The precise synthetic control over particle morphologies, however, has remained elusive. Conventional growth techniques rely on the kinetic assembly of atomic units, where supersaturation and precipitation processes can lead to a broad distribution of particle shapes. In this paper, we demonstrate that replacing atomic precursors with small-size nanocrystals as building blocks for larger colloids offers an easier, more predictive control over nanoparticle shape evolution. The reported growth strategy is illustrated via shape-selective syntheses of CdSe and CdS NC cubes, spheres, rods, as well as unprecedented “donut” and ring-like structures. Growth of desired particle morphologies was achieved by choosing an appropriate reaction solvent that minimizes the surface free energy through a unique shape formation. This so-called "aggregative growth mechanism" is explained using a thermodynamic model for interacting viscous colloids. We expect that this novel growth strategy will offer a viable platform for shape–selective synthesis of many inorganic colloids, providing pathways to optimizable optoelectronic materials.

View Accepted Manuscript (DOE)

Research Organization:: Bowling Green State Univ., OH (United States)

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

Grant/Contract Number:: SC0016872

OSTI ID:: 1865406

Alternate ID(s):: OSTI ID: 1905102

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 5 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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