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Temperature-Controlled Reversible Formation and Phase Transformation of 3D Nanocrystal Superlattices Through In Situ Small-Angle X-ray Scattering
Abstract
For decades, the spontaneous organization of nanocrystals into superlattices has captivated the scientific community. However, achieving direct control over the formation of the superlattice and its phase transformations has proven to be a grand challenge, often resulting in the generation of multiple symmetries under the same experimental conditions. Here, we achieve direct control over the formation of the superlattice and its phase transformations by modulating the thermal energy of a nanocrystal dispersion without relying on solvent evaporation. In this study, we follow the temperature-dependent dynamics of the self-assembly process using synchrotron-based small-angle X-ray scattering. When cooled below –24.5 °C, lead sulfide nanocrystals form micrometer-sized three-dimensional phase-pure body-centered cubic superlattices. When cooled below –35.1 °C, these superlattices undergo a collective diffusionless phase transformation that yields denser body-centered tetragonal phases. These structural changes can be reversed by increasing the temperature of the dispersion and may lead to the direct modulation of the optical properties of these artificial solids.
- Authors:
-
[1];
[2];
- Univ. of Pennsylvania, Philadelphia, PA (United States); Univ. degli Studi di Palermo (Italy)
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)
- OSTI Identifier:
- 2229629
- Report Number(s):
- BNL-225050-2023-JAAM
Journal ID: ISSN 1530-6984
- Grant/Contract Number:
- SC0012704; DMR-2019444
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 23; Journal Issue: 10; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; nanocrystal; phase transformation; self-assembly; superlattice; SAXS; reversible
Citation Formats
Marino, Emanuele, Rosen, Daniel J., Yang, Shengsong, Tsai, Esther H. R., and Murray, Christopher B. Temperature-Controlled Reversible Formation and Phase Transformation of 3D Nanocrystal Superlattices Through In Situ Small-Angle X-ray Scattering. United States: N. p., 2023.
Web. doi:10.1021/acs.nanolett.3c00299.
Marino, Emanuele, Rosen, Daniel J., Yang, Shengsong, Tsai, Esther H. R., & Murray, Christopher B. Temperature-Controlled Reversible Formation and Phase Transformation of 3D Nanocrystal Superlattices Through In Situ Small-Angle X-ray Scattering. United States. https://doi.org/10.1021/acs.nanolett.3c00299
Marino, Emanuele, Rosen, Daniel J., Yang, Shengsong, Tsai, Esther H. R., and Murray, Christopher B. Mon .
"Temperature-Controlled Reversible Formation and Phase Transformation of 3D Nanocrystal Superlattices Through In Situ Small-Angle X-ray Scattering". United States. https://doi.org/10.1021/acs.nanolett.3c00299.
@article{osti_2229629,
title = {Temperature-Controlled Reversible Formation and Phase Transformation of 3D Nanocrystal Superlattices Through In Situ Small-Angle X-ray Scattering},
author = {Marino, Emanuele and Rosen, Daniel J. and Yang, Shengsong and Tsai, Esther H. R. and Murray, Christopher B.},
abstractNote = {For decades, the spontaneous organization of nanocrystals into superlattices has captivated the scientific community. However, achieving direct control over the formation of the superlattice and its phase transformations has proven to be a grand challenge, often resulting in the generation of multiple symmetries under the same experimental conditions. Here, we achieve direct control over the formation of the superlattice and its phase transformations by modulating the thermal energy of a nanocrystal dispersion without relying on solvent evaporation. In this study, we follow the temperature-dependent dynamics of the self-assembly process using synchrotron-based small-angle X-ray scattering. When cooled below –24.5 °C, lead sulfide nanocrystals form micrometer-sized three-dimensional phase-pure body-centered cubic superlattices. When cooled below –35.1 °C, these superlattices undergo a collective diffusionless phase transformation that yields denser body-centered tetragonal phases. These structural changes can be reversed by increasing the temperature of the dispersion and may lead to the direct modulation of the optical properties of these artificial solids.},
doi = {10.1021/acs.nanolett.3c00299},
journal = {Nano Letters},
number = 10,
volume = 23,
place = {United States},
year = {Mon May 15 00:00:00 EDT 2023},
month = {Mon May 15 00:00:00 EDT 2023}
}
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