Laser-assisted nanofabrication of multielement complex oxide core–shell nanoparticles

Soumya Mandal, Ashish Kumar Gupta, Elena Echeverria, David N. McIlroy, Jonathan D. Poplawsky, Ritesh Sachan

Research output: Contribution to journalArticlepeer-review

13 Scopus citations

Abstract

Nanoparticles with core–shell motifs are of particular interest because they enable combining multiple functionalities at nanoscale. However, a key challenge in designing such novel structures is to phase-separate the constituents at the core and shell regions, especially in thermodynamically miscible systems. In this study, we report the successful formation of self-organized Cr2O3-Fe2O3 core–shell nanoparticles by adopting a non-equilibrium route of pulsed laser-induced dewetting of an alloyed thin film. In this process, the evolution of nanoparticles takes place from the rupture of the initially flat liquid-phase alloyed film under laser irradiation. A continued laser pulsing results in the ripening of the morphologies at different stages eventually leading to a final droplet shape nanoparticle. Using highly sensitive 3D chemical mapping of individual nanoparticles and thermal simulations, we reveal that thermodynamically-soluble Cr2O3 and Fe2O3 phase-segregate in the core and shell regions, respectively, within ∼ 100 ns during a fast solidification process, leveraging the difference in the cooling rates, surface energies and enthalpy of mixing at high-temperatures. With these results, we present a non-equilibrium laser-assisted pathway that can be used to create core–shell nanostructures with dissimilar characteristics.

Original languageEnglish
Article number110882
JournalMaterials and Design
Volume220
DOIs
StatePublished - Aug 2022

Funding

This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://energy.gov/downloads/doe-public-access-plan). RS acknowledges the support of faculty start-up funding at Oklahoma State University. APT was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The authors would like to thank James Burns for assistance in performing APT sample preparation and running the APT experiments. RS acknowledges the support of faculty start-up funding at Oklahoma State University. APT was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The authors would like to thank James Burns for assistance in performing APT sample preparation and running the APT experiments.

Keywords

  • Atom probe tomography
  • Core–shell nanoparticles
  • Dewetting phenomenon
  • Multielement oxide
  • Nanosecond pulsed laser deposition

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