Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys

Abstract Laser ablation in liquid (LAL) is a reference technique for the synthesis of multicomponent non‐equilibrium nanomaterials which have potentially disruptive properties in photonics, nanomedicine, and catalysis. Yet, ablation dynamics is poorly understood regarding the multielement matter and...

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Main Authors: Vito Coviello, Catherine Reffatto, Mehdi W. Fawaz, Benoit Mahler, Arnaud Sollier, Bratislav Lukic, Alexander Rack, David Amans, Vincenzo Amendola
Format: Article
Language:English
Published: Wiley 2025-06-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202416035
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author Vito Coviello
Catherine Reffatto
Mehdi W. Fawaz
Benoit Mahler
Arnaud Sollier
Bratislav Lukic
Alexander Rack
David Amans
Vincenzo Amendola
author_facet Vito Coviello
Catherine Reffatto
Mehdi W. Fawaz
Benoit Mahler
Arnaud Sollier
Bratislav Lukic
Alexander Rack
David Amans
Vincenzo Amendola
author_sort Vito Coviello
collection DOAJ
description Abstract Laser ablation in liquid (LAL) is a reference technique for the synthesis of multicomponent non‐equilibrium nanomaterials which have potentially disruptive properties in photonics, nanomedicine, and catalysis. Yet, ablation dynamics is poorly understood regarding the multielement matter and, therefore, the remarkable potential of LAL for controlling the local atomic structure of metastable nanophases remains largely unexploited. Here, the dynamics of LAL are investigated with non‐equilibrium gold‐iron nanoalloys generated in the presence of gas‐evolving additives, which drive the formation of different nanostructures. With analytical electron microscopy, the structure in the different conditions is properly identified through complete segregation into oxide‐metal heterostructures, precipitation of nanoclusters within the nanoalloys, or ordered solid solutions. To elucidate the unforeseen effects of the solutes on the atomic structure of nanoalloys, the early and full dynamics of LAL is investigated with time‐resolved experiments, leading to the pivotal evidence that alloying of metastable compounds with different chemical reactivity is favored by decreasing the pressure of the shockwave front. The resulting picture indicates LAL with gas‐evolving additives as a strategy for molding the atomic structure of non‐equilibrium nanoalloys, opening the way to the development of a library of advanced nanomaterials otherwise inaccessible.
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spelling doaj-art-e7a7c8920e694ebca13577f96a621a752025-08-20T02:02:58ZengWileyAdvanced Science2198-38442025-06-011221n/an/a10.1002/advs.202416035Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium NanoalloysVito Coviello0Catherine Reffatto1Mehdi W. Fawaz2Benoit Mahler3Arnaud Sollier4Bratislav Lukic5Alexander Rack6David Amans7Vincenzo Amendola8Department of Chemical Sciences Università di Padova via Marzolo 1 Padova I‐35131 ItalyDepartment of Chemical Sciences Università di Padova via Marzolo 1 Padova I‐35131 ItalyUniversité Claude Bernard Lyon 1 UMR 5306 CNRS Institut Lumière Matière Villeurbanne F‐69100 FranceUniversité Claude Bernard Lyon 1 UMR 5306 CNRS Institut Lumière Matière Villeurbanne F‐69100 FranceCEA DAM DIF Arpajon F‐91297 FranceESRF‐The European Synchrotron CS40220 Grenoble F‐38043 FranceESRF‐The European Synchrotron CS40220 Grenoble F‐38043 FranceUniversité Claude Bernard Lyon 1 UMR 5306 CNRS Institut Lumière Matière Villeurbanne F‐69100 FranceDepartment of Chemical Sciences Università di Padova via Marzolo 1 Padova I‐35131 ItalyAbstract Laser ablation in liquid (LAL) is a reference technique for the synthesis of multicomponent non‐equilibrium nanomaterials which have potentially disruptive properties in photonics, nanomedicine, and catalysis. Yet, ablation dynamics is poorly understood regarding the multielement matter and, therefore, the remarkable potential of LAL for controlling the local atomic structure of metastable nanophases remains largely unexploited. Here, the dynamics of LAL are investigated with non‐equilibrium gold‐iron nanoalloys generated in the presence of gas‐evolving additives, which drive the formation of different nanostructures. With analytical electron microscopy, the structure in the different conditions is properly identified through complete segregation into oxide‐metal heterostructures, precipitation of nanoclusters within the nanoalloys, or ordered solid solutions. To elucidate the unforeseen effects of the solutes on the atomic structure of nanoalloys, the early and full dynamics of LAL is investigated with time‐resolved experiments, leading to the pivotal evidence that alloying of metastable compounds with different chemical reactivity is favored by decreasing the pressure of the shockwave front. The resulting picture indicates LAL with gas‐evolving additives as a strategy for molding the atomic structure of non‐equilibrium nanoalloys, opening the way to the development of a library of advanced nanomaterials otherwise inaccessible.https://doi.org/10.1002/advs.202416035laser ablationmagneto‐plasmonicsnanoalloysnanoparticlesnonequilibriumtime‐resolved
spellingShingle Vito Coviello
Catherine Reffatto
Mehdi W. Fawaz
Benoit Mahler
Arnaud Sollier
Bratislav Lukic
Alexander Rack
David Amans
Vincenzo Amendola
Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys
Advanced Science
laser ablation
magneto‐plasmonics
nanoalloys
nanoparticles
nonequilibrium
time‐resolved
title Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys
title_full Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys
title_fullStr Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys
title_full_unstemmed Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys
title_short Time‐Resolved Dynamics of Laser Ablation in Liquid with Gas‐Evolving Additives: Toward Molding the Atomic Structure of Nonequilibrium Nanoalloys
title_sort time resolved dynamics of laser ablation in liquid with gas evolving additives toward molding the atomic structure of nonequilibrium nanoalloys
topic laser ablation
magneto‐plasmonics
nanoalloys
nanoparticles
nonequilibrium
time‐resolved
url https://doi.org/10.1002/advs.202416035
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