Pulsed Laser Synthesis of Carbon Nanostructures from Organic Molecular Liquids: Structure, Kinetics and Photophysical Properties

The striking one-step bottom-up synthesis of carbon nanoparticles (CNPs) from visible and near infrared (NIR) light transparent air-equilibrated liquid aromatic compounds (benzene, toluene, chlorobenzene, aniline, pyrrole, and thiophene) under unfocused pulsed nanosecond laser irradiation (532/1064...

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Detalles Bibliográficos
Autores: Ribeiro-González, Antonio, Agudo-Blanco, Carlos, Ramírez-Barroso, Sergio, Navío, Cristina, Bañares, Luis, Bresolí-Obach, Roger, Nonell, Santi, Martín, Nazario, García-Fresnadillo, David
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universitat Ramon Llull (URL)
Repositorio:DAU Arxiu Digital de la Universitat Ramon Llull
OAI Identifier:oai:dau.url.edu:20.500.14342/5602
Acceso en línea:http://hdl.handle.net/20.500.14342/5602
https://doi.org/10.1002/advs.202505883
Access Level:acceso abierto
Palabra clave:Carbon nanodot
Carbon nanoparticle
Graphene quantum dot
Pulsed laser synthesis
Wavelength-dependent fluorescence
Materials nanoestructurats
Nanopartícules
Carboni
Grafè
Dipòsit per làser pulsat
620
Descripción
Sumario:The striking one-step bottom-up synthesis of carbon nanoparticles (CNPs) from visible and near infrared (NIR) light transparent air-equilibrated liquid aromatic compounds (benzene, toluene, chlorobenzene, aniline, pyrrole, and thiophene) under unfocused pulsed nanosecond laser irradiation (532/1064 nm) is reported. The formation of CNPs follows zero-order kinetics with an induction period dependent on the reactivity of the organic precursor. Experimental evidence suggests a surface-catalyzed photochemical process involving a partial change in C-atom hybridization from sp2 to sp3, with oxygen-based functional groups passivating the surface of the nanostructures. The presence of additional heteroatoms depends on the structure and composition of the precursor. Contingent on the starting compound, the prepared CNPs can be classified as amorphous carbon nanodots (CNDs) or layered curved-graphene quantum dots (c-GQDs), resembling nano-onion fragments. CNDs are obtained from substituted benzenes or heterocyclic compounds, whereas c-GQDs can be synthesized from benzene. Photophysical characterization of the CNPs shows both wavelength-dependent excitation and emission bands, with constant emission quantum yields in the 1–10% range, and wavelength-dependent emission decays displaying several lifetime components in the range 1–20 ns. Triplet exciton lifetimes longer than 5 µs and wavelength-dependent singlet oxygen production quantum yields in the 10–40% range have been measured.