Role of thermally occupied hole states in room-temperature broadband gain in CdSe/CdS giant-shell nanocrystals
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Otros documentos de la autoría: Tanghe, Ivo; Llusar, Jordi; Climente, Juan I.; Barker, Alex J.; Paternò, Giuseppe Maria; Scotognella, Francesco; Polovitsyn, Anatolii; Khan, Ali Hossain; hens, zeger; Van Thourhout, Dries; Geiregat, Pieter; Moreels, Iwan
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Mostrar el registro completo del ítemcomunitat-uji-handle:10234/9
comunitat-uji-handle2:10234/7013
comunitat-uji-handle3:10234/8638
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INVESTIGACIONMetadatos
Título
Role of thermally occupied hole states in room-temperature broadband gain in CdSe/CdS giant-shell nanocrystalsAutoría
Fecha de publicación
2022Editor
WileyISSN
2195-1071Cita bibliográfica
Tanghe, I., Llusar, J., Climente, J. I., Barker, A., Paternò, G., Scotognella, F., Polovitsyn, A., Khan, A. H., Hens, Z., Van Thourhout, D., Geiregat, P., Moreels, I., Role of Thermally Occupied Hole States in Room-Temperature Broadband Gain in CdSe/CdS Giant-Shell Nanocrystals. Adv. Optical Mater. 2022, 2201378. https://doi.org/10.1002/adom.202201378Tipo de documento
info:eu-repo/semantics/articleVersión
info:eu-repo/semantics/publishedVersionPalabras clave / Materias
Resumen
Growing CdSe/CdS nanocrystals from a large CdSe core, and employing a giant CdS shell, a continuous, broadband gain spectrum, covering the spectral range between the CdSe and the CdS band edge, is induced. As revealed ... [+]
Growing CdSe/CdS nanocrystals from a large CdSe core, and employing a giant CdS shell, a continuous, broadband gain spectrum, covering the spectral range between the CdSe and the CdS band edge, is induced. As revealed by k·p calculations, this feature is enabled by a set of closely spaced S-, P- and, for larger CdSe cores, D-state hole levels, which are thermally occupied at room temperature, combined with a sparse density of electron states. This leads to a range of bleach signals in the transient absorption spectra that persist up to a microsecond. By extending a state-filling model including relevant higher-energy states and a Fermi–Dirac distribution of holes at finite temperature, it is shown that thermal occupancy can lower the gain threshold for excited states. Inclusion of Gaussian broadening of discrete transitions also leads to a smoothening of the gain threshold spectrum. Next to a direct measurement of the gain threshold, a method is also developed to extract this from the gain lifetime, taking advantage that population inversion is limited by Auger recombination and recombination rates scale with the exciton density as 〈N〉·(〈N〉 − 1). The results should be readily extendable to other systems, such as perovskite or III–V colloidal nanocrystals. [-]
Publicado en
Advanced Optical Materials 2022, 2201378Entidad financiadora
European Comission | Generalitat Valencian
Identificador de la entidad financiadora
PHOCONA
Código del proyecto o subvención
info:eu-repo/grantAgreement/EC/H2020/714876 | PROMETEO/2018/098
Derechos de acceso
info:eu-repo/semantics/openAccess
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