Optical and Magneto-Optical Properties of Donor-Bound Excitons in Vacancy-Engineered Colloidal Nanocrystals

Autor: Sergio Brovelli, Francesco Meinardi, Scott A. Crooker, Matteo L. Zaffalon, Marco Fanciulli, Andrea Camellini, Silvia Rotta Loria, Francesco Carulli, Fabrizio Moro, Valerio Pinchetti, Margherita Zavelani-Rossi
Přispěvatelé: Carulli, F, Pinchetti, V, Zaffalon, M, Camellini, A, Rotta Loria, S, Moro, F, Fanciulli, M, Zavelani-Rossi, M, Meinardi, F, Crooker, S, Brovelli, S
Rok vydání: 2021
Předmět:
Zdroj: Nano Letters
ISSN: 1530-6992
1530-6984
DOI: 10.1021/acs.nanolett.1c01818
Popis: Controlled insertion of electronic states within the band gap of semiconductor nanocrystals (NCs) is a powerful tool for tuning their physical properties. One compelling example is II-VI NCs incorporating heterovalent coinage metals in which hole capture produces acceptor-bound excitons. To date, the opposite donor-bound exciton scheme has not been realized because of the unavailability of suitable donor dopants. Here, we produce a model system for donor-bound excitons in CdSeS NCs engineered with sulfur vacancies (VS) that introduce a donor state below the conduction band (CB), resulting in long-lived intragap luminescence. VS-localized electrons are almost unaffected by trapping, and suppression of thermal quenching boosts the emission efficiency to 85%. Magneto-optical measurements indicate that the VS are not magnetically coupled to the NC bands and that the polarization properties are determined by the spin of the valence-band photohole, whose spin flip is massively slowed down due to suppressed exchange interaction with the donor-localized electron.
Databáze: OpenAIRE