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

Carulli, Francesco; Pinchetti, Valerio; Zaffalon, Matteo L.; Camellini, Andrea; Loria, Silvia Rotta; Moro, Fabrizio; Fanciulli, Marco; Zavelani-Rossi, Margherita; Meinardi, Francesco; Crooker, Scott A.; Brovelli, Sergio

doi:10.1021/acs.nanolett.1c01818

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

Journal Article · 13 July 2021 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.1c01818 · OSTI ID:1833263

^[1];

^[1]; Camellini, Andrea ^[2]; Loria, Silvia Rotta ^[2]; Moro, Fabrizio ^[1];

^[1];

^[2]; Meinardi, Francesco ^[1];

^[3];

^[1]

Univ. degli Studi di Milano-Bicocca (Italy)
Politecnico di Milano (Italy)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

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 (V_S) that introduce a donor state below the conduction band (CB), resulting in long-lived intragap luminescence. V_S-localized electrons are almost unaffected by trapping, and suppression of thermal quenching boosts the emission efficiency to 85%. Magneto-optical measurements indicate that the V_S 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.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: National Science Foundation (NSF)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1833263

Report Number(s):: LA-UR-21-24222

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 14 Vol. 21; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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77 NANOSCIENCE AND NANOTECHNOLOGY
bound exciton
electronic doping
high magnetic field science
magneto-optics
nanocrystal quantum dots
spectro-electrochemistry
sulfur vacancy

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

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