Quantized Electronic Doping towards Atomically Controlled “Charge-Engineered” Semiconductor Nanocrystals

Capitani, Chiara; Pinchetti, Valerio; Gariano, Graziella; Santiago-González, Beatriz; Santambrogio, Carlo; Campione, Marcello; Prato, Mirko; Brescia, Rosaria; Camellini, Andrea; Bellato, Fulvio; Carulli, Francesco; Anand, Abhinav; Zavelani-Rossi, Margherita; Meinardi, Francesco; Crooker, Scott A.; Brovelli, Sergio

doi:10.1021/acs.nanolett.8b04904

Title: Quantized Electronic Doping towards Atomically Controlled “Charge-Engineered” Semiconductor Nanocrystals

Journal Article · 20 January 2019 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.8b04904 · OSTI ID:1503187

Capitani, Chiara ^[1];

^[2]; Gariano, Graziella ^[3]; Santiago-González, Beatriz ^[4]; Santambrogio, Carlo ^[5]; Campione, Marcello ^[6];

^[7]; Brescia, Rosaria ^[7]; Camellini, Andrea ^[8]; Bellato, Fulvio ^[2];

^[2]; Anand, Abhinav ^[2];

^[8]; Meinardi, Francesco ^[2];

^[9];

^[2]

Univ. of Milano-Bicocca, Milan (Italy). Dept. of Materials Science; Glass to Power SpA, Rovereto (Italy)
Univ. of Milano-Bicocca, Milan (Italy). Dept. of Materials Science
Glass to Power SpA, Rovereto (Italy)
Univ. of Milano-Bicocca, Milan (Italy). Dept. of Materials Science; International Iberian Nanotechnology Lab., Braga (Portugal). Nanophotonics Dept. Ultrafast Bio- and Nanophotonics Group
Univ. of Milano-Bicocca, Milan (Italy). Dept. of Biotechnology and Biosciences
Univ. of Milano-Bicocca, Milan (Italy). Dept. of Environmental and Land Sciences and Earth Sciences
Italian Inst. of Technology (IIT), Genoa (Italy)
Polytechnic Univ. of Milan (Italy). Dept. of Energy
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

“Charge engineering” of semiconductor nanocrystals (NCs) through so-called electronic impurity doping is a long-standing challenge in colloidal chemistry and holds promise for ground-breaking advancements in many optoelectronic, photonic, and spin-based nanotechnologies. To date, our knowledge is limited to a few paradigmatic studies on a small number of model compounds and doping conditions, with important electronic dopants still unexplored in nanoscale systems. Equally importantly, fine-tuning of charge engineered NCs is hampered by the statistical limitations of traditional approaches. The resulting intrinsic doping inhomogeneity restricts fundamental studies to statistically averaged behaviors and complicates the realization of advanced device concepts based on their advantageous functionalities. We aim to address these issues by realizing the first example of II–VI NCs electronically doped with an exact number of heterovalent gold atoms, a known p-type acceptor impurity in bulk chalcogenides. Single-dopant accuracy across entire NC ensembles is obtained through a novel non-injection synthesis employing ligand-exchanged gold clusters as “quantized” dopant sources to seed the nucleation of CdSe NCs in organic media. Structural, spectroscopic, and magneto-optical investigations trace a comprehensive picture of the physical processes resulting from the exact doping level of the NCs. Gold atoms, doped here for the first time into II–VI NCs, are found to incorporate as nonmagnetic Au⁺ species activating intense size-tunable intragap photoluminescence and artificially offsetting the hole occupancy of valence band states. Fundamentally, the transient conversion of Au⁺ to paramagnetic Au²⁺ (5d⁹ configuration) under optical excitation results in strong photoinduced magnetism and diluted magnetic semiconductor behavior revealing the contribution of individual paramagnetic impurities to the macroscopic magnetism of the NCs. Altogether, our results demonstrate a new chemical approach toward NCs with physical functionalities tailored to the single impurity level and offer a versatile platform for future investigations and device exploitation of individual and collective impurity processes in quantum confined structures.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Milano-Bicocca, Milan (Italy)

Sponsoring Organization:: Ministry of Education, Universities and Research (MIUR) (Italy); National Science Foundation (NSF) (United States); USDOE

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1503187

Report Number(s):: LA-UR--18-28429

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 2 Vol. 19; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
diluted magnetic semiconductors
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nanocrystal quantum dots
photophysics
seeded growth

Title: Quantized Electronic Doping towards Atomically Controlled “Charge-Engineered” Semiconductor Nanocrystals

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