Optical and Electronic Properties of Nonconcentric PbSe/CdSe Colloidal Quantum Dots.
Lead chalcogenide colloidal quantum dots are attractive candidates for applications operating in the near infrared spectral range. However, their function is forestalled by limited stability under ambient conditions. Prolonged temperature-activated cation-exchange of Cd(2+) for Pb(2+) forms PbSe/CdSe core/shell heterostructures, unveiling a promising surface passivation route and a method to modify the dots' electronic properties. Here, we follow early stages of an-exchange process, using spectroscopic and structural characterization tools, as well as numerical calculations. We illustrate that preliminary-exchange stages involve the formation of nonconcentric heterostructures, presumably due to a facet selective reaction, showing a pronounced change in the optical properties upon the increase of the degree of nonconcentricity or/and plausible creation of core/shell interfacial alloying. However, progressive-exchange stages lead to rearrangement of the shell segment into uniform coverage, providing tolerance to oxygen exposure with a spectral steadiness already on the formation of a monolayer shell.
§Schulich Faculty of Chemistry, Solid State Institute, Russell Berrie Nanotechnology Institute, Technion-Israel Institute of Technology, Haifa 3200025, Israel.
Gary
G
Zaiats
§Schulich Faculty of Chemistry, Solid State Institute, Russell Berrie Nanotechnology Institute, Technion-Israel Institute of Technology, Haifa 3200025, Israel.
Arthur
A
Shapiro
§Schulich Faculty of Chemistry, Solid State Institute, Russell Berrie Nanotechnology Institute, Technion-Israel Institute of Technology, Haifa 3200025, Israel.
Diana
D
Yanover
†Department of Materials Science and Engineering, Technion-Israel Institute of Technology, Haifa 3200025, Israel.
Yaron
Y
Kauffmann
§Schulich Faculty of Chemistry, Solid State Institute, Russell Berrie Nanotechnology Institute, Technion-Israel Institute of Technology, Haifa 3200025, Israel.
Aldona
A
Sashchiuk
§Schulich Faculty of Chemistry, Solid State Institute, Russell Berrie Nanotechnology Institute, Technion-Israel Institute of Technology, Haifa 3200025, Israel.
Efrat
E
Lifshitz
D019187:Cadmium Compounds / Q000737:chemistry*; D004581:Electronics; D007854:Lead / Q000737:chemistry*; D045663:Quantum Dots; D018036:Selenium Compounds / Q000737:chemistry*; D013057:Spectrum Analysis / Q000379:methods*
D019187:Cadmium Compounds; D018036:Selenium Compounds; C088065:lead selenide; D007854:Lead
cation-exchange; colloidal quantum dots; effective mass approximation; nonconcentric core/shell