Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 135, Issue 14, Pages 5278-5281Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja400948t
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Funding
- Global Frontier R&D Program by the Center for Multiscale Energy Systems [2011-0031566]
- WCU program [R31-2008-000-10071-0]
- Industrial Core Grant [10035274]
- NRF grant [2012-046191]
- Korea government (MEST)
- National Research Foundation of Korea [2012R1A2A2A01046191, 2011-0031566, R31-2012-000-10071-0] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Ambient stability of colloidal nanocrystal quantum dots (QDs) is imperative for low-cost, high-efficiency QD photovoltaics. We synthesized air-stable, ultrasmall PbS QDs with diameter (D) down to 1.5 nm, and found an abrupt transition at D approximate to 4 nm in the air stability as the QD size was varied from 1.5 to 7.5 nm. X-ray photoemission spectroscopy measurements and density functional theory calculations reveal that the stability transition is closely associated with the shape transition of oleate-capped QDs from octahedron to cuboctahedron, driven by steric hindrance and thus size-dependent surface energy of oleate-passivated Pb-rich QD facets. This microscopic understanding of the surface chemistry on ultrasmall QDs, up to a few nanometers, should be very useful for precisely and accurately controlling physicochemical properties of colloidal QDs such as doping polarity, carrier mobility, air stability, and hot-carrier dynamics for solar cell applications.
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