TY - JOUR
T1 - Controllable modulation of precursor reactivity using chemical additives for systematic synthesis of high-quality quantum dots
AU - Park, Joonhyuck
AU - Jayaraman, Arun
AU - Schrader, Alex W
AU - Hwang, Gyu Weon
AU - Han, Hee-Sun
N1 - Funding Information:
This work was supported by a start-up fund from the University of Illinois at Urbana-Champaign. G.W.H. acknowledges the financial support from the Korea Institute of Science and Technology (KIST) Institution Program (Grant number 2E30100). We thank Professor Thomas B. Rauchfuss for providing helpful discussions. We thank the SCS NMR Lab and George L. Clark X-Ray Facilities, University of Illinois, for its technical support. The Varian Inova 400-MHz NMR spectrometer was obtained with the financial support of the Roy J. Carver Charitable Trust. Transmission electron microscope measurements were carried out in part in the Materials Research Laboratory Central Research Facilities, University of Illinois. Single QD blinking traces were acquired at Carl R. Woese Institute for Genomic Biology on a demo Alba system provided by ISS, Inc. We thank ISS, Inc. for providing this instrument and Austin Cyphersmith for training and assistance using the Alba system.
PY - 2020/12
Y1 - 2020/12
N2 - The optical and electronic performance of quantum dots (QDs) are affected by their size distribution and structural quality. Although the synthetic strategies for size control are well established and widely applicable to various QD systems, the structural characteristics of QDs, such as morphology and crystallinity, are tuned mostly by trial and error in a material-specific manner. Here, we show that reaction temperature and precursor reactivity, the two parameters governing the surface-reaction kinetics during growth, govern the structural quality of QDs. For conventional precursors, their reactivity is determined by their chemical structure. Therefore, a variation of precursor reactivity requires the synthesis of different precursor molecules. As a result, existing precursor selections often have significant gaps in reactivity or require synthesis of precursor libraries comprising a large number of variants. We designed a sulfur precursor employing a boron-sulfur bond, which enables controllable modulation of their reactivity using commercially available Lewis bases. This precursor chemistry allows systematic optimization of the reaction temperature and precursor reactivity using a single precursor and grows high-quality QDs from cores of various sizes and materials. This work provides critical insights into the nanoparticle growth process and precursor designs, enabling the systematic preparation of high-quality QD of any sizes and materials.
AB - The optical and electronic performance of quantum dots (QDs) are affected by their size distribution and structural quality. Although the synthetic strategies for size control are well established and widely applicable to various QD systems, the structural characteristics of QDs, such as morphology and crystallinity, are tuned mostly by trial and error in a material-specific manner. Here, we show that reaction temperature and precursor reactivity, the two parameters governing the surface-reaction kinetics during growth, govern the structural quality of QDs. For conventional precursors, their reactivity is determined by their chemical structure. Therefore, a variation of precursor reactivity requires the synthesis of different precursor molecules. As a result, existing precursor selections often have significant gaps in reactivity or require synthesis of precursor libraries comprising a large number of variants. We designed a sulfur precursor employing a boron-sulfur bond, which enables controllable modulation of their reactivity using commercially available Lewis bases. This precursor chemistry allows systematic optimization of the reaction temperature and precursor reactivity using a single precursor and grows high-quality QDs from cores of various sizes and materials. This work provides critical insights into the nanoparticle growth process and precursor designs, enabling the systematic preparation of high-quality QD of any sizes and materials.
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U2 - 10.1038/s41467-020-19573-4
DO - 10.1038/s41467-020-19573-4
M3 - Article
C2 - 33184282
SN - 2041-1723
VL - 11
SP - 5748
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 5748
ER -