Zinc-Phosphorus Complex Working as an Atomic Valve for Colloidal Growth of Monodisperse Indium Phosphide Quantum Dots

被引:68
作者
Koh, Sungjun [1 ]
Eom, Taedaehyeong [2 ]
Kim, Whi Dong [1 ]
Lee, Kangha [1 ]
Lee, Dongkyu [1 ]
Lee, Young Kuk [3 ]
Kim, Hyungjun [2 ]
Bae, Wan Ki [4 ]
Lee, Doh C. [1 ]
机构
[1] Korea Adv Inst Sci & Technol, KAIST Inst Nanocentury, Dept Chem & Biomol Engn, Daejeon 34141, South Korea
[2] Korea Adv Inst Sci & Technol, Grad Sch Energy Environm Water & Sustainabil EEWS, Daejeon 34141, South Korea
[3] Korea Res Inst Chem Technol, Adv Mat Div, Daejeon 34114, South Korea
[4] Korea Inst Sci & Technol, Photoelect Hybrids Res Ctr, Seoul 02792, South Korea
基金
新加坡国家研究基金会;
关键词
LIGHT-EMITTING-DIODES; INP-AT-ZNSES; PRECURSOR CONVERSION; SEMICONDUCTOR NANOCRYSTALS; INP/ZNS NANOCRYSTALS; SUPPRESSED BLINKING; MASS-SPECTROMETRY; PERFORMANCE; CDSE; CHEMISTRY;
D O I
10.1021/acs.chemmater.7b01648
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Growth of monodisperse indium phosphide (InP) quantum dots (QDs) represents a pressing demand in display applications, as size uniformity is related to color purity in display products. Here, we report the colloidal synthesis of InP QDs in the presence of Zn precursors in which size uniformity is markedly enhanced as compared to the case of InP QDs synthesized without Zn precursors. Nuclear magnetic resonance spectroscopy, X-ray photoelectron spectroscopy, and mass spectrometry analyses on aliquots taken during the synthesis allow us to monitor the appearance of metal phosphorus complex intermediates in the growth of InP QDs. In the presence of zinc carboxylate, intermediate species containing Zn-P bonding appears. The Zn-P intermediate complex with P(SiMe3)(3) exhibits lower reactivity than that of the In P complex, which is corroborated by our prediction based on density functional theory and electrostatic potential charge analysis. The formation of a stable Zn P intermediate complex results in lower reactivity, which enables slow growth of QDs and lowers the extreme reactivity of P(SiMe3)(3), hence monodisperse QDs. Insights from experimental and theoretical studies advance mechanistic understanding and control of nucleation and growth of InP QDs, which are key to the preparation of monodisperse InP-based QDs in meeting the demand of the display market.
引用
收藏
页码:6346 / 6355
页数:10
相关论文
共 55 条
[1]   Perspectives on the physical chemistry of semiconductor nanocrystals [J].
Alivisatos, AP .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (31) :13226-13239
[2]   Mechanistic Insights into the Formation of InP Quantum Dots [J].
Allen, Peter M. ;
Walker, Brian J. ;
Bawendi, Moungi G. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (04) :760-762
[3]   Progress in Non-Cd Quantum Dot Development for Lighting Applications [J].
Anc, M. J. ;
Pickett, N. L. ;
Gresty, N. C. ;
Harris, J. A. ;
Mishra, K. C. .
ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY, 2013, 2 (02) :R3071-R3082
[4]   Quantitative 1H NMR spectroscopy [J].
Bharti, Santosh Kumar ;
Roy, Raja .
TRAC-TRENDS IN ANALYTICAL CHEMISTRY, 2012, 35 :5-26
[5]   Jaguar: A high-performance quantum chemistry software program with strengths in life and materials sciences [J].
Bochevarov, Art D. ;
Harder, Edward ;
Hughes, Thomas F. ;
Greenwood, Jeremy R. ;
Braden, Dale A. ;
Philipp, Dean M. ;
Rinaldo, David ;
Halls, Mathew D. ;
Zhang, Jing ;
Friesner, Richard A. .
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, 2013, 113 (18) :2110-2142
[6]   Mechanistic Insight and Optimization of InP Nanocrystals Synthesized with Aminophosphines [J].
Buffard, Aude ;
Dreyfuss, Sebastien ;
Nadal, Brice ;
Heuclin, Hadrien ;
Xu, Xiangzhen ;
Patriarche, Gilles ;
Mezailles, Nicolas ;
Dubertret, Benoit .
CHEMISTRY OF MATERIALS, 2016, 28 (16) :5925-5934
[7]   Interfacial engineering of core/shell heterostructured nanocrystal quantum dots for light-emitting applications [J].
Chang, Jun Hyuk ;
Hahm, Donghyo ;
Char, Kookheon ;
Bae, Wan Ki .
Journal of Information Display, 2017, 18 (02) :57-65
[8]  
Chen O, 2013, NAT MATER, V12, P445, DOI [10.1038/NMAT3539, 10.1038/nmat3539]
[9]   Control of exciton dynamics in nanodots for quantum operations [J].
Chen, PC ;
Piermarocchi, C ;
Sham, LJ .
PHYSICAL REVIEW LETTERS, 2001, 87 (06) :67401-1
[10]   Shining Light on Indium Phosphide Quantum Dots: Understanding the Interplay among Precursor Conversion, Nucleation, and Growth [J].
Cossairt, Brandi M. .
CHEMISTRY OF MATERIALS, 2016, 28 (20) :7181-7189