Structure and Ultrafast Dynamics of White-Light-Emitting CdSe Nanocrystals

被引:89
作者
Bowers, Michael J., II [1 ]
McBride, James R. [1 ]
Garrett, Maria D. [1 ]
Sammons, Jessica A. [1 ]
Dukes, Albert D., III [1 ]
Schreuder, Michael A. [1 ]
Watt, Tony L. [1 ]
Lupini, Andrew R. [5 ]
Pennycook, Stephen J. [5 ]
Rosenthal, Sandra J. [1 ,2 ,3 ,4 ]
机构
[1] Vanderbilt Univ, Dept Chem, Nashville, TN 37235 USA
[2] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA
[3] Vanderbilt Univ, Dept Pharmacol, Nashville, TN 37235 USA
[4] Vanderbilt Univ, Dept Chem & Biomol Engn, Nashville, TN 37235 USA
[5] Oak Ridge Natl Lab, Div Mat Sci & Technol, Oak Ridge, TN 37831 USA
关键词
CARRIER DYNAMICS; QUANTUM DOTS; SIZE; EMISSION; SURFACE;
D O I
10.1021/ja900529h
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
White-light emission from ultrasmall CdSe nanocrystals offers an alternative approach to the realization of solid-state lighting as an appealing technology for consumers. Unfortunately, their extremely small size limits the feasibility of traditional methods for nanocrystal characterization. This paper reports the first images of their structure, which were obtained using aberration-corrected atomic number contrast scanning transmission electron microscopy (Z-STEM). With subangstrom resolution, Z-STEM is one of the few available methods that can be used to directly image the nanocrystal's structure. The initial images suggest that they are crystalline and approximately four lattice planes in diameter. In addition to the structure, for the first time, the exciton dynamics were measured at different wavelengths of the white-light spectrum using ultrafast fluorescence upconversion spectroscopy. The data suggest that a myriad of trap states are responsible for the broad-spectrum emission. It is hoped that the information presented here will provide a foundation for the future development and improvement of white-light-emitting nanocrystals.
引用
收藏
页码:5730 / +
页数:4
相关论文
共 24 条
[1]   Perspectives on the physical chemistry of semiconductor nanocrystals [J].
Alivisatos, AP .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (31) :13226-13239
[2]   ELECTRONIC-STRUCTURE AND PHOTOEXCITED-CARRIER DYNAMICS IN NANOMETER-SIZE CDSE CLUSTERS [J].
BAWENDI, MG ;
WILSON, WL ;
ROTHBERG, L ;
CARROLL, PJ ;
JEDJU, TM ;
STEIGERWALD, ML ;
BRUS, LE .
PHYSICAL REVIEW LETTERS, 1990, 65 (13) :1623-1626
[3]   LUMINESCENCE PROPERTIES OF CDSE QUANTUM CRYSTALLITES - RESONANCE BETWEEN INTERIOR AND SURFACE LOCALIZED STATES [J].
BAWENDI, MG ;
CARROLL, PJ ;
WILSON, WL ;
BRUS, LE .
JOURNAL OF CHEMICAL PHYSICS, 1992, 96 (02) :946-954
[4]   White-light emission from magic-sized cadmium selenide nanocrystals [J].
Bowers, MJ ;
McBride, JR ;
Rosenthal, SJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (44) :15378-15379
[5]   Electron shuttling across the interface of CdSe nanoparticles monitored by femtosecond laser spectroscopy [J].
Burda, C ;
Green, TC ;
Link, S ;
El-Sayed, MA .
JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (11) :1783-1788
[6]   Pinned emission from ultrasmall cadmium selenide nanocrystals [J].
Dukes, Albert D., III ;
Schreuder, Michael A. ;
Sammons, Jessica A. ;
McBride, James R. ;
Smith, Nathanael J. ;
Rosenthal, Sandra J. .
JOURNAL OF CHEMICAL PHYSICS, 2008, 129 (12)
[7]   Band edge dynamics in CdSe nanocrystals observed by ultrafast fluorescence upconversion [J].
Garrett, Maria Danielle ;
Bowers, Michael J., II ;
McBride, James R. ;
Orndorff, Rebecca L. ;
Pennycook, Stephen J. ;
Rosenthal, Sandra J. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (02) :436-442
[8]   Intraband relaxation in CdSe quantum dots [J].
Guyot-Sionnest, P ;
Shim, M ;
Matranga, C ;
Hines, M .
PHYSICAL REVIEW B, 1999, 60 (04) :R2181-R2184
[9]   Phosphine-free synthesis of CdSe nanocrystals [J].
Jasieniak, J ;
Bullen, C ;
van Embden, J ;
Mulvaney, P .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (44) :20665-20668
[10]   Structure-property correlation of CdSe clusters using experimental results and first-principles DFT calculations [J].
Jose, R ;
Zhanpeisov, NU ;
Fukumura, H ;
Baba, Y ;
Ishikawa, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (02) :629-636