Exciton Dissociation in CdSe Quantum Dots by Hole Transfer to Phenothiazine

被引:171
作者
Huang, Jier [1 ]
Huang, Zhuangqun [1 ]
Jin, Shengye [1 ]
Lian, Tianquan [1 ]
机构
[1] Emory Univ, Dept Chem, Atlanta, GA 30322 USA
基金
美国国家科学基金会;
关键词
D O I
10.1021/jp808291u
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
Ultrafast charge transfer from quantum dots (QDs) is essential for their application in solar cells. Photoinduced hole transfer from CdSe QDs (with first exciton peak at 462 run and estimated radius of 1.8 nm) to phenothiazine (PTZ) was investigated by time-resolved fluorescence and transient absorption spectroscopy. Fluorescence lifetime measurements showed that the presence of PTZ reduced the exciton lifetime of CdSe QDs, and the quenching rate increased with increasing PTZ concentration. Transient absorption spectra of CdSe-PTZ complexes directly revealed the formation of PTZ cation radical, suggesting that the excitons in CdSe dissociated by hole transfer to PTZ. A kinetic model based on a Poisson distribution of the number of adsorbates on each QD was found to adequately describe the adsorbate concentration-dependent fluorescence decay kinetics. According to this model, the hole transfer time was similar to 2.5 ns in 1: 1 CdSe-PTZ complexes and reached similar to 300 ps in samples with an average of similar to 6 PTZ per QD.
引用
收藏
页码:19734 / 19738
页数:5
相关论文
共 62 条
[1]   Influence of electronic structure and multiexciton spectral density on multiple-exciton generation in semiconductor nanocrystals: Tight-binding calculations [J].
Allan, G. ;
Delerue, C. .
PHYSICAL REVIEW B, 2008, 77 (12)
[2]   Multiple exciton generation in colloidal silicon nanocrystals [J].
Beard, Matthew C. ;
Knutsen, Kelly P. ;
Yu, Pingrong ;
Luther, Joseph M. ;
Song, Qing ;
Metzger, Wyatt K. ;
Ellingson, Randy J. ;
Nozik, Arthur J. .
NANO LETTERS, 2007, 7 (08) :2506-2512
[3]   On the absence of detectable carrier multiplication in a transient absorption study of InAs/CdSe/ZnSe core/shell1/shell2 quantum dots [J].
Ben-Lulu, Meirav ;
Mocatta, David ;
Bonn, Mischa ;
Banin, Uri ;
Ruhman, Sanford .
NANO LETTERS, 2008, 8 (04) :1207-1211
[4]   Electron transfer dynamics in quantum dot/titanium dioxide composites formed by in situ chemical bath deposition [J].
Blackburn, JL ;
Selmarten, DC ;
Nozik, AJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (51) :14154-14157
[5]   Ultrafast charge separation at CdS quantum dot/rhodamine B molecule interface [J].
Boulesbaa, Abdelaziz ;
Issac, Abey ;
Stockwell, Dave ;
Huang, Zhuangqun ;
Huang, Jier ;
Guo, Jianchang ;
Lian, Tianquan .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (49) :15132-+
[8]   The pump power dependence of the femtosecond relaxation of CdSe nanoparticles observed in the spectral range from visible to infrared [J].
Burda, C ;
Link, S ;
Mohamed, MB ;
El-Sayed, M .
JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (09) :3828-3833
[9]   The relaxation pathways of CdSe nanoparticles monitored with femtosecond time-resolution from the visible to the IR: Assignment of the transient features by carrier quenching [J].
Burda, C ;
Link, S ;
Mohamed, M ;
El-Sayed, M .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (49) :12286-12292
[10]   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