Lifetime blinking in nonblinking nanocrystal quantum dots

被引:208
作者
Galland, Christophe [1 ,2 ]
Ghosh, Yagnaseni [3 ,4 ]
Steinbrueck, Andrea [3 ,4 ]
Hollingsworth, Jennifer A. [3 ,4 ]
Htoon, Han [1 ,4 ]
Klimov, Victor I. [1 ,2 ]
机构
[1] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
[2] Los Alamos Natl Lab, Ctr Adv Solar Photophys, Los Alamos, NM 87545 USA
[3] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA
[4] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA
来源
NATURE COMMUNICATIONS | 2012年 / 3卷
关键词
PHOTOLUMINESCENCE; INTERMITTENCY; INTENSITY; CHARGE;
D O I
10.1038/ncomms1916
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Nanocrystal quantum dots are attractive materials for applications as nanoscale light sources. One impediment to these applications is fluctuations of single-dot emission intensity, known as blinking. Recent progress in colloidal synthesis has produced nonblinking nanocrystals; however, the physics underlying blinking suppression remains unclear. Here we find that ultra-thick-shell CdSe/CdS nanocrystals can exhibit pronounced fluctuations in the emission lifetimes (lifetime blinking), despite stable nonblinking emission intensity. We demonstrate that lifetime variations are due to switching between the neutral and negatively charged state of the nanocrystal. Negative charging results in faster radiative decay but does not appreciably change the overall emission intensity because of suppressed nonradiative Auger recombination for negative trions. The Auger process involving excitation of a hole (positive trion pathway) remains efficient and is responsible for charging with excess electrons, which occurs via Auger-assisted ionization of biexcitons accompanied by ejection of holes.
引用
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页数:7
相关论文
共 34 条
[1]   Nano-engineered electron-hole exchange interaction controls exciton dynamics in core-shell semiconductor nanocrystals [J].
Brovelli, S. ;
Schaller, R. D. ;
Crooker, S. A. ;
Garcia-Santamaria, F. ;
Chen, Y. ;
Viswanatha, R. ;
Hollingsworth, J. A. ;
Htoon, H. ;
Klimov, V. I. .
NATURE COMMUNICATIONS, 2011, 2
[2]   Giant multishell CdSe nanocrystal quantum dots with suppressed blinking [J].
Chen, Yongfen ;
Vela, Javier ;
Htoon, Han ;
Casson, Joanna L. ;
Werder, Donald J. ;
Bussian, David A. ;
Klimov, Victor I. ;
Hollingsworth, Jennifer A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (15) :5026-5027
[3]   Suppression of Auger Processes in Confined Structures [J].
Cragg, George E. ;
Efros, Alexander L. .
NANO LETTERS, 2010, 10 (01) :313-317
[4]   Random telegraph signal in the photoluminescence intensity of a single quantum dot [J].
Efros, AL ;
Rosen, M .
PHYSICAL REVIEW LETTERS, 1997, 78 (06) :1110-1113
[5]   ABSORPTION AND INTENSITY-DEPENDENT PHOTOLUMINESCENCE MEASUREMENTS ON CDSE QUANTUM DOTS - ASSIGNMENT OF THE 1ST ELECTRONIC-TRANSITIONS [J].
EKIMOV, AI ;
HACHE, F ;
SCHANNEKLEIN, MC ;
RICARD, D ;
FLYTZANIS, C ;
KUDRYAVTSEV, IA ;
YAZEVA, TV ;
RODINA, AV ;
EFROS, AL .
JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 1993, 10 (01) :100-107
[6]   Universal emission intermittency in quantum dots, nanorods and nanowires [J].
Frantsuzov, Pavel ;
Kuno, Masaru ;
Janko, Boldizsar ;
Marcus, Rudolph A. .
NATURE PHYSICS, 2008, 4 (07) :519-522
[7]   Model of Fluorescence Intermittency of Single Colloidal Semiconductor Quantum Dots Using Multiple Recombination Centers [J].
Frantsuzov, Pavel A. ;
Volkan-Kacso, Sandor ;
Janko, Boldizsar .
PHYSICAL REVIEW LETTERS, 2009, 103 (20)
[8]   Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots [J].
Galland, Christophe ;
Ghosh, Yagnaseni ;
Steinbrueck, Andrea ;
Sykora, Milan ;
Hollingsworth, Jennifer A. ;
Klimov, Victor I. ;
Htoon, Han .
NATURE, 2011, 479 (7372) :203-U75
[9]   Breakdown of Volume Scaling in Auger Recombination in CdSe/CdS Heteronanocrystals: The Role of the Core-Shell Interface [J].
Garcia-Santamaria, Florencio ;
Brovelli, Sergio ;
Viswanatha, Ranjani ;
Hollingsworth, Jennifer A. ;
Htoon, Han ;
Crooker, Scott A. ;
Klimov, Victor I. .
NANO LETTERS, 2011, 11 (02) :687-693
[10]   Suppressed Auger Recombination in "Giant" Nanocrystals Boosts Optical Gain Performance [J].
Garcia-Santamaria, Florencio ;
Chen, Yongfen ;
Vela, Javier ;
Schaller, Richard D. ;
Hollingsworth, Jennifer A. ;
Klimov, Victor I. .
NANO LETTERS, 2009, 9 (10) :3482-3488