Towards non-blinking colloidal quantum dots

被引:689
作者
Mahler, Benoit [2 ]
Spinicelli, Piernicola [1 ]
Buil, Stephanie [3 ]
Quelin, Xavier [3 ]
Hermier, Jean-Pierre [1 ,3 ]
Dubertret, Benoit [2 ]
机构
[1] Univ Paris 06, Ecole Normale Super, CNRS UMR8552, Lab Kastler Brossel, F-75231 Paris 05, France
[2] ESPCI, UPR5, CNRS, Lab Photons & Mat, F-75231 Paris, France
[3] Univ Versailles St Quentin en Yvelines, CNRS, UMR 8635, Grp Etud Mat Condensee, F-78035 Versailles, France
关键词
D O I
10.1038/nmat2222
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
At a single-molecule level, fluorophore emission intensity fluctuates between bright and dark states. These fluctuations, known as blinking, limit the use of fluorophores in single-molecule experiments. The dark-state duration shows a universal heavy-tailed power-law distribution characterized by the occurrence of long non-emissive periods. Here we have synthesized novel CdSe-CdS core-shell quantum dots with thick crystalline shells, 68% of which do not blink when observed individually at 33 Hz for 5 min. We have established a direct correlation between shell thickness and blinking occurrences. Importantly, the statistics of dark periods that appear at high acquisition rates (1 kHz) are not heavy tailed, in striking contrast with previous observations. Blinking statistics are thus not as universal as thought so far. We anticipate that our results will help to better understand the physico-chemistry of single-fluorophore emission and rationalize the design of other fluorophores that do not blink.
引用
收藏
页码:659 / 664
页数:6
相关论文
共 32 条
[1]   Statistical aging and nonergodicity in the fluorescence of single nanocrystals [J].
Brokmann, X ;
Hermier, JP ;
Messin, G ;
Desbiolles, P ;
Bouchaud, JP ;
Dahan, M .
PHYSICAL REVIEW LETTERS, 2003, 90 (12) :4-120601
[2]   Power-law intermittency of single emitters [J].
Cichos, F. ;
von Borczyskowski, C. ;
Orrit, M. .
CURRENT OPINION IN COLLOID & INTERFACE SCIENCE, 2007, 12 (06) :272-284
[3]   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
[4]   Explanation of quantum dot blinking without the long-lived trap hypothesis [J].
Frantsuzov, PA ;
Marcus, RA .
PHYSICAL REVIEW B, 2005, 72 (15)
[5]   Blinking and surface chemistry of single CdSe nanocrystals [J].
Gómez, DE ;
van Embden, J ;
Jasieniak, J ;
Smith, TA ;
Mulvaney, P .
SMALL, 2006, 2 (02) :204-208
[6]   Single nonblinking CdTe qnantnm dots synthesized in aqueous thiopropionic acid [J].
He, Hua ;
Qian, Huifeng ;
Dong, Chaoqing ;
Wang, Kanglin ;
Ren, Jicun .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (45) :7588-7591
[7]   Effect of the shell on the blinking statistics of core-shell quantum dots: A single-particle fluorescence study [J].
Heyes, Colin D. ;
Kobitski, Andrei Yu. ;
Breus, Vladimir V. ;
Nienhaus, G. Ulrich .
PHYSICAL REVIEW B, 2007, 75 (12)
[8]   Near-complete suppression of quantum dot blinking in ambient conditions [J].
Hohng, S ;
Ha, T .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (05) :1324-1325
[9]   Power-law blinking in the fluorescence of single organic molecules [J].
Hoogenboom, Jacob P. ;
Hernando, Jordi ;
van Dijk, Erik M. H. R. ;
van Hulst, Niek F. ;
Garcia-Parajo, Maria F. .
CHEMPHYSCHEM, 2007, 8 (06) :823-833
[10]   Power-law-distributed dark states are the main pathway for photobleaching of single organic molecules -: art. no. 097401 [J].
Hoogenboom, JP ;
van Dijk, EMHP ;
Hernando, J ;
van Hulst, NF ;
García-Parajó, MF .
PHYSICAL REVIEW LETTERS, 2005, 95 (09)