Memory in Single Emitter Fluorescence Blinking Reveals the Dynamic Character of Nanoscale Charge Tunneling

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• 作者：Jacob P. Hoogenboom ; Jordi Hernando ; Mar&iacute ; a F. Garc&iacute ; a-Parajó ; Niek F. van Hulst
• 刊名：Journal of Physical Chemistry C
• 出版年：2008
• 出版时间：March 6, 2008
• 年：2008
• 卷：112
• 期：9
• 页码：3417 - 3422
• 全文大小：190K
• 年卷期：v.112,no.9(March 6, 2008)
• ISSN：1932-7455

文摘

Luminescence blinking of single emitters is one of the most profound and intriguing issues in nano-opticsand related areas. Its mechanisms and in particular the often observed deviant power-law statistics are asubject of ongoing recent debate. We examine on-off blinking in a dedicated synthetic trichromophoricassembly of perylene molecules. This trimeric system allows us to unambiguously discern blinking fromphotobleaching events and furthermore displays sufficient blinking events for a single-molecule analysis. Anintriguing memory effect is observed, evidenced in clear correlations between successive on-times. In contrast,successive off-times are only weakly correlated and cross-correlations between on- and off-times are absent.Our results reveal the importance of nanoscale environmental dynamics on top of charge tunneling inunderstanding single emitter luminescence blinking. Dynamics of the polymer matrix and charge carrierstherein is crucial to explain the power-law distribution of on-times. This result is directly relevant for relatedsystems like semiconductor quantum dots, fluorescent proteins, and conjugated polymers.