Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots
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作者:
Galland, Christophe
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Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Los Alamos Natl Lab, Ctr Adv Solar Photophys, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Galland, Christophe
[1
,2
]
Ghosh, Yagnaseni
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Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Ghosh, Yagnaseni
[3
]
Steinbrueck, Andrea
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机构:
Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Steinbrueck, Andrea
[3
]
Sykora, Milan
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Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Sykora, Milan
[1
]
Hollingsworth, Jennifer A.
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Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Hollingsworth, Jennifer A.
[3
]
Klimov, Victor I.
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机构:
Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Los Alamos Natl Lab, Ctr Adv Solar Photophys, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Klimov, Victor I.
[1
,2
]
Htoon, Han
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机构:
Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Los Alamos Natl Lab, Ctr Adv Solar Photophys, Los Alamos, NM 87545 USA
Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USALos Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA
Htoon, Han
[1
,2
,3
]
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, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA
Photoluminescence blinking-random switching between states of high (ON) and low (OFF) emissivities-is a universal property of molecular emitters found in dyes(1), polymers(2), biological molecules(3) and artificial nanostructures such as nanocrystal quantum dots, carbon nanotubes and nanowires(4-6). For the past 15 years, colloidal nanocrystals have been used as a model system to study this phenomenon(5,6). The occurrence of OFF periods in nanocrystal emission has been commonly attributed to the presence of an additional charge(7), which leads to photoluminescence quenching by non-radiative recombination (the Auger mechanism)(8). However, this 'charging' model was recently challenged in several reports(9,10). Here we report time-resolved photoluminescence studies of individual nanocrystal quantum dots performed while electrochemically controlling the degree of their charging, with the goal of clarifying the role of charging in blinking. We find that two distinct types of blinking are possible: conventional (A-type) blinking due to charging and discharging of the nanocrystal core, in which lower photoluminescence intensities correlate with shorter photoluminescence lifetimes; and a second sort (B-type), in which large changes in the emission intensity are not accompanied by significant changes in emission dynamics. We attribute B-type blinking to charge fluctuations in the electron-accepting surface sites. When unoccupied, these sites intercept 'hot' electrons before they relax into emitting core states. Both blinking mechanisms can be electrochemically controlled and completely suppressed by application of an appropriate potential.
机构:
Univ Colorado, Boulder, CO 80309 USA
JILA, Natl Inst Stand & Technol, Boulder, CO USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USAUniv Colorado, Boulder, CO 80309 USA
Fomenko, Vasiliy
;
Nesbitt, David J.
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机构:
Univ Colorado, Boulder, CO 80309 USA
JILA, Natl Inst Stand & Technol, Boulder, CO USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USAUniv Colorado, Boulder, CO 80309 USA
机构:
Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Frantsuzov, Pavel
;
Kuno, Masaru
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机构:
Univ Notre Dame, Dept Chem & Biochem, Notre Dame, IN 46556 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Kuno, Masaru
;
Janko, Boldizsar
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机构:
Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Janko, Boldizsar
;
Marcus, Rudolph A.
论文数: 0引用数: 0
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机构:
CALTECH, Arthur Amos Noyes Lab Chem Phys, Pasadena, CA 91125 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
机构:
Univ Colorado, Boulder, CO 80309 USA
JILA, Natl Inst Stand & Technol, Boulder, CO USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USAUniv Colorado, Boulder, CO 80309 USA
Fomenko, Vasiliy
;
Nesbitt, David J.
论文数: 0引用数: 0
h-index: 0
机构:
Univ Colorado, Boulder, CO 80309 USA
JILA, Natl Inst Stand & Technol, Boulder, CO USA
Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USAUniv Colorado, Boulder, CO 80309 USA
机构:
Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Frantsuzov, Pavel
;
Kuno, Masaru
论文数: 0引用数: 0
h-index: 0
机构:
Univ Notre Dame, Dept Chem & Biochem, Notre Dame, IN 46556 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Kuno, Masaru
;
Janko, Boldizsar
论文数: 0引用数: 0
h-index: 0
机构:
Univ Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA
Janko, Boldizsar
;
Marcus, Rudolph A.
论文数: 0引用数: 0
h-index: 0
机构:
CALTECH, Arthur Amos Noyes Lab Chem Phys, Pasadena, CA 91125 USAUniv Notre Dame, Dept Phys, Notre Dame, IN 46556 USA