Surface-Enhanced Emission from Single Semiconductor Nanocrystals

Shimizu, Ken D.; Woo, Wing-Keung; Fisher, Brent; Eisler, Hans‐Jürgen; Bawendi, Moungi G.

doi:10.1103/physrevlett.89.117401

Cited by 605 publications

(639 citation statements)

References 25 publications

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“…The development of techniques in probing single molecules has provided a tool to study its intrinsic properties and its interaction with the surroundings. One of the unusual phenomena observed in nanoparticles is fluorescence intermittency of quantum dots and the power-law statistics for the duration time for the ''on'' an ''off'' events [1][2][3][4][5][6][7][8][9][10]. Supplementing previous theoretical studies [6,7,[11][12][13][14][15][16], a mechanism is provided in this Letter to elucidate these phenomena.…”

mentioning

confidence: 91%

Diffusion-Controlled Electron Transfer Processes and Power-Law Statistics of Fluorescence Intermittency of Nanoparticles

2005

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A mechanism involving diffusion-controlled electron transfer processes in Debye and non-Debye dielectric media is proposed to elucidate the power-law distribution for the lifetime of a blinking quantum dot. This model leads to two complementary regimes of power law with a sum of the exponents equal to 2, and to a specific value for the exponent in terms of a distribution of the diffusion correlation times. It also links the exponential bending tail with energetic and kinetic parameters. DOI: 10.1103/PhysRevLett.95.107401 PACS numbers: 78.67.Bf, 73.21.La, 73.63.Kv, 78.67.Hc Recent advances in nanoscience and nanotechnology and their potential applications have generated wide interest. The development of techniques in probing single molecules has provided a tool to study its intrinsic properties and its interaction with the surroundings. One of the unusual phenomena observed in nanoparticles is fluorescence intermittency of quantum dots and the power-law statistics for the duration time for the ''on'' an ''off'' events [1][2][3][4][5][6][7][8][9][10]. Supplementing previous theoretical studies [6,7,[11][12][13][14][15][16]], a mechanism is provided in this Letter to elucidate these phenomena. This model involves diffusioncontrolled charge transfer processes in energy or configuration space [17,18]. For fast diffusion, the model yields the well-known simple exponential decay. However, in the regime of slow diffusion, the model leads naturally to a power-law behavior. To be more general, we consider anomalous diffusion in a non-Debye dielectric medium with a distribution of diffusion correlation times. There exists in the literature two approaches, partial ordering prescription (POP) with a time-dependent but nonretarded diffusion coefficient, and chronological ordering prescription (COP) with convolution of a time-retarded diffusion kernel [19]. POP is more commonly used in treating electron transfer reactions [20], These diffusion-controlled reaction models provide physical insight into the specific value of the exponent, a reason for the bending tail at longer times, and the connection of the bending factor to the activation energy of the electron transfer rate constant.In this work, one models stochastic processes in the energy or configuration space that represent the fluctuating interactions of a probe (a single molecule or a quantum dot) with its surrounding heat bath (supporting substrate or anchored organic molecules). We consider a POP type 1D non-Markovian equation, with a population sink at the potential energy crossing (Q Q c ) between U 1 Q for the ''light'' state j1i and U 2 Q for the ''dark'' state j2i. One hasOne can obtain the Green function for sink-free diffusion in a harmonic potential q 2 =2 as [20]where the diffusion constant D k t is related to the dielectric response function s and the dielectric permittivity " s by [20]For a Debye medium CD . At times t much longer than the diffusion correlation time, however, 2 t becomes a constant as the system approaches thermal equilibrium. The asym...

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confidence: 91%

Diffusion-Controlled Electron Transfer Processes and Power-Law Statistics of Fluorescence Intermittency of Nanoparticles

2005

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“…Prominent recent applications include midinfrared quantum cascade lasers, where SPPs confined to the boundary between the gain medium and a thin metallic layer were found to substantially enhance the overlap between the optical mode and the gain medium and further enabled reduced cladding heights compared to semiconducting layers, 101,102 and the demonstration of emission enhancement of Ref. 103 and strong coupling 104 to semiconductor quantum dots.…”

Section: Interactions With Optically Active Mediamentioning

confidence: 99%

“…When studying the interaction of emissive species such as quantum dots 103 and wells, 101 fluophores 105 or rare-earth ions 106 with metallic surfaces, 107 gratings 105 or nanoparticles, 108 special care must be taken for a distinction between radiative and nonradiative contributions to the total enhanced decay rate. The huge increase of the non-radiative decay rate observed for emissive species placed in nanometric distances to metallic surfaces makes the design of plasmonic cavities for emissive devices challenging, 109 but promising routes for the creation of efficient emissive devices such as light-emmiting diodes ͑LEDs͒ based on SPPsupporting cavities have been developed 110,111 and partly demonstrated.…”

Section: Interactions With Optically Active Mediamentioning

confidence: 99%

Plasmonics: Localization and guiding of electromagnetic energy in metal/dielectric structures

Maier

Atwater

2005

Journal of Applied Physics

1,800

1,217

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We review the basic physics of surface-plasmon excitations occurring at metal/dielectric interfaces with special emphasis on the possibility of using such excitations for the localization of electromagnetic energy in one, two, and three dimensions, in a context of applications in sensing and waveguiding for functional photonic devices. Localized plasmon resonances occurring in metallic nanoparticles are discussed both for single particles and particle ensembles, focusing on the generation of confined light fields enabling enhancement of Raman-scattering and nonlinear processes. We then survey the basic properties of interface plasmons propagating along flat boundaries of thin metallic films, with applications for waveguiding along patterned films, stripes, and nanowires. Interactions between plasmonic structures and optically active media are also discussed.

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“…Since the discovery of the Purcell effect [9], efforts to increase the sensitivity of fluorescence detection have focused on controlling the local electromagnetic (EM) environment of the fluorophores and taking advantage of the interaction between an emitter and its surroundings. The dielectric environment has a profound influence on the emission of a fluorophore, through its spontaneous emission rate and local modifications of the electromagnetic field: fluorescence quenching [10] [12], fluorescence enhancement [13]- [15] or both [16] [17] have all been reported. It has been shown experimentally, and supported by theoretical calculations, that the fluorescence enhancement factors of metal nanostructures depend on the particle size, shape, interparticle separation, surrounding dielectric medium, as well as the particle arrangement geometry and distance between the metal and fluorophore.…”

Section: Introductionmentioning

confidence: 99%

Nanoscale control of Ag nanostructures for plasmonic fluorescence enhancement of near-infrared dyes

Xie

Pang

Centeno³

et al. 2013

Nano Res.

125

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Surface-Enhanced Emission from Single Semiconductor Nanocrystals

Cited by 605 publications

References 25 publications

Diffusion-Controlled Electron Transfer Processes and Power-Law Statistics of Fluorescence Intermittency of Nanoparticles

Diffusion-Controlled Electron Transfer Processes and Power-Law Statistics of Fluorescence Intermittency of Nanoparticles

Plasmonics: Localization and guiding of electromagnetic energy in metal/dielectric structures

Nanoscale control of Ag nanostructures for plasmonic fluorescence enhancement of near-infrared dyes

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