Classical Aspects of Energy Transfer in Molecular Systems

Kuhn, Hans

doi:10.1063/1.1673749

Cited by 616 publications

(315 citation statements)

References 18 publications

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“…The same results happen when we place the emitter in the cavity [152,153]. As the cavity itself can have different scales, shapes, and components, only specific modes of EM will be supported [154].…”

Section: Weak Coupling Conditions Of Cavity-qedmentioning

confidence: 55%

Exciton-plasmon coupling interactions: from principle to applications

et al. 2017

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Abstract:The interaction of exciton-plasmon coupling and the conversion of exciton-plasmon-photon have been widely investigated experimentally and theoretically. In this review, we introduce the exciton-plasmon interaction from basic principle to applications. There are two kinds of exciton-plasmon coupling, which demonstrate different optical properties. The strong exciton-plasmon coupling results in two new mixed states of light and matter separated energetically by a Rabi splitting that exhibits a characteristic anticrossing behavior of the exciton-LSP energy tuning. Compared to strong coupling, such as surface-enhanced Raman scattering, surface plasmon (SP)-enhanced absorption, enhanced fluorescence, or fluorescence quenching, there is no perturbation between wave functions; the interaction here is called the weak coupling. SP resonance (SPR) arises from the collective oscillation induced by the electromagnetic field of light and can be used for investigating the interaction between light and matter beyond the diffraction limit. The study on the interaction between SPR and exaction has drawn wide attention since its discovery not only due to its contribution in deepening and broadening the understanding of SPR but also its contribution to its application in light-emitting diodes, solar cells, low threshold laser, biomedical detection, quantum information processing, and so on.

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Section: Weak Coupling Conditions Of Cavity-qedmentioning

confidence: 55%

Exciton-plasmon coupling interactions: from principle to applications

et al. 2017

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“…This phenomenon was first observed by Drexhage 26 and was theoretically explained by several authors. [29][30][31] As the distance decreases further to the order of ∼50 Å to 100 Å, the radiative ion starts experiencing the electromagnetic field associated with surface plasmons. This decay has been observed experimentally and discussed earlier.…”

Section: Radiative Lifetime Of An Optically Active Ion Near a Metallimentioning

confidence: 99%

Theory of Radiative Lifetime of an Activator Ion due to Surface Plasmons

Mishra

Collins

Piquette

2018

ECS J. Solid State Sci. Technol.

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We consider the lifetime of a phosphor layer situated near a metallic film. We first make general observations of the effect of the plasmons on the lifetime and quantum efficiency of the luminescent ions in the phosphor layer and on the role of the plasmons in the emission process. The effect of the plasmons in the excitation process and on the total luminescence from the system is also discussed. We then derive an expression for the lifetime of the optical ions interacting with the surface plasmon modes using the Einstein A and B coefficient formalism, which requires a determination of the mode density of the surface plasmons. Because the surface plasmons represent a 2-dimensional system, a length parameter must be introduced into the expression of the mode density. We derive this parameter using a semi-classical approach, and show its dependence on the dielectric constants of the system and on the distance from the metallic layer. Recently there has been considerable interest on utilizing surface plasmons in metallic thin films to enhance internal quantum efficiency of luminescent materials [1][2][3][4][5][6][7][8][9][10][11][12] and light emitting diodes (LED). 13-22The most important effect of the surface plasmons on luminescent ions is on their lifetime in the excited state which could contribute to improving the internal quantum efficiency of luminescent materials in the form of a slab or a layer. In this paper, we have studied how the change in the excited state lifetime of the radiating atoms could be described using the dispersion relations of the surface plasmons. The lifetime of an excited ion, τ as measured by the decay measurements consists of two components, radiative lifetime,τ R and nonradiative lifetime, τ N R the reciprocals of which are additive,The radiative lifetime of an ion depends on the transition moments of the ion, i.e., the matrix element of the electric dipole and quadrupole moments or magnetic moments between the excited and ground state wavefunctions of the radiating ions. Normally the radiative lifetime is a characteristic of the optical ion and does not change unless the wavefunctions of the optical ions are perturbed. On the other hand, nonradiative lifetime is associated with the relaxation of the excited state to phonons, lattice defects and impurities with a loss of the excited state energy. It is sometimes possible to increase the nonradiative lifetime by controlling the purity of the material, operating temperature, better material processing etc., thus decreasing the probability of nonradiative relaxation of the ion. From Eq. 1, it can be shown that when the nonradiative lifetime increases, the lifetime of the excited state increases. This increase in lifetime usually results in an increase of the internal quantum efficiency.If a new nonradiative pathway is opened, the nonradiative lifetime will decrease. It will not always decrease the internal quantum efficiency if the transferred energy is not completely lost as it is in the case of phonons. Such could be the case for s...

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“…It has previously been reported that gold quenches lanthanide luminescence. 23 However, as such quenching is distance dependent, we proposed that our design would minimise any such quenching due to the presence of the C 12 spacer between 1ÁEu and the surface. To establish this, the delayed emission of 1ÁEu and 1ÁEuÁ2 and 1ÁEuÁ3 was recorded upon excitation at 281 nm.…”

mentioning

confidence: 99%

Luminescent self-assembly formation on a gold surface observed by reversible ‘off–on’ switching of Eu(iii) emission

2009

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The formation of a self-assembly between a sensitising antenna and an Eu(III) functionalised cyclen complex 1ÁEu, tethered to a gold surface via a C 12 alkyl thiol spacer, is described where changes in the Eu(III) emission signal the formation, and dissociation, of a ternary complex.The design and synthesis of functional material are of great current interest in chemistry and nanoscience. [1][2][3] In particular, systems based on the use of self-assembly formation have been developed and studied in solution as mimics of macroscopic devices such as molecular switches and sensors, integrated logic gates, and as artificial molecular machines.4-8 Immobilising such systems onto various solid substrates offers an attractive means of forming practical devices that possess more highly ordered and populated species than would generally be present in solution.9,10 The use of luminescence to investigate the properties and function of supramolecular assemblies has been extensively employed due to its non-invasive nature, fast response time and high sensitivity. 19,20 While the unique photophysical properties of the lanthanides make them ideal for observing self-assembly formation and for sensing, to the best of our knowledge, their use on gold substrates has not been achieved to date. Such modification would further increase their potential use in sensing applications, for instance, by combining them with atomic force microscope (AFM)-based micromechanical sensors, 21 which could result in the development of dual functioning sensory systems. We have previously demonstrated the formation of luminescent ternary complexes in solution formed through self-assembly using sensitising antennae and coordinatively unsaturated Eu(III) or Tb(III) complexes.22 Herein, we demonstrate that by anchoring such a lanthanide complex, 1ÁEu, onto a gold substrate, via an alkyl thiol linker, the lanthanide luminescence is 'switched on' upon formation of a self-assembly between 1ÁEu and a sensitising antenna, 2. The emission of this assembly can then be 'switched off' upon addition of 3, an anion possessing an antenna with unfavourable excited state energies for the population of the Eu(III) excited state.The rationale for our design is shown in Fig. 1. The gold substrates employed were made by firstly sonicating discs (9 mm diameter) of mica in ethanol, and then evaporating a thin layer of gold (approximately 10 nm). Following evaporation, the samples were immersed in 1 mM solutions of 1ÁEu and left overnight. This was followed by thoroughly rinsing the surface with ethanol and drying under N 2 .z Similarly, samples possessing 1ÁEu and 2 (1ÁEuÁ2) and 1ÁEu and the phosphate anion, flavin monophosphate 3 (1ÁEuÁ3), were also made for comparison purposes. The FTIR analysis of these modified gold surfaces showed the presence of both 1ÁEu and 1ÁEuÁ2 with a number of characteristic resonances being identified (see ESIw). For instance, the CQO stretch assigned to the carboxy amide of 1ÁEu appeared at 1624 cm À1 with a shoulder at 1636 cm À1, while the as...

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Classical Aspects of Energy Transfer in Molecular Systems

Cited by 616 publications

References 18 publications

Exciton-plasmon coupling interactions: from principle to applications

Exciton-plasmon coupling interactions: from principle to applications

Theory of Radiative Lifetime of an Activator Ion due to Surface Plasmons

Luminescent self-assembly formation on a gold surface observed by reversible ‘off–on’ switching of Eu(iii) emission

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